The 100 most-cited articles in Environmental Science & Technology, 2024

Micro- and nanoplastics (MNPs) are attracting increasing attention due to their persistence and potential ecological risks. This review critically summarizes the effects of photo-oxidation on the physical, chemical, and biological behaviors of MNPs in aquatic and terrestrial environments. The core of this paper explores how photo-oxidation-induced surface property changes in MNPs affect their adsorption toward contaminants, the stability and mobility of MNPs in water and porous media, as well as the transport of pollutants such as organic pollutants (OPs) and heavy metals (HMs). It then reviews the photochemical processes of MNPs with coexisting constituents, highlighting critical factors affecting the photo-oxidation of MNPs, and the contribution of MNPs to the phototransformation of other contaminants. The distinct biological effects and mechanism of aged MNPs are pointed out, in terms of the toxicity to aquatic organisms, biofilm formation, planktonic microbial growth, and soil and sediment microbial community and function. Furthermore, the research gaps and perspectives are put…

Persulfate (PS)-based advanced oxidation processes (AOPs) for pollutant removal have attracted extensive interest, but some controversies about the identification of reactive species were usually observed. This critical review aims to comprehensively introduce basic concepts and rectify cognitive biases and appeals to pay more attention to experimental details in PS-AOPs, so as to accurately explore reaction mechanisms. The review scientifically summarizes the character, generation, and identification of different reactive species. It then highlights the complexities about the analysis of electron paramagnetic resonance, the uncertainties about the use of probes and scavengers, and the necessities about the determination of scavenger concentration. The importance of the choice of buffer solution, operating mode, terminator, and filter membrane is also emphasized. Finally, we discuss current challenges and future perspectives to alleviate the misinterpretations toward reactive species and reaction mechanisms in PS-AOPs.

Trifluoroacetic acid (TFA) is a persistent and mobile substance that has been increasing in concentration within diverse environmental media, including rain, soils, human serum, plants, plant-based foods, and drinking water. Currently, TFA concentrations are orders of magnitude higher than those of other per- and polyfluoroalkyl substances (PFAS). This accumulation is due to many PFAS having TFA as a transformation product, including several fluorinated gases (F-gases), pesticides, pharmaceuticals, and industrial chemicals, in addition to direct release of industrially produced TFA. Due to TFA's extreme persistence and ongoing emissions, concentrations are increasing irreversibly. What remains less clear are the thresholds where irreversible effects on local or global scales occur. There are indications from mammalian toxicity studies that TFA is toxic to reproduction and that it exhibits liver toxicity. Ecotoxicity data are scarce, with most data being for aquatic systems; fewer data are available for terrestrial plants, where TFA bioaccumulates most readily. Collectively, these…

This perspective presents the latest advancements in selective polymerization pathways in advanced oxidation processes (AOPs) for removal of featured organic pollutants in wastewater. In radical-based homogeneous reactions, SO 4 • – -based systems exhibit superior oxidative activity toward aromatics with electron-donating substituents via single electron transfer and radical adduct formation (RAF). The produced organic radical cations subsequently undergo coupling and polymerization reactions to produce polymers. For • OH-based oxidation, metal ions facilitate the production of monomer radicals via RAF. Additionally, heterogeneous catalysts can mediate both coupling and polymerization reactions via persulfate activation without generating inorganic radicals. Metal-based catalysts will mediate a direct oxidation pathway toward polymerization. In contrast, carbon-based catalysts will induce coupling reactions to produce low-molecular-weight oligomers (≤4 units) via an electron transfer process. In comparison to mineralization, polymerization pathways remarkably reduce peroxide usage,…

China is one of the major global consumers of veterinary antibiotics. Insufficient recognition of emissions and environmental contamination hamper global efforts to prevent antibiotic resistance development. This pioneering study combined empirical data and modeling approaches to predict total 2010–2020 emissions of 80 veterinary antibiotics ranging from 23,110 to 40,850 tonnes/year, after 36–50% antibiotic removal by manure treatment. Following an initial increase of 10% from 2010 to 2015, emissions declined thereafter by 43%. While 85% of emissions discharged into soils, approximately 56%, 23%, and 18% of environmental residue were ultimately distributed in soils, freshwaters, and seawaters under steady-state conditions. In 2020, 657 (319–1470) tonnes entered the ocean from inland freshwaters. Median ∑antibiotics concentrations were estimated at 4.7 × 10 3 ng/L in freshwaters and 2.9 ng/g in soils, with tetracyclines and sulfonamides as the predominant components. We identified 44 veterinary antibiotics potentially posing high risks of resistance development in freshwaters, with…

The lithium iron phosphate (LFP) battery has been widely used in electric vehicles and energy storage for its good cyclicity, high level of safety, and low cost. The massive application of LFP battery generates a large number of spent batteries. Recycling and regenerating materials from spent LFP batteries has been of great concern because it can significantly recover valuable metals and protect the environment. This paper aims to critically assess the latest technical information available on the echelon utilization and recycling of spent LFP batteries. First, it focuses on the progress of disassembly, evaluation and detection, regrouping, and application in echelon utilization. Then, the recycling technologies, including pretreatment, direct repair, and material regeneration, of spent LFPs are summarized. Finally, the paper proposes some challenges in the echelon utilization and recycling of spent LFP batteries, and concludes with recommendations for an intelligent, refined, and clean LFP battery circulation system that are required to ensure the sustainable development of spent…

Microplastics (MPs) are ubiquitous in global ecosystems and may pose a potential risk to human health. However, critical information on MP exposure and risk to female reproductive health is still lacking. In this study, we characterized MPs in human endometrium and investigated their size-dependent entry mode as well as potential reproductive toxicity. Endometrial tissues of 22 female patients were examined, revealing that human endometrium was contaminated with MPs, mainly polyamide (PA), polyurethane (PU), polyethylene terephthalate (PET), polypropylene (PP), polystyrene (PS), and polyethylene (PE), ranging from 2–200 μm in size. Experiments conducted in mice demonstrated that the invasion of the uterus by MPs was modulated either through diet–blood circulation (micrometer-sized particles) or via the vagina–uterine lacuna mode (larger particles reaching a size of 100 μm. Intravenous exposure to MPs resulted in reduced fertility and abnormal sex ratio in mouse offspring ( P < 0.05). After 3.5 months of intragastric exposure, there was a significant inflammatory response in the…

High Resolution Image Download MS PowerPoint Slide Microplastics are ubiquitous environmental contaminants for which there are documented human exposures, but there is a paucity of research evaluating their impacts on human health. We conducted a rapid systematic review using the “Navigation Guide” systematic review method. We searched four databases in July 2022 and April 2024 with no restriction on the date. We included studies using predefined eligibility criteria that quantitatively examined the association of microplastic exposure with any health outcomes. We amended the eligibility criteria after screening studies and prioritized digestive, reproductive, and respiratory outcomes for further evaluation. We included three human observational studies examining reproductive ( n = 2) and respiratory ( n = 1) outcomes and 28 animal studies examining reproductive ( n = 11), respiratory ( n = 7), and digestive ( n = 10) outcomes. For reproductive outcomes (sperm quality) and digestive outcomes (immunosuppresion) we rated overall body evidence as “high” quality and concluded…

Per- and polyfluoroalkyl substances (PFAS) are a diverse class of highly persistent anthropogenic chemicals that are detectable in the serum of most humans. PFAS exposure has been associated with many adverse effects on human health including immunotoxicity, increased risk of certain cancers, and metabolic disruption. PFAS binding to the most abundant blood serum proteins (human serum albumin [HSA] and globulins) is thought to affect transport to active sites, toxicity, and elimination half-lives. However, few studies have investigated the competitive binding of PFAS to these proteins in human serum. Here, we use C18 solid-phase microextraction fibers to measure HSA–water and globulin–water distribution coefficients ( D HSA/w, D glob/w ) for PFAS with carbon chains containing 4 to 13 perfluorinated carbons (η pfc = 4–13) and several functional head-groups. PFAS with η pfc < 7 were highly bound to HSA relative to globulins, whereas PFAS with η pfc ≥ 7 showed a greater propensity for binding to globulins. Experimentally measured D HSA/w and D glob/w and concentrations of serum…

Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), as a promising technology for water decontamination, are constrained by low reaction kinetics due to limited reaction selectivity and mass transfer. Herein, we designed a nanoconfined FeCo 2 O 4 -embedded ceramic membrane (FeCo 2 O 4 −CM) under flow-through pattern for PMS activation. Confining PMS and FeCo 2 O 4 within nanochannels (3.0−4.7 nm) enhanced adsorption interactions (−7.84 eV vs −2.20 eV), thus boosting mass transfer. Nanoconfinement effect regulated electron transfer pathways from PMS to FeCo 2 O 4 −CM by modulating the active site transformation to ≡Co(III) in nanoconfined FeCo 2 O 4 −CM, enabling selectively generating 1 O 2 . The primary role of 1 O 2 in the nanoconfined system was confirmed by kinetic solvent isotope experiments and indicative anthracene endoperoxide (DPAO 2 ). The system enabled 100% removal of atrazine (ATZ) within a hydraulic retention time of 2.124 ms, demonstrating a rate constant over 5 orders of magnitude higher than the nonconfined system (3.50 × 10 3 s −1 vs 0.42 min −1 ).…

Ensuring water quality and safety requires the effective detection of emerging contaminants, which present significant risks to both human health and the environment. Field deployable low-cost sensors provide solutions to detect contaminants at their source and enable large-scale water quality monitoring and management. Unfortunately, the availability and utilization of such sensors remain limited. This Perspective examines current sensing technologies for detecting emerging contaminants and analyzes critical barriers, such as high costs, lack of reliability, difficulties in implementation in real-world settings, and lack of stakeholder involvement in sensor design. These technical and nontechnical barriers severely hinder progression from proof-of-concepts and negatively impact user experience factors such as ease-of-use and actionability using sensing data, ultimately affecting successful translation and widespread adoption of these technologies. We provide examples of specific sensing systems and explore key strategies to address the remaining scientific challenges that must be…

Surface-enhanced Raman spectroscopy (SERS) has gained significant attention for its ability to detect environmental contaminants with high sensitivity and specificity. The cost-effectiveness and potential portability of the technique further enhance its appeal for widespread application. However, challenges such as the management of voluminous quantities of high-dimensional data, its capacity to detect low-concentration targets in the presence of environmental interferents, and the navigation of the complex relationships arising from overlapping spectral peaks have emerged. In response, there is a growing trend toward the use of machine learning (ML) approaches that encompass multivariate tools for effective SERS data analysis. This comprehensive review delves into the detailed steps needed to be considered when applying ML techniques for SERS analysis. Additionally, we explored a range of environmental applications where different ML tools were integrated with SERS for the detection of pathogens and (in)organic pollutants in environmental samples. We sought to comprehend the…

Foliar application of beneficial nanoparticles (NPs) exhibits potential in reducing cadmium (Cd) uptake in crops, necessitating a systematic understanding of their leaf–root–microorganism process for sustainable development of efficient nano-enabled agrochemicals. Herein, wheat grown in Cd-contaminated soil (5.23 mg/kg) was sprayed with different rates of four commonly used NPs, including nano selenium (SeNPs)/silica (SiO 2 NPs)/zinc oxide/manganese dioxide. SeNPs and SiO 2 NPs most effectively reduced the Cd concentration in wheat grains. Compared to the control, Cd concentration in grains was significantly decreased by 35.0 and 33.3% by applying 0.96 mg/plant SeNPs and 2.4 mg/plant SiO 2 NPs, and the grain yield was significantly increased by 33.9% with SeNPs application. Down-regulated gene expression of Cd transport proteins ( TaNramp 5 and TaLCT 1) and up-regulated gene expression of vacuolar Cd fixation proteins ( TaHMA 3 and TaTM 20) were observed with foliar SeNPs and SiO 2 NPs use. SeNPs increased the levels of leaf antioxidant metabolites. Additionally, foliar spray of…

The groundwater table fluctuation (GTF) zone is an important medium for the hydrologic cycle between unsaturated soil and saturated aquifers, which accelerates the migration, transformation, and redistribution of contaminants and further poses a potential environmental risk to humans. In this review, we clarify the key processes in the generation of the GTF zone and examine its links with the variation of the hydrodynamic and hydrochemistry field, colloid mobilization, and contaminant migration and transformation. Driven by groundwater recharge and discharge, GTF regulates water flow and the movement of the capillary fringe, which further control the advection and dispersion of contaminants in soil and groundwater. In addition, the formation and variation of the reactive oxygen species (ROS) waterfall are impacted by GTF. The changing ROS components partially determine the characteristic transformation of solutes and the dynamic redistribution of the microbial population. GTF facilitates the migration and transformation of contaminants (such as nitrogen, heavy metals, non-aqueous…

Significant efforts have recently been exerted toward construction of singlet oxygen ( 1 O 2 )-dominated catalytic oxidation systems for selective removal of organic contaminants from wastewater, with peroxides serving as the chemical source. However, the relevance of 1 O 2 in the removal of pollutants remains ambiguous and requires elucidation. In this study, we scrupulously exclude the significant role of 1 O 2 in contaminant degradation in various peroxymonosulfate (PMS) activation systems. Multiple experimental results indicate that the activation of PMS catalyzed by CuO, MnO 2, Fe-doped g-C 3 N 4 (Fe–CN), or N-doped graphite does not predominantly follow the 1 O 2 pathway. More importantly, the reactivity of 1 O 2 is remarkably overestimated in the literature, given its inferior capacity in degradation of a range of heterocyclic contaminants and aromatic compounds possessing electron-withdrawing groups. In addition, the strong physical quenching effect of water, coupled with the low oxidizing ability of 1 O 2, would notably reduce the utilization efficiency of peroxide, which…

Nitrate, a prevalent water pollutant, poses substantial public health concerns and environmental risks. Electrochemical reduction of nitrate (eNO 3 RR) has emerged as an effective alternative to conventional biological treatments. While extensive lab work has focused on designing efficient electrocatalysts, implementation of eNO 3 RR in practical wastewater settings requires careful consideration of the effects of various constituents in real wastewater. In this critical review, we examine the interference of ionic species commonly encountered in electrocatalytic systems and universally present in wastewater, such as halogen ions, alkali metal cations, and other divalent/trivalent ions (Ca 2+, Mg 2+, HCO 3 – /CO 3 2–, SO 4 2–, and PO 4 3– ). Notably, we categorize and discuss the interfering mechanisms into four groups: (1) loss of active catalytic sites caused by competitive adsorption and precipitation, (2) electrostatic interactions in the electric double layer (EDL), including ion pairs and the shielding effect, (3) effects on the selectivity of N intermediates and final…

Microplastics (MPs) contamination presents a significant global environmental challenge, with its potential to influence soil carbon (C) dynamics being a crucial aspect for understanding soil C changes and global C cycling. This meta-analysis synthesizes data from 110 peer-reviewed publications to elucidate the directional, magnitude, and driving effects of MPs exposure on soil C dynamics globally. We evaluated the impacts of MPs characteristics (including type, biodegradability, size, and concentration), soil properties (initial pH and soil organic C [SOC]), and experimental conditions (such as duration and plant presence) on various soil C components. Key findings included the significant promotion of SOC, dissolved organic C, microbial biomass C, and root biomass following MPs addition to soils, while the net photosynthetic rate was reduced. No significant effects were observed on soil respiration and shoot biomass. The study highlights that the MPs concentration, along with other MPs properties and soil attributes, critically influences soil C responses. Our results demonstrate…

PFASs are linked to serious health and environmental concerns. Among their widespread applications, PFASs are known to be used in food packaging and directly contribute to human exposure. However, information about PFASs in food packaging is scattered. Therefore, we systematically map the evidence on PFASs detected in migrates and extracts of food contact materials and provide an overview of available hazard and biomonitoring data. Based on the FCCmigex database, 68 PFASs have been identified in various food contact materials, including paper, plastic, and coated metal, by targeted and untargeted analyses. 87% of these PFASs belong to the perfluorocarboxylic acids and fluorotelomer-based compounds. Trends in chain length demonstrate that long-chain perfluoroalkyl acids continue to be found, despite years of global efforts to reduce the use of these substances. We utilized ToxPi to illustrate that hazard data are available for only 57% of the PFASs that have been detected in food packaging. For those PFASs for which toxicity testing has been performed, many adverse outcomes have been…

In the modern "omics" era, measurement of the human exposome is a critical missing link between genetic drivers and disease outcomes. High-resolution mass spectrometry (HRMS), routinely used in proteomics and metabolomics, has emerged as a leading technology to broadly profile chemical exposure agents and related biomolecules for accurate mass measurement, high sensitivity, rapid data acquisition, and increased resolution of chemical space. Non-targeted approaches are increasingly accessible, supporting a shift from conventional hypothesis-driven, quantitation-centric targeted analyses toward data-driven, hypothesis-generating chemical exposome-wide profiling. However, HRMS-based exposomics encounters unique challenges. New analytical and computational infrastructures are needed to expand the analysis coverage through streamlined, scalable, and harmonized workflows and data pipelines that permit longitudinal chemical exposome tracking, retrospective validation, and multi-omics integration for meaningful health-oriented inferences. In this article, we survey the literature on…

Heavy metal pollution treatment in industrial wastewater is crucial for protecting biological and environmental safety. However, the highly efficient and selective removal of heavy metal ions from multiple cations in wastewater is a significant challenge. This work proposed a pulse electrochemical method with a low-/high-voltage periodic appearance to selectively recover heavy metal ions from complex wastewater. It exhibited a higher recovery efficiency for heavy metal ions (100% for Pb 2+ and Cd 2+, >98% for Mn 2+ ) than other alkali and alkaline earth metal ions (Na +, Ca 2+, and Mg 2+ were kept below 3.6, 1.3, and 2.6%, respectively) in the multicomponent solution. The energy consumption was only 34–77% of that of the direct current electrodeposition method. The results of characterization and experiment unveil the mechanism that the low-/high-voltage periodic appearance can significantly suppress the water-splitting reaction and break the mass-transfer limitation between heavy metal ions and electrodes. In addition, the plant study demonstrates the feasibility of treated…

Cu(II)-catalyzed peracetic acid (PAA) processes have shown significant potential to remove contaminants in water treatment. Nevertheless, the role of coexistent H 2 O 2 in the transformation from Cu(II) to Cu(I) remained contentious. Herein, with the Cu(II)/PAA process as an example, the respective roles of PAA and H 2 O 2 on the Cu(II)/Cu(I) cycling were comprehensively investigated over the pH range of 7.0–10.5. Contrary to previous studies, it was surprisingly found that the coexistent deprotonated H 2 O 2 (HO 2 – ), instead of PAA, was crucial for accelerating the transformation from Cu(II) to Cu(I) ( k HO2–/Cu(II) = (0.17–1) × 10 6 M –1 s –1, k PAA/Cu(II) < 2.33 ± 0.3 M –1 s –1 ). Subsequently, the formed Cu(I) preferentially reacted with PAA ( k PAA/Cu(I) = (5.84 ± 0.17) × 10 2 M –1 s –1 ), rather than H 2 O 2 ( k H2O2/Cu(I) = (5.00 ± 0.2) × 10 1 M –1 s –1 ), generating reactive species to oxidize organic contaminants. With naproxen as the target pollutant, the proposed synergistic role of H 2 O 2 and PAA was found to be highly dependent on the solution pH with weakly alkaline…

Per- and polyfluoroalkyl substances (PFASs) are a large group of anthropogenic fluorinated chemicals. Ultrashort-chain perfluoroalkyl acids (PFAAs) have recently gained attention due to their prevalence in the environment and increasing environmental concerns. In this review, we established a literature database from 1990 to 2024, encompassing environmental and biological concentrations (>3,500 concentration records) of five historically overlooked ultrashort-chain PFAAs (perfluoroalkyl carboxylic and sulfonic acids with less than 4 carbons): trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), trifluoromethanesulfonic acid (TFMS), perfluoroethanesulfonate (PFEtS), and perfluoropropanesulfonate (PFPrS). Our data mining and analysis reveal that (1) ultrashort-chain PFAAs are globally distributed in various environments including water bodies, solid matrices, and air, with concentrations usually higher than those of longer-chain compounds; (2) TFA, the most extensively studied ultrashort-chain PFAA, shows a consistent upward trend in concentrations in surface water, rainwater,…

Radical-based advanced oxidation processes (AOPs) are among the most effective technologies employed to destroy organic pollutants. Compared to common inorganic radicals, such as • OH, O 2 •–, and SO 4 •–, organic radicals are widespread, and more selective, but are easily overlooked. Furthermore, a systematic understanding of the generation and contributions of organic radicals remains lacking. In this review, we systematically summarize the properties, possible generation pathways, detection methods, and contributions of organic radicals in AOPs. Notably, exploring organic radicals in AOPs is challenging due to (1) limited detection methods for generated organic radicals; (2) controversial organic radical-mediated reaction mechanisms; and (3) rapid transformation of organic radicals as reaction intermediates. In addition to their characteristics and reactivity, we examine potential scenarios of organic radical generation in AOPs, including during the peroxide activation process, in water matrices or with coexisting organic pollutants, and due to the addition of quenching agents.…

Microplastics (MPs), plastic particles smaller than 5 mm, are now a growing environmental and public health issue, as they are detected pervasively in freshwater and marine environments, ingested by organisms, and then enter the human body. Industrial development drives this environmental burden caused by MP formation and human uptake by elevating plastic pollution levels and shaping the domestic dietary structure. We map the MP human uptake across 109 global countries on five continents from 1990 to 2018, focusing on the world's major coastlines that are affected by plastic pollution that affects the United Nations' Sustainable Development Goals (SDGs): SDG 6 (Clean Water and Sanitation), SDG 14 (Life Below Water), and SDG 15 (Life on Land). Amid rapid industrial growth, Indonesia tops the global per capita MP dietary intake at 15 g monthly. In Asian, African, and American countries, including China and the United States, airborne and dietary MP uptake increased over 6-fold from 1990 to 2018. Eradicating 90% of global aquatic plastic debris can help decrease MP uptake by more than…

Metal-free carbon material-mediated nonradical oxidation processes (C-NOPs) have emerged as a research hotspot due to their excellent performance in selectively eliminating organic pollutants in aqueous environments. However, the selective oxidation mechanisms of C-NOPs remain obscure due to the diversity of organic pollutants and nonradical active species. Herein, quantitative structure-activity relationship (QSAR) models were employed to unveil the origins of C-NOP selectivity toward organic pollutants in different oxidant systems. QSAR analysis based on adsorption and oxidation descriptors revealed that C-NOP selectivity depends on the oxidation potentials of organic pollutants rather than on adsorption interactions. However, the dominance of electronic effects in selective oxidation decreases with increasing structural complexity of organic pollutants. Moreover, the oxidation threshold solely depends on the inherent electronic nature of organic pollutants and not on the reactivity of nonradical active species. Notably, the accuracy of substituent descriptors (Hammett constants)…

Direct interspecies electron transfer (DIET) provides an innovative way to achieve efficient methanogenesis, and this study proposes a new approach to upregulate the DIET pathway by enhancing quorum sensing (QS). Based on long-term reactor performance, QS enhancement achieved more vigorous methanogenesis with 98.7% COD removal efficiency. In the control system, methanogenesis failure occurred at the accumulated acetate of 7420 mg of COD/L and lowered pH of 6.04, and a much lower COD removal of 41.9% was observed. The more significant DIET in QS-enhancing system was supported by higher expression of conductive pili and the c -Cyts cytochrome secretion-related genes, resulting in 12.7- and 10.3-fold improvements. Moreover, QS enhancement also improved the energy production capability, with the increase of F-type and V/A-type ATPase expression by 6.3- and 4.2-fold, and this effect probably provided more energy for nanowires and c -Cyts cytochrome secretion. From the perspective of community structure, QS enhancement increased the abundance of Methanosaeta and Geobacter from 54.3 and…

Electrocatalytic nitrate reduction to ammonia (NITRR) offers an attractive solution for alleviating environmental concerns, yet in neutral media, it is challenging as a result of the reliance on the atomic hydrogen (H*) supply by breaking the stubborn HO–H bond (∼492 kJ/mol) of H2O. Herein, we demonstrate that fluorine modification on a Cu electrode (F-NFs/CF) favors the formation of an O–H···F hydrogen bond at the Cu–H2O interface, remarkably stretching the O–H bond of H2O from 0.98 to 1.01 Å and lowering the energy barrier of water dissociation into H* from 0.64 to 0.35 eV at neutral pH. As a benefit from these advantages, F-NFs/CF could rapidly reduce NO3– to NH3 with a rate constant of 0.055 min–1 and a NH3 selectivity of ∼100%, far higher than those (0.004 min–1 and 9.2%) of the Cu counterpart. More importantly, we constructed a flow-through coupled device consisting of a NITRR electrolyzer and a NH3 recovery unit, realizing 98.1% of total nitrogen removal with 99.3% of NH3 recovery and reducing the denitrification cost to $5.1/kg of N. This study offers an effective strategy…

The discovery of the significant lethal impacts of the tire additive transformation product N -(1,3-dimethylbutyl)- N ′-phenyl- p -phenylenediamine quinone (6PPD-Q) on coho salmon has garnered global attention. However, the bioaccumulation and trophic transfer of tire additives and their transformation products (TATPs) within food webs remain obscure. This study first characterized the levels and compositions of 15 TATPs in the Pearl River Estuary, estimated their bioaccumulation and trophic transfer potential in 21 estuarine species, and identified priority contaminants. Our observations indicated that TATPs were prevalent in the estuarine environment. Eight, six, seven, and 10 TATPs were first quantified in the shrimp, sea cucumber, snail, and fish samples, with total mean levels of 45, 56, 64, and 67 ng/g (wet weight), respectively. N, N ′-Diphenyl- p -phenylenediamine (DPPD) and N, N ′-bis(2-methylphenyl)-1,4-benzenediamine (DTPD) exhibited high bioaccumulation. Significant biodilution was only identified for benzothiazole, while DPPD and DTPD displayed biomagnification trends…

Heterogeneous electro-Fenton degradation with 1 O 2 and • OH generated from O 2 reduction is cost-effective for the removal of refractory organic pollutants from wastewater. As 1 O 2 is more tolerant to background constituents such as salt ions and a high pH value than • OH, tuning the production of 1 O 2 and • OH is important for efficient electro-Fenton degradation. However, it remains a great challenge to selectively produce 1 O 2 and improve the species yield. Herein, the electronic structure of atomically dispersed Cu–N 4 sites was regulated by doping electron-deficient B into porous hollow carbon microspheres (CuBN-HCMs), which improved *O 2 adsorption and significantly enhanced 1 O 2 selectivity in electro-Fenton degradation. Its 1 O 2 yield was 2.3 times higher than that of a Cu single-atom catalyst without B doping. Meanwhile, • OH was simultaneously generated as a minor species. The CuBN-HCMs were efficient for the electro-Fenton degradation of phenol, sulfamethoxazole, and bisphenol A with a high mineralization efficiency. Its kinetic constants showed insignificant…

Microbial nitrogen metabolism is a complicated and key process in mediating environmental pollution and greenhouse gas emissions in rivers. However, the interactive drivers of microbial nitrogen metabolism in rivers have not been identified. Here, we analyze the microbial nitrogen metabolism patterns in 105 rivers in China driven by 26 environmental and socioeconomic factors using an interpretable causal machine learning (ICML) framework. ICML better recognizes the complex relationships between factors and microbial nitrogen metabolism than traditional linear regression models. Furthermore, tipping points and concentration windows were proposed to precisely regulate microbial nitrogen metabolism. For example, concentrations of dissolved organic carbon (DOC) below tipping points of 6.2 and 4.2 mg/L easily reduce bacterial denitrification and nitrification, respectively. The concentration windows for NO 3 – -N (15.9–18.0 mg/L) and DOC (9.1–10.8 mg/L) enabled the highest abundance of denitrifying bacteria on a national scale. The integration of ICML models and field data clarifies the…

Soil microbes, the main driving force of terrestrial biogeochemical cycles, facilitate soil organic matter turnover. However, the influence of the soil fauna on microbial communities remains poorly understood. We investigated soil microbiota dynamics by introducing competition and predation among fauna into two soil ecosystems with different fertilization histories. The interactions significantly affected rare microbial communities including bacteria and fungi. Predation enhanced the abundance of C/N cycle-related genes. Rare microbial communities are important drivers of soil functional gene enrichment. Key rare microbial taxa, including SM1A02, Gammaproteobacteria, and HSB_OF53-F07, were identified. Metabolomics analysis suggested that increased functional gene abundance may be due to specific microbial metabolic activity mediated by soil fauna interactions. Predation had a stronger effect on rare microbes, functional genes, and microbial metabolism compared to competition. Long-term organic fertilizer application increased the soil resistance to animal interactions. These…

The rising in situ chemical oxidation (ISCO) technologies based on polymerization reactions have advanced the removal of emerging contaminants in the aquatic environment. However, despite their promise, uncertainties persist regarding their effectiveness in eliminating structurally complex contaminants, such as sulfonamide antibiotics (SAs). This study elucidated that oligomerization, rather than mineralization, predominantly governs the removal of SAs in the carbon materials/periodate system. The amine groups in SAs played a crucial role in forming organic radicals and subsequent coupling reactions due to their high f – index and low bond orders. Moreover, the study highlighted the robust adhesion of oligomers to the catalyst surface, facilitated by enhanced van der Waals forces and hydrophobic interactions. Importantly, plant and animal toxicity assessments confirmed the nontoxic nature of oligomers deposited on the carbon material surface, affirming the efficacy of carbon material-based ISCO in treating contaminated surface water and groundwater. Additionally, a novel…

Advanced oxidation processes (AOPs) are rapidly evolving but still lack well-established protocols for reliably identifying oxidative reactive species (ORSs). This Perspective presents both the radical and nonradical ORSs that have been identified or proposed, along with the extensive controversies surrounding oxidative mechanisms. Conventional identification tools, such as quenchers, probes, and spin trappers, might be inadequate for the analytical demands of systems in which multiple ORSs coexist, often yielding misleading results. Therefore, the challenges of identifying these complex, short-lived, and transient ORSs must be fully acknowledged. Refining analytical methods for ORSs is necessary, supported by rigorous experiments and innovative paradigms, particularly through kinetic analysis based on in situ spectroscopic techniques and multiple-probe strategies. To demystify these complex ORSs, future efforts should be made to develop advanced tools and strategies to enhance the mechanism understanding. In addition, integrating real-world conditions into experimental designs will…

Solar desalination, a green, low-cost, and sustainable technology, offers a promising way to get clean water from seawater without relying on electricity and complex infrastructures. However, the main challenge faced in solar desalination is salt accumulation, either on the surface of or inside the solar evaporator, which can impair solar-to-vapor efficiency and even lead to the failure of the evaporator itself. While many ideas have been tried to address this ″salt accumulation″, scientists have not had a clear system for understanding what works best for the enhancement of salt-rejecting ability. Therein, for the first time, we classified the state-of-the-art salt-rejecting designs into isolation strategy (isolating the solar evaporator from brine), dilution strategy (diluting the concentrated brine), and crystallization strategy (regulating the crystallization site into a tiny area). Through the specific equations presented, we have identified key parameters for each strategy and highlighted the corresponding improvements in the solar desalination performance. This Review…

When chemical pollutants enter the environment, they can undergo diverse transformation processes, forming a wide range of transformation products (TPs), some of them benign and others more harmful than their precursors. To date, the majority of TPs remain largely unrecognized and unregulated, particularly as TPs are generally not part of routine chemical risk or hazard assessment. Since many TPs formed from oxidative processes are more polar than their precursors, they may be especially relevant in the context of persistent, mobile, and toxic (PMT) and very persistent and very mobile (vPvM) substances, which are two new hazard classes that have recently been established on a European level. We highlight herein that as a result, TPs deserve more attention in research, chemicals regulation, and chemicals management. This perspective summarizes the main challenges preventing a better integration of TPs in these areas: (1) the lack of reliable high-throughput TP identification methods, (2) uncertainties in TP prediction, (3) inadequately considered TP formation during (advanced) water…

Tire wear particles (TWPs) have caused increasing concerns due to their detrimental effects on the soil ecosystem. However, the role of weathering in altering the toxicity of TWP to soil organisms is poorly understood. In this study, the toxicity of original and photoaged TWP was compared using earthworms ( Eisenia fetida ) as soil model organisms. The obtained results indicated that photoaging of TWP resulted in an increase of environmentally persistent free radicals (EPFRs) from 3.69 × 10 17 to 5.20 × 10 17 spin/g. Meanwhile, photoaged TWP induced the changes of toxic endpoint in E. fetide, i.e., the increase of the weight loss and death ratio from 0.0425 to 0.0756 g/worm and 23.3 to 50% compared to original TWP under a 10% concentration, respectively. Analyses of transcriptomics, antioxidant enzyme activity, and histopathology demonstrated that the enhanced toxicity was mainly due to oxidative damage, which was induced by disruption in the antioxidant defense system. Free-radical quenching and correlation analysis further suggested that the excessive production of ex vivo…

Microplastic mixtures are ubiquitously distributed in global ecosystems and include varying types. However, it remains unknown how microplastic diversity affects the biotic interactions of microbes. Here, we developed novel experiments of 600 microcosms with microplastic diversity ranging from 1 to 6 types and examined ecological networks for microbial communities in lake sediments after 2 months of incubation at 15 and 20 °C. We found that microplastic diversity generally enhanced the complexity of microbial networks at both temperatures, such as increasing network connectance and reducing average path length. This phenomenon was further confirmed by strengthened species interactions toward high microplastic diversity except for the negative interactions at 15 °C. Interestingly, increasing temperatures further exaggerated the effects of microplastic diversity on network structures, resulting in higher network connectivity and species interactions. Consistently, using species extinction simulations, we found that higher microplastic diversity and temperature led to more robust…

There is only sparse empirical data on the settling velocity of small, nonbuoyant microplastics thus far, although it is an important parameter governing their vertical transport within aquatic environments. This study reports the settling velocities of 4031 exemplary microplastic particles. Focusing on the environmentally most prevalent particle shapes, irregular microplastic fragments of four different polymer types (9-289 μm) and five discrete length fractions (50-600 μm) of common nylon and polyester fibers are investigated, respectively. All settling experiments are carried out in quiescent water by using a specialized optical imaging setup. The method has been previously validated in order to minimize disruptive factors, e.g., thermal convection or particle interactions, and thus enable the precise measurements of the velocities of individual microplastic particles (0.003-9.094 mm/s). Based on the obtained data, ten existing models for predicting a particle's terminal settling velocity are assessed. It is concluded that models, which were specifically deduced from empirical…

Peracetic acid (PAA) oxidation catalyzed by metal-free carbons is promising for advanced water decontamination. Nevertheless, developing reaction-oriented and high-performance carbocatalysts has been limited by the ambiguous understanding of the intrinsic relationship between carbon chemical/molecular structure and PAA transformation behavior. Herein, we comprehensively investigated the PAA activation using a family of well-defined sp 2 /sp 3 carbon hybrids from annealed nanodiamonds (ANDs). The activity of ANDs displays a volcano-type trend, with respect to the sp 2 /sp 3 ratio. Intriguingly, sp 3 -C-enriched AND exhibits the best catalytic activity for PAA activation and phenolic oxidation, which is different from persulfate chemistry in which the sp 2 network normally outperforms sp 3 hybridization. At the electron-rich sp 2 -C site, PAA undergoes a reduction reaction to generate a reactive complex (AND-PAA*) and induces an electron-transfer oxidation pathway. At the sp 3 -C site adjacent to C═O, PAA is oxidized to surface-confined OH* and O* successively, which ultimately…

Advanced oxidation processes (AOPs), such as hydroxyl radical (HO • )- and sulfate radical (SO 4 •– )-mediated oxidation, are attractive technologies used in water and wastewater treatments. To evaluate the treatment efficiencies of AOPs, monitoring the primary radicals (HO • and SO 4 •– ) as well as the secondary radicals generated from the reaction of HO • /SO 4 •– with water matrices is necessary. Therefore, we developed a novel chemical probe method to examine five key radicals simultaneously, including HO •, SO 4 •–, Cl •, Cl 2 •–, and CO 3 •– . Five probes, including nitrobenzene, para -chlorobenzoic acid, benzoic acid, 2,4,6-trimethylbenzoic acid, and 2,4,6-trimethylphenol, were selected in this study. Their bimolecular reaction rate constants with diverse radicals were first calibrated under the same conditions to minimize systematic errors. Three typical AOPs (UV/H 2 O 2, UV/S 2 O 8 2–, and UV/HSO 5 – ) were tested to obtain the radical steady-state concentrations. The effects of dissolved organic matter, Br –, and the probe concentration were inspected. Our results suggest…

Polymeric membranes have been widely used for liquid and gas separation in various industrial applications over the past few decades because of their exceptional versatility and high tunability. Traditional trial-and-error methods for material synthesis are inadequate to meet the growing demands for high-performance membranes. Machine learning (ML) has demonstrated huge potential to accelerate design and discovery of membrane materials. In this review, we cover strengths and weaknesses of the traditional methods, followed by a discussion on the emergence of ML for developing advanced polymeric membranes. We describe methodologies for data collection, data preparation, the commonly used ML models, and the explainable artificial intelligence (XAI) tools implemented in membrane research. Furthermore, we explain the experimental and computational validation steps to verify the results provided by these ML models. Subsequently, we showcase successful case studies of polymeric membranes and emphasize inverse design methodology within a ML-driven structured framework. Finally, we conclude…

Pharmaceutical residues in sediments are concerning as ubiquitous emerging contaminants. Pyrite is the most abundant sulfide minerals in the estuarine and coastal sediments, making it a major sink for pharmaceutical pollutants such as sulfamethoxazole (SMX). However, research on the adsorption and redox behaviors of SMX on the pyrite surface is limited. Here, we investigated the impact of the nonphotochemical process of pyrite on the fate of coexisting SMX. Remarkably, sulfur vacancies (SVs) on pyrite promoted the generation of nonradical species (hydrogen peroxide, H 2 O 2 and singlet oxygen, 1 O 2 ), thereby exhibiting prominent SMX degradation performance under darkness. Nonradical 1 O 2 contributed approximately 73.1% of the total SMX degradation. The SVs with high surrounding electron density showed an advanced affinity for adsorbing O 2 and then initiated redox reactions in the sediment electron-storing geobattery pyrite, resulting in the extensive generation of H 2 O 2 through a two-electron oxygen reduction pathway. Surface Fe(III) (hydro)oxides on pyrite facilitated the…

O system controls the long-term mobility of iron complexes in natural aquifers and other environmentally and industrially relevant systems. The fundamental mechanism controlling the formation of these phases has remained enigmatic. We develop a general partial equilibrium model, leveraging recent synchrotron-based data on the time evolution of solid Fe(III) hydroxides along with aqueous complexes. We combine thermodynamic considerations and particle-morphology-dependent kinetic rate equations under full consideration of the aqueous phase in disequilibrium with one or more of the forming minerals. The new model predicts the rate of amorphous 2-line ferrihydrite precipitation, dissolution, and overall transformation to crystalline goethite. It is found that the precipitation of goethite (i) occurs from solution and (ii) is limited by the comparatively slow dissolution of the first forming amorphous phase 2-line ferrihydrite. A generalized transformation mechanism further illustrates that differences in the kinetics of Fe(III) precipitation are controlled by the coordination…

Large amounts of wastewater containing low-concentration (<10 ppm) rare-earth ions (REIs) are discharged annually in China’s rare-earth mining and processing industry, resulting in severe environmental pollution and economic losses. Hence, achieving efficient selective recovery of low-concentration REIs from REIs-containing wastewater is essential for environmental protection and resource recovery. In this study, a pseudocapacitance system was designed for highly efficient capacitive selective recovery of REIs from wastewater using the titanium dioxide/P/C (TiO 2 /P/C) composite electrode, which exhibited over 99% recovery efficiency for REIs, such as Eu 3+, Dy 3+, Tb 3+, and Lu 3+ in mixed solution. This system maintained high efficiency and more than 90 times the enrichment concentration of REIs even after 100 cycles. Ti 4+ of TiO 2 was reduced to Ti 3+ of Ti 3 O 5 under forward voltage in the system, which trapped the electrons of phosphorus site and caused it to be oxidized to phosphate with a strong affinity for REIs, thus improving the selectivity of REIs. Under reverse…

Advanced oxidation process (AOP) wet scrubber is a powerful and clean technology for organic pollutant treatment but still presents great challenges in removing the highly toxic and hydrophobic volatile organic compounds (VOCs). Herein, we elaborately designed a bifunctional cobalt sulfide (CoS2)/activated carbon (AC) catalyst to activate peroxymonosulfate (PMS) for efficient toxic VOC removal in an AOP wet scrubber. By combining the excellent VOC adsorption capacity of AC with the highly efficient PMS activation activity of CoS2, CoS2/AC can rapidly capture VOCs from the gas phase to proceed with the SO4•– and HO• radical-induced oxidation reaction. More than 90% of aromatic VOCs were removed over a wide pH range (3–11) with low Co ion leaching (0.19 mg/L). The electron-rich sulfur vacancies and low-valence Co species were the main active sites for PMS activation. SO4•– was mainly responsible for the initial oxidation of VOCs, while HO• and O2 acted in the subsequent ring-opening and mineralization processes of intermediates. No gaseous intermediates from VOC oxidation were…

High Resolution Image Download MS PowerPoint Slide During the growing season of 2021, 201 soil samples from conventionally and organically managed fields from 10 European countries and 8 cropping systems were taken, and 192 residues of synthetic pesticides were analyzed. Pesticide residues were found in 97% of the samples, and 88% of the samples contained mixtures of at least 2 substances. A maximum of 21 substances were found in conventionally managed fields, and a maximum of 12 were found in organically managed fields. The number and concentration of pesticide residues varied significantly between conventional and organic fields in 70 and 50% of the case study sites, respectively. Application records were available for a selected number of fields ( n = 82), and these records were compared to the detected substances. Residues from 52% of the applied pesticides were detected in the soils. Only 21% of the pesticide residues detected in the soil samples were applied during the 2021 growing season. From the application data, predicted environmental concentrations of residues in soil…

The massive production of plastics causes the ubiquitous existence of microplastics (MPs) in the biota, therefore, posing exposure risks and potential health concerns to human beings. However, the exact mechanisms of MPs-induced toxicities and abnormalities are largely unknown. In this study, we developed a mouse model of gavage polystyrene microplastics (PS MPs) for 30 days. We found that PS MPs can damage the intestinal barrier, accumulate in the liver tissue, and cause injury. The liver and intestine are both highly associated with bile acid (BA) metabolism. Indeed, we found that PS MPs dysregulate BA synthesis and efflux-related gene expression in the liver, causing cholestasis. Tandemly, PS MPs alter the ratio of primary to secondary BA in the feces by affecting the composition of the intestinal flora. At last, PS MPs alter mice's fecal BA profile, which affects normal BA metabolism. Taken together, the present study provides robust data on the mechanism of toxicity of MPs causing the disturbance of BA metabolism via a 4-step gut-liver loop.

Microplastics (MPs)-derived dissolved organic matter (MPs-DOM) is becoming a non-negligible source of DOM pools in aquatic systems, but there is limited understanding about the photoreactivity of different MPs-DOM. Herein, MPs-DOM from polystyrene (PS), polyethylene terephthalate (PET), poly(butylene adipate- co -terephthalate) (PBAT), PE, and polypropylene (PP), representing aromatic, biodegradable, and aliphatic plastics, were prepared to examine their photoreactivity. Spectral and high-resolution mass spectrometry analyses revealed that PS/PET/PBAT-DOM contained more unsaturated aromatic components, whereas PE/PP-DOM was richer in saturated aliphatic components. Photodegradation experiments observed that unsaturated aromatic molecules were prone to be degraded compared to saturated aliphatic molecules, leading to a higher degradation of PS/PET/PBAT-DOM than PE/PP-DOM. PS/PET/PBAT-DOM was mainly degraded by hydroxyl ( • OH) via attacking unsaturated aromatic structures, whereas PE/PP-DOM by singlet oxygen ( 1 O 2 ) through oxidizing aliphatic side chains. The [ • OH]ss was…

Plastics are controversial due to their production from fossil fuels, emissions during production and disposal, potential toxicity, and leakage to the environment. In light of these concerns, calls to use less plastic products and move toward nonplastic alternatives are common. However, these calls often overlook the environmental impacts of alternative materials. This article examines the greenhouse gas (GHG) emission impact of plastic products versus their alternatives. We assess 16 applications where plastics are used across five key sectors: packaging, building and construction, automotive, textiles, and consumer durables. These sectors account for about 90% of the global plastic volume. Our results show that in 15 of the 16 applications a plastic product incurs fewer GHG emissions than their alternatives. In these applications, plastic products release 10% to 90% fewer emissions across the product life cycle. Furthermore, in some applications, such as food packaging, no suitable alternatives to plastics exist. These results demonstrate that care must be taken when formulating…

Increasing radical yields to reduce UV fluence requirement for achieving targeted removal of micropollutants in water would make UV-based advanced oxidation processes (AOPs) less energy demanding in the context of United Nations’ Sustainable Development Goals and carbon neutrality. We herein demonstrate that, by switching the UV radiation source from conventional low-pressure UV at 254 nm (UV 254 ) to emerging Far-UVC at 222 nm (UV 222 ), the fluence-based concentration of HO • in the UV/peroxydisulfate (UV/PDS) AOP increases by 6.40, 2.89, and 6.00 times in deionized water, tap water, and surface water, respectively, with increases in the fluence-based concentration of SO 4 •– also by 5.06, 5.81, and 55.47 times, respectively. The enhancement to radical generation is confirmed using a kinetic model. The pseudo-first-order degradation rate constants of 16 micropollutants by the UV 222 /PDS AOP in surface water are predicted to be 1.94–13.71 times higher than those by the UV 254 /PDS AOP. Among the tested water matrix components, chloride and nitrate decrease SO 4 •– but increase HO…

The increasing global attention on micro(nano)plastics (MNPs) is a result of their ubiquity in the water, air, soil, and biosphere, exposing humans to MNPs on a daily basis and threatening human health. However, crucial data on MNPs in the human body, including the sources, occurrences, behaviors, and health risks, are limited, which greatly impedes any systematic assessment of their impact on the human body. To further understand the effects of MNPs on the human body, we must identify existing knowledge gaps that need to be immediately addressed and provide potential solutions to these issues. Herein, we examined the current literature on the sources, occurrences, and behaviors of MNPs in the human body as well as their potential health risks. Furthermore, we identified key knowledge gaps that must be resolved to comprehensively assess the effects of MNPs on human health. Additionally, we addressed that the complexity of MNPs and the lack of efficient analytical methods are the main barriers impeding current investigations on MNPs in the human body, necessitating the development of…

Nanofiltration (NF) has the potential to achieve precise ion–ion separation at the subnanometer scale, which is necessary for resource recovery and a circular water economy. Fabricating NF membranes for selective ion separation is highly desirable but represents a substantial technical challenge. Dipole–dipole interaction is a mechanism of intermolecular attractions between polar molecules with a dipole moment due to uneven charge distribution, but such an interaction has not been leveraged to tune membrane structure and selectivity. Herein, we propose a novel strategy to achieve tunable surface charge of polyamide membrane by introducing polar solvent with a large dipole moment during interfacial polymerization, in which the dipole–dipole interaction with acyl chloride groups of trimesoyl chloride (TMC) can successfully intervene in the amidation reaction to alter the density of surface carboxyl groups in the polyamide selective layer. As a result, the prepared positively charged (PEI-TMC)-NH 2 and negatively charged (PEI-TMC)-COOH composite membranes, which show similarly high…

Electrochemically converting nitrate, a widely distributed nitrogen contaminant, into harmless N 2 is a feasible and environmentally friendly route to close the anthropogenic nitrogen-based cycle. However, it is currently hindered by sluggish kinetics and low N 2 selectivity, as well as scarce attention to reactor configuration. Here, we report a flow-through zero-gap electrochemical reactor that shows a high performance of nitrate reduction with 100% conversion and 80.36% selectivity of desired N 2 in the chlorine-free system at 100 mg-N·L –1 NO 3 – while maintaining a rapid reduction kinetics of 0.07676 min –1 . More importantly, the mass transport and current utilization efficiency are significantly improved by shortening the inter-electrode distance, especially in the zero-gap electrocatalytic system where the current efficiency reached 50.15% at 5 mA·cm –2 . Detailed characterizations demonstrated that during the electroreduction process, partial Cu(OH) 2 on the cathode surface was reconstructed into stable Cu/Cu 2 O as the active phase for efficient nitrate reduction. In situ…

Microbial carbon (C) use efficiency (CUE) drives soil C formation, while physical-chemical protection stabilizes subsequent microbial necromass, both shaped by soil aggregates and minerals. Soils inherit many properties from the parent material, yet the influence of lithology and associated soil geochemistry on microbial CUE and necromass stabilization remains unknow. Here, we quantified microbial CUE in well-aggregated bulk soils and crushed aggregates, as well as microbial necromass in bulk soils and the mineral-associated organic matter fraction, originating from carbonate-containing (karst) and carbonate-free (clastic rock, nonkarst) parent materials along a broad climatic gradient. We found that aggregate crushing significantly increased microbial CUE in both karst and nonkarst soils. Additionally, compared to nonkarst soils, calcium-rich karst soils increased macroaggregate stability and decreased the ratio of oligotrophic to copiotrophic microbial taxa, leading to a reduction in microbial CUE. Moreover, microbial CUE was negatively associated with iron (hydr)oxides in karst…

ADVERTISEMENT RETURN TO ARTICLES ASAPPREVViewpointNEXTMineralization or Polymerization: That Is the QuestionYing-Jie ZhangYing-Jie ZhangDepartment of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, ChinaMore by Ying-Jie ZhangView Biography and Han-Qing Yu*Han-Qing YuDepartment of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, China*[email protected]More by Han-Qing YuView Biographyhttps://orcid.org/0000-0001-5247-6244Cite this: Environ. Sci. Technol. 2024, XXXX, XXX, XXX-XXXPublication Date (Web):June 21, 2024Publication History Received12 May 2024Published online21 June 2024https://pubs.acs.org/doi/10.1021/acs.est.4c04726https://doi.org/10.1021/acs.est.4c04726article-commentaryACS Publications© 2024 American Chemical Society. This publication is available under these Terms of Use. Request reuse permissions This publication is free to access through this site. Learn MoreArticle Views-Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full…

Microplastic pollution, an emerging pollution issue, has become a significant environmental concern globally due to its ubiquitous, persistent, complex, toxic, and ever-increasing nature. As a multifaceted and diverse suite of small plastic particles with different physicochemical properties and associated matters such as absorbed chemicals and microbes, future research on microplastics will need to comprehensively consider their multidimensional attributes. Here, we introduce a novel, conceptual framework of the "microplastome", defined as the entirety of various plastic particles (<5 mm), and their associated matters such as chemicals and microbes, found within a sample and its overall environmental and toxicological impacts. As a novel concept, this paper aims to emphasize and call for a collective quantification and characterization of microplastics and for a more holistic understanding regarding the differences, connections, and effects of microplastics in different biotic and abiotic ecosystem compartments. Deriving from this lens, we present our insights and prospective…

Organic ligands have been extensively used to enhance the catalytic performance of manganese ion (Mn(II)) for peracetic acid (PAA). In this study, sodium bicarbonate (NaHCO 3 ), an economical and eco-friendly inorganic ligand, was introduced to enhance the degradation of emerging contaminants (ECs) in the Mn(II)/PAA process. NaHCO 3 could significantly improve the oxidizing ability of the Mn(II)/PAA process over the initial pH range of 3.0–11.0. Mn(V) was identified as the primary reactive species for degrading naproxen in the NaHCO 3 /Mn(II)/PAA process. HCO 3 – could complex with Mn(II) to generate Mn(II)-HCO 3 –, which has a lower redox potential to enhance the catalytic activity of Mn(II). Mn(II)-HCO 3 – reacted with PAA to produce Mn(III)-HCO 3 – and CH 3 C(O)O • . Mn(V)-HCO 3 – was generated via two-electron transfer between Mn(III)-HCO 3 – and PAA. Although organic radicals were detected in the NaHCO 3 /Mn(II)/PAA process, naproxen was mainly degraded by Mn(V)-HCO 3 – via one-electron transfer along with the formation of MnO 2 . Notably, the coexisting hydrogen peroxide was…

Excessive production of reactive oxygen species (ROS) induced by micro/nanoplastics (MPs/NPs) is highly toxic to microbes. However, the mechanisms underlying ROS generation and metabolic regulation within anaerobic guilds remain poorly understood. In this study, we investigated the effects of environmentally relevant levels of polypropylene (PP)-MPs/NPs on oxidative stress and microbial ecology during anaerobic digestion (AD). Electron paramagnetic resonance spectroscopy revealed that PP-MPs/NPs elevated the concentrations of environmentally persistent free radicals (EPFRs) and derived hydroxyl radicals ( • OH). EPFRs were identified as the primary contributors to • OH generation, as evidenced by a high Spearman correlation coefficient ( r = 0.884, p < 0.001) and free radical-quenching studies. The formation of • OH enhanced ROS production by 86.2–100.9%, resulting in decreased cellular viability and methane production (by 37.5–50.5%) at 100 mg/g TS PP-MPs/NPs. Genome-centric metagenomic and metatranscriptomic analyses suggested that PP-MPs/NPs induced the reassembly of community…

Plastics are complex chemical mixtures of polymers and various intentionally and nonintentionally added substances. Despite the well-established links between certain plastic chemicals (bisphenols and phthalates) and adverse health effects, the composition and toxicity of real-world mixtures of plastic chemicals are not well understood. To assess both, we analyzed the chemicals from 36 plastic food contact articles from five countries using nontarget high-resolution mass spectrometry and reporter-gene assays for four nuclear receptors that represent key components of the endocrine and metabolic system. We found that chemicals activating the pregnane X receptor (PXR), peroxisome proliferator receptor γ (PPARγ), estrogen receptor α (ERα), and inhibiting the androgen receptor (AR) are prevalent in plastic packaging. We detected up to 9936 chemical features in a single product and found that each product had a rather unique chemical fingerprint. To tackle this chemical complexity, we used stepwise partial least-squares regressions and prioritized and tentatively identified the chemical…

How the plastisphere mediated by the residual microplastic film in farmlands affects microhabitat systems is unclear. Here, microbial structure, assembly, and biogeochemical cycling in the plastisphere and soil in 33 typical farmland sites were analyzed by amplicon sequencing of 16S rRNA genes and ITS and metagenome analysis. The results indicated that residual microplastic film was colonized by microbes, forming a unique niche called the plastisphere. Notable differences in the microbial community structure and function were observed between soil and plastisphere. Residual microplastic film altered the microbial symbiosis and assembly processes. Stochastic processes significantly dominated the assembly of the bacterial community in the plastisphere and soil but only in the plastisphere for the fungal community. Deterministic processes significantly dominated the assembly of fungal communities only in soil. Moreover, the plastisphere mediated by the residual microplastic film acted as a preferred vector for pathogens and microorganisms associated with plastic degradation and the…

In recent years, multifarious new materials have been developed for environmental governance. Thereinto, metal organic framework (MOF)-based catalysts have been widely employed for heterogeneous catalysis because of their high porosity to confine noble metal particles faraway from aggregation. However, the potential reactions between residual species from the material synthesis process and target pollutants, which could form highly toxic byproducts, are often neglected. Herein, we took the widely used Zr-MOF, UiO-66, with highly thermal stability supported Pd catalysts as the example to investigate how the residual species in catalysts are involved in aromatic volatile organic compounds (VOCs) degradation reaction. The results showed that residual Cl species originated from the ZrCl 4 metal precursor participated in the VOC degradation reaction, leading to the production of various chlorine-containing byproducts, even the hypertoxicity dioxin precursor, dichlorobenzene. Meanwhile, the chlorination mechanism for the formation of chlorine-containing byproducts was revealed by density…

Abstract Soil organic carbon (SOC) is pivotal for both agricultural activities and climate change mitigation, and biochar stands as a promising tool for bolstering SOC and curtailing soil carbon dioxide (CO2) emissions. However, the involvements of biochar in SOC dynamics and the underlying interactions between biochar, soil microbes, minerals (notably Fe oxides), and fresh organic matter (FOM, such as plant debris) remain largely unknown, especially in agricultural soils after long-term biochar amendment. We therefore introduced FOM to soils with and without a decade-long history of biochar amendment, performed soil microcosm incubations, and evaluated carbon and iron cycling as well as microbial properties. Biochar amendment resulted in 2-fold SOC accrual over a decade and attenuated FOM-induced CO2 emissions by approximately 11% during a 56-day incubation through diverse pathways. Notably, biochar facilitated microbially driven iron reduction and subsequent Fenton-like reactions, potentially having enhanced microbial extracellular electron transfer and the carbon utilization…

Nitrous oxide (N 2 O) has a detrimental impact on the greenhouse effect, and its efficient catalytic decomposition at low temperatures remains challenging. Herein, the cobalt-based high-entropy oxide with a spinel-type structure (Co-HEO) is successfully fabricated via a facile coprecipitation method for N 2 O catalytic decomposition. The obtained Co-HEO catalyst displays more remarkable catalytic performance and higher thermal stability compared with single and binary Co-based oxides, as the temperature of 90% N 2 O decomposition ( T 90 ) is 356 °C. A series of characterization results reveal that the synergistic effect of multiple elements enhances the reducibility and augments oxygen vacancy in the high-entropy system, thus boosting the activity of the Co-HEO catalyst. Moreover, density functional theory (DFT) calculations and the temperature-programmed surface reaction (TPSR) with isotope labeling demonstrate that N 2 O decomposition on the Co-HEO catalyst follows the Langmuir–Hinshelwood (L-H) mechanism with the promotion of abundant oxygen vacancies. This work provides a…

The recently proposed partial denitrification (PD), terminating nitrate reduction to nitrite, has been regarded as a promising alternative to nitrite supplying for anammox bacteria. The most important aspect of the PD process for engineering application is the stable and continuous supply of nitrite. However, the activity of nitrate reductase is often higher than that of nitrite reductase (NIR), making it difficult to accumulate nitrite during the denitrification process. Herein, a strategy for achieving efficient and stable partial denitrification using the biosafe additive dimethyl sulfoxide (DMSO) was constructed, and the mechanism of DMSO inhibiting NIR was analyzed. DMSO addition reduced the expression of NIR gene, and 1% DMSO addition can significantly inhibit NIR enzyme activity to achieve a stable PD process. When the DMSO concentration increased to 3.5%, the NIR enzyme activity was almost inhibited with the enzyme activity of only 0.95 mg nitrite/min. However, the addition of DMSO has almost no inhibitory effect on the nitrate reductase (NAR) enzyme. The affinity constant…

Reactive oxygen species (ROS) are ubiquitous in the natural environment and play a pivotal role in biogeochemical processes. However, the spatiotemporal distribution and production mechanisms of ROS in riparian soil remain unknown. Herein, we performed uninterrupted monitoring to investigate the variation of ROS at different soil sites of the Weihe River riparian zone throughout the year. Fluorescence imaging and quantitative analysis clearly showed the production and spatiotemporal variation of ROS in riparian soils. The concentration of superoxide (O 2 •– ) was 300% higher in summer and autumn compared to that in other seasons, while the highest concentrations of 539.7 and 20.12 μmol kg –1 were observed in winter for hydrogen peroxide (H 2 O 2 ) and hydroxyl radicals ( • OH), respectively. Spatially, ROS production in riparian soils gradually decreased along with the stream. The results of the structural equation and random forest model indicated that meteorological conditions and soil physicochemical properties were primary drivers mediating the seasonal and spatial variations in…

High Resolution Image Download MS PowerPoint Slide The evaporative emissions of anthropogenic volatile organic compounds (AVOCs) are sensitive to ambient temperature. This sensitivity forms an air pollution-meteorology connection that has not been assessed on a regional scale. We parametrized the temperature dependence of evaporative AVOC fluxes in a regional air quality model and evaluated the impacts on surface ozone in the Beijing–Tianjin–Hebei (BTH) area of China during the summer of 2017. The temperature dependency of AVOC emissions drove an enhanced simulated ozone-temperature sensitivity of 1.0 to 1.8 μg m –3 K –1, comparable to the simulated ozone-temperature sensitivity driven by the temperature dependency of biogenic VOC emissions (1.7 to 2.4 μg m –3 K –1 ). Ozone enhancements driven by temperature-induced AVOC increases were localized to their point of emission and were relatively more important in urban areas than in rural regions. The inclusion of the temperature-dependent AVOC emissions in our model improved the simulated ozone-temperature sensitivities on days of…

Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-C 3 N 4 ) nanomaterials were used to construct Fe–N x sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-C 3 N 4 catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.0843 min –1, marking a 21.6-fold improvement over the carbon nitride (CN)-based PAA system. DFT calculations further corroborate the superior adsorption capacity of the Fe–N x sites for PAA, facilitating its activation. Charge transfer mechanisms, with PAA serving as an electron acceptor, were identified as the source of high-valent iron-oxo species. Moreover, the BNQDs-FCN system preferentially targets oxygen-containing functional groups in antibiotic structures, elucidating the selective attack patterns of these highly electrophilic species. This research not only elucidates the…

ADVERTISEMENT RETURN TO ARTICLES ASAPPREVViewpointNEXTThe Need to Include a Fluorine Mass Balance in the Development of Effective Technologies for PFAS DestructionSanne J. Smith*Sanne J. SmithDepartment of Water Management, Delft University of Technology, Stevinweg 1, 2628 CN Delft, The Netherlands*[email protected]More by Sanne J. SmithView Biographyhttps://orcid.org/0000-0002-3487-0528, Mélanie LauriaMélanie LauriaDepartment of Environmental Science, Stockholm University, Svante Arrhenius Väg 8, 10691 Stockholm, SwedenMore by Mélanie Lauriahttps://orcid.org/0000-0002-5304-650X, Christopher P. HigginsChristopher P. HigginsDepartment of Civil and Environmental Engineering, Colorado School of Mines, 1500 Illinois Street, Golden, Colorado 80401, United StatesMore by Christopher P. Higginshttps://orcid.org/0000-0001-6220-8673, Kurt D. PennellKurt D. PennellSchool of Engineering, Brown University, 184 Hope Street, Box D, Providence, Rhode Island 02912, United StatesMore by Kurt D. Pennellhttps://orcid.org/0000-0002-5788-6397, Jens BlotevogelJens BlotevogelCommonwealth Scientific and…

Seawater reverse osmosis (SWRO) desalination facilities produce freshwater and, at the same time, discharge hypersaline brine that often includes various chemical additives such as antiscalants and coagulants. This dense brine can sink to the sea bottom and creep over the seabed, reaching up to 5 km from the discharge point. Previous reviews have discussed the effects of SWRO desalination brine on various marine ecosystems, yet little attention has been paid to the impacts on benthic habitats. This review comprehensibly discusses the effects of SWRO brine discharge on marine benthic fauna and flora. We review previous studies that indicated a suite of impacts by SWRO brine on benthic organisms, including bacteria, seagrasses, polychaetes, and corals. The effects within the discharge mixing zones range from impaired activities and morphological deformations to changes in the community composition. Recent modeling work demonstrated that brine could spread over the seabed, beyond the mixing zone, for up to several tens of kilometers and impair nutrient fluxes from the sediment to the…

Abstract Organic pollutants removal via a polymerization transfer (PT) pathway based on the use of single-atom catalysts (SACs) promises efficient water purification with minimal energy/chemical inputs. However, the precise engineering of such catalytic systems toward PT decontamination is still challenging, and the conventional SACs are plagued by low structural stability of carbon material support. Here, we adopted magnesium oxide (MgO) as a structurally stable alternative for loading single copper (Cu) atoms to drive peroxymonosulfate-based Fenton-like reactions. Through fine-tuning the Cu atom steric location from lattice-embedding to surface-loading, the system exhibited a fundamental transition in the catalytic pathways toward the PT process and drastically improved decontamination efficiency. The catalytic pathway change was mainly ascribed to a downshifted d-band center of the Cu atoms. The optimized catalyst achieved complete, rapid removal of phenolic compounds from water via nearly 100% PT pathway, accompanied by high oxidant utilization efficiency surpassing most…

Lithium (Li) is an important resource that drives sustainable mobility and renewable energy. Its demand is projected to continue to increase in the coming decades. However, the risk of Li pollution has also emerged as a global concern. Here, we investigated the pollution characteristics, sources, exposure levels, and associated health risks of Li in the Jinjiang River basin, the largest area for Li 2 CO 3 production in China. Our results revealed the dominant role of Li extraction activities in the pollution of the river, with over 95% of dissolved Li in downstream river water being emitted from this source. Moreover, the Li concentration in aquatic plants (i.e., water hyacinth) and animals (i.e., fish) significantly increased from upstream to downstream areas, indicating a significant risk to local aquatic ecosystems. More importantly, our study found that local residents were suffering potential chronic noncarcinogenic health risks primarily from consuming contaminated water and vegetables. We also investigated the pollution characteristics of associated elements present in Li…

The feasibility of a synergistic endogenous partial denitrification-phosphorus removal coupled anammox (SEPD-PR/A) system was investigated in a modified anaerobic baffled reactor (mABR) for synchronous carbon, nitrogen, and phosphorus removal. The mABR comprising four identical compartments (i.e., C1–C4) was inoculated with precultured denitrifying glycogen-accumulating organisms (DGAOs), denitrifying polyphosphate-accumulating organisms, and anammox bacteria. After 136 days of operation, the chemical oxygen demand (COD), total nitrogen, and phosphorus removal efficiencies reached 88.6 ± 1.0, 97.2 ± 1.5, and 89.1 ± 4.2%, respectively. Network-based analysis revealed that the biofilmed community demonstrated stable nutrient removal performance under oligotrophic conditions in C4. The metagenome-assembled genomes (MAGs) such as MAG106, MAG127, MAG52, and MAG37 annotated as denitrifying phosphorus-accumulating organisms (DPAOs) and MAG146 as a DGAO were dominated in C1 and C2 and contributed to 89.2% of COD consumption. MAG54 and MAG16 annotated as Candidatus_Brocadia (total relative…

Microplastics threaten soil ecosystems, strongly influencing carbon (C) and nitrogen (N) contents. Interactions between microplastic properties and climatic and edaphic factors are poorly understood. We conducted a meta-analysis to assess the interactive effects of microplastic properties (type, shape, size, and content), native soil properties (texture, pH, and dissolved organic carbon (DOC)) and climatic factors (precipitation and temperature) on C and N contents in soil. We found that low-density polyethylene reduced total nitrogen (TN) content, whereas biodegradable polylactic acid led to a decrease in soil organic carbon (SOC). Microplastic fragments especially depleted TN, reducing aggregate stability, increasing N-mineralization and leaching, and consequently increasing the soil C/N ratio. Microplastic size affected outcomes; those <200 μm reduced both TN and SOC contents. Mineralization-induced nutrient losses were greatest at microplastic contents between 1 and 2.5% of soil weight. Sandy soils suffered the highest microplastic contamination-induced nutrient depletion.…

The denitrifying sulfur (S) conversion-associated enhanced biological phosphorus removal (DS-EBPR) process for treating saline wastewater is characterized by its unique microbial ecology that integrates carbon (C), nitrogen (N), phosphorus (P), and S biotransformation. However, operational instability arises due to the numerous parameters and intricates bacterial interactions. This study introduces a two-stage interpretable machine learning approach to predict S conversion-driven P removal efficiency and optimize DS-EBPR process. Stage one utilized the XGBoost regression model, achieving an R 2 value of 0.948 for predicting sulfate reduction (SR) intensity from anaerobic parameters with feature engineering. Stage two involved the CatBoost classification and regression model integrating anoxic parameters with the predicted SR values for predicting P removal, reaching an accuracy of 94% and an R 2 value of 0.93, respectively. This study identified key environmental factors, including SR intensity (20–45 mg S/L), influent P concentration (<9.0 mg P/L), mixed liquor volatile suspended…

While the extent of environmental contamination by per- and polyfluoroalkyl substances (PFAS) has mobilized considerable efforts around the globe in recent years, publicly available data on PFAS in Europe were very limited. In an unprecedented experiment of "expert-reviewed journalism" involving 29 journalists and seven scientific advisers, a cross-border collaborative project, the "Forever Pollution Project" (FPP), drew on both scientific methods and investigative journalism techniques such as open-source intelligence (OSINT) and freedom of information (FOI) requests to map contamination across Europe, making public data that previously had existed as "unseen science". The FPP identified 22,934 known contamination sites, including 20 PFAS manufacturing facilities, and 21,426 "presumptive contamination sites", including 13,745 sites presumably contaminated with fluorinated aqueous film-forming foam (AFFF) discharge, 2911 industrial facilities, and 4752 sites related to PFAS-containing waste. Additionally, the FPP identified 231 "known PFAS users", a new category for sites with an…

Environmental pollutants have been recognized for their ability to induce various adverse outcomes in both the environment and human health, including inflammation, apoptosis, necrosis, pyroptosis, and autophagy. Understanding these biological mechanisms has played a crucial role in risk assessment and management efforts. However, the recent identification of ferroptosis as a form of programmed cell death has emerged as a critical mechanism underlying pollutant-induced toxicity. Numerous studies have demonstrated that fine particulates, heavy metals, and organic substances can trigger ferroptosis, which is closely intertwined with lipid, iron, and amino acid metabolism. Given the growing evidence linking ferroptosis to severe diseases such as heart failure, chronic obstructive pulmonary disease, liver injury, Parkinson's disease, Alzheimer's disease, and cancer, it is imperative to investigate the role of pollutant-induced ferroptosis. In this review, we comprehensively analyze various pollutant-induced ferroptosis pathways and intricate signaling molecules and elucidate their…

In this study, a sample of 2-methylimidazole zinc salt (ZIF-8) demonstrated high selectivity for the recovery of heavy rare earth elements (REEs) from real rare earth mining wastewater. Results show that the distribution coefficient values of Y 3+ (4.02 × 10 4 mL·g –1 ), Gd 3+ (7.8 × 10 4 mL·g –1 ), and Dy 3+ (6.8 × 10 4 mL·g –1 ) are orders of magnitude higher than those of K + (359.51 mL·g –1 ), Mn 2+ (266.67 mL·g –1 ), Ca 2+ (396.42 mL·g –1 ), and Mg 2+ (239.48 mL·g –1 ). Moreover, the desorption efficiency of heavy REEs exceeded 40%. Advanced characterizations and density functional theory (DFT) calculations were utilized to elucidate that the heavy REEs were more likely to bind to the nitrogen atoms of imidazole groups on ZIF-8 compared to non-REEs. Furthermore, the adsorption and desorption of heavy REEs primarily depend on the chemical interaction confirmed by adsorption kinetics, isotherm model, and thermodynamic analysis, which involves the dissociation of water and the formation of REE–O bonds. Finally, the ZIF-8 exhibits a remarkable recovery efficiency of over 40% for…

Research on plant-nanomaterial interactions has greatly advanced over the past decade. One particularly fascinating discovery encompasses the immunomodulatory effects in plants. Due to the low doses needed and the comparatively low toxicity of many nanomaterials, nanoenabled immunomodulation is environmentally and economically promising for agriculture. It may reduce environmental costs associated with excessive use of chemical pesticides and fertilizers, which can lead to soil and water pollution. Furthermore, nanoenabled strategies can enhance plant resilience against various biotic and abiotic stresses, contributing to the sustainability of agricultural ecosystems and the reduction of crop losses due to environmental factors. While nanoparticle immunomodulatory effects are relatively well-known in animals, they are still to be understood in plants. Here, we provide our perspective on the general components of the plant's immune system, including the signaling pathways, networks, and molecules of relevance for plant nanomodulation. We discuss the recent scientific progress in…

Thin film composite (TFC) polyamide membranes have been widely applied for environmental applications, such as desalination and water reuse. The separation performance of TFC polyamide membranes strongly depends on their nanovoid-containing roughness morphology. These nanovoids not only influence the effective filtration area of the polyamide film but also regulate the water transport pathways through the film. Although there have been ongoing debates on the formation mechanisms of nanovoids, a nanofoaming theory─stipulating the shaping of polyamide roughness morphology by nanobubbles of degassed CO 2 and the vapor of volatile solvents─has gained much attention in recent years. In this review, we provide a comprehensive summary of the nanofoaming mechanism, including related fundamental principles and strategies to tailor nanovoid formation for improved membrane separation performance. The effects of nanovoids on the fouling behaviors of TFC membranes are also discussed. In addition, numerical models on the role of nanovoids in regulating the water transport pathways toward improved…

The concerns about the fate of per- and polyfluoroalkyl substances (PFAS) in the atmosphere are continuously growing. In this study, size-fractionated particles, gas, and rainwater samples were simultaneously collected in Shijiazhuang, China, to investigate the multiphase distribution of PFAS in the atmosphere. Perfluoroalkyl carboxylic acids (PFCAs) dominated the total concentration of PFAS in atmospheric media. A strong positive relationship (0.79 < R 2 < 0.99) was observed between the concentration of PFCAs and organic matter fraction ( f OM ) in different particle size fractions, while no such relationship for perfluoroalkyl sulfonic acids (PFSAs) and f OM, suggesting f OM may be an important factor influencing the size-dependent distribution of PFCAs. Temperature played a key role in the gas-particle partitioning of PFAS, while it did not significantly affect their particle-size-dependent distribution. The associative concentration fluctuation of particle and particle-bound PFAS during precipitation suggested that precipitation scavenging was an important mechanism for the…

The antioxidant N -(1,3-Dimethylbutyl)- N ′-phenyl- p -phenylenediamine (6PPD) and its oxidized quinone product 6PPD-quinone (6PPD-Q) in rubber have attracted attention due to the ecological risk that they pose. Both 6PPD and 6PPD-Q have been detected in various environments that humans cohabit. However, to date, a clear understanding of the biotransformation of 6PPD-Q and a potential biomarker for exposure in humans are lacking. To address this issue, this study presents a comprehensive analysis of the extensive biotransformation of 6PPD-Q across species, encompassing both in vitro and in vivo models. We have tentatively identified 17 biotransformation metabolites in vitro, 15 in mice in vivo, and confirmed the presence of two metabolites in human urine samples. Interestingly, different biotransformation patterns were observed across species. Through semiquantitative analysis based on peak areas, we found that almost all 6PPD-Q underwent biotransformation within 24 h of exposure in mice, primarily via hydroxylation and subsequent glucuronidation. This suggests a rapid metabolic…

Recent investments in "clean" hydrogen as an alternative to fossil fuels are driven by anticipated climate benefits. However, most climate benefit calculations do not adequately account for all climate warming emissions and impacts over time. This study reanalyzes a previously published life cycle assessment as an illustrative example to show how the climate impacts of hydrogen deployment can be far greater than expected when including the warming effects of hydrogen emissions, observed methane emission intensities, and near-term time scales; this reduces the perceived climate benefits upon replacement of fossil fuel technologies. For example, for blue (natural gas with carbon capture) hydrogen pathways, the inclusion of upper-end hydrogen and methane emissions can yield an increase in warming in the near term by up to 50%, whereas lower-end emissions decrease warming impacts by at least 70%. For green (renewable-based electrolysis) hydrogen pathways, upper-end hydrogen emissions can reduce climate benefits in the near term by up to 25%. We also consider renewable electricity…

CO 2 -enhanced oil recovery (CO 2 -EOR) is widely used in reservoir development, but its implementation is often limited by scarce pure CO 2 sources and high carbon capture costs. Flue gas from steam injection boilers typically contains 10–15% CO 2 and 80–85% N 2, both of which serve as effective gas displacement agents. Injecting flue gas or CO 2 /N 2 mixtures into reservoirs can reduce carbon emissions, sequester CO 2, and enhance recovery. Therefore, this study proposes a concept of enriching rather than capturing flue gas for storage, with a focus on how N 2 as an impurity affects the safety of CO 2 storage. This study examines interactions between gas mixtures with varying CO 2 enrichment rates (with N 2 impurities) and minerals. It performs microarea analyses of aged rocks using ultradepth-of-field microscope and atomic force microscopy (AFM), assesses calcite wettability via contact angle tests, and evaluates CO 2 storage column height under experimental conditions. Results indicate that with a CO 2 enrichment of at least 50%, adding N 2 creates additional dissolution pits on…

Wildfires are becoming more frequent and intense on a global scale, raising concerns about their acute and long-term effects on human health. We conducted a systematic review of the current epidemiological evidence on wildfire health risks and a meta-analysis to investigate the association between wildfire smoke exposure and various health outcomes. We discovered that wildfire smoke increases the risk of premature deaths and respiratory morbidity in the general population. Meta-analysis of cause-specific mortality and morbidity revealed that wildfire smoke had the strongest associations with cardiovascular mortality (RR: 1.018, 95% CI: 1.014-1.021), asthma hospitalization (RR: 1.054, 95% CI: 1.026-1.082), and asthma emergency department visits (RR: 1.117, 95% CI: 1.035-1.204) in the general population. Subgroup analyses of age found that adults and elderly adults were more susceptible to the cardiopulmonary effects of wildfire smoke. Next, we systematically addressed the toxicological mechanisms of wildfire smoke, including direct toxicity, oxidative stress, inflammatory reactions,…

The Yangtze River Estuary is the terminal sink of terrestrial per- and polyfluoroalkyl substances (PFAS) from the Yangtze River, while the environmental fate characteristics of legacy and emerging PFAS around this region have rarely been discussed. Here, 24 targeted PFAS in seawater, sediments, suspended particulate matter (SPM), and plankton in the offshore region adjacent to this estuary were investigated. The three dominant PFAS in all phases were perfluorooctanoic acid (PFOA, 23.8–61.9%), perfluorobutanoic acid (PFBA, 23.6–42.8%), and perfluoro(2-methyl-3-oxahexanoic) acid (HFPO-DA, 6.1–12.1%), and perfluoro-1-butane sulfonamide (FBSA, 0.1–7.3%) was first detected. The horizontal distributions of PFAS were dependent on salinity and disturbed by multiple water masses, while the vertical variations could be explained by their different partitioning characteristics in the water-SPM-sediment system (partition coefficients, Log K d and Log K oc ) and plankton (bioaccumulation factors, Log BAF). Although physical mixing was the major driver for PFAS settling (>83.7%), the absolute…

Although exogenous chemicals frequently exhibit a biphasic response in regulating plant growth, characterized by low-dose stimulation and high-dose inhibition, the underlying mechanisms remain elusive. This study demonstrates, for the first time, the compensatory function of rhizosphere microbiota in assisting plants to withstand pesticide stress. It was observed that pak choi plants, in response to foliar-spraying imidacloprid at both low and high doses, could increase the total number of rhizosphere bacteria and enrich numerous beneficial bacteria. These bacteria have capabilities for promoting plant growth and degrading the pesticide, such as Nocardioides, Brevundimonas, and Sphingomonas . The beneficial bacterial communities were recruited by stressed plants through increasing the release of primary metabolites in root exudates, such as amino acids, fatty acids, and lysophosphatidylcholines. At low doses of pesticide application, the microbial compensatory effect overcame pesticide stress, leading to plant growth promotion. However, with high doses of pesticide application, the…

The semiconductor industry has claimed that perfluorooctanesulfonate (PFOS), a persistent per- and polyfluoroalkyl substance (PFAS), has been eliminated from semiconductor production; however, information about the use of alternative compounds remains limited. This study aimed to develop a nontarget approach to discovering diverse PFAS substitutions used in semiconductor manufacturing. A distinct fragment-based approach has been established to identify the hydrophobic and hydrophilic features of acidic and neutral fluorosurfactants through fragments and neutral losses, including those outside the homologous series. Ten sewage samples from 5 semiconductor plants were analyzed with target and nontarget analysis. Among the 20 identified PFAS spanning 12 subclasses, 15 were reported in semiconductor sewage for the first time. The dominant identified PFAS compounds were C4 sulfonamido derivatives, including perfluorobutane sulfonamido ethanol (FBSE), perfluorobutane sulfonamide (FBSA), and perfluorobutane sulfonamido diethanol (FBSEE diol), with maximum concentrations of 482 μg/L, 141…

Microplastics (MPs), as an emerging contaminants category, can undergo complex aging in a variety of environmental matrices in which the chemical bonds of polymer molecules can be broken to form free radicals. While the existence of free radicals in aged plastics has been known for over half a century, only recently has significant research on a new type of environmentally risky substance, namely environmentally persistent free radicals (EPFRs), present in aged MPs and their environmental effects, been started, but it is still in its infancy. To address these issues, this work examines EPFR generation on MPs and their environmental effect by reviewing publications from 2012 to 2023. The aging processes and mechanisms of MPs in the environment are first summarized. Then, the occurrence and formation mechanisms of EPFRs on aged MPs are specifically discussed. Additionally, the reactivity of EPFRs on aging MPs and their influencing factors are comprehensively considered, such as their physicochemical properties, oxygen content, and coexisting substances. Due to their reactivity, EPFRs…

Volatile organic compounds (VOCs) have caused serious harm to human health and ecological environment, and have received much attention in recent years. Despite the successful applications of catalytic combustion of VOCs as the core technology of VOCs removal in industry, the development of efficient catalysts that can mineralize VOCs into nontoxic CO 2 and H 2 O at low temperatures remains a great challenge. Recent studies show that spinel-based materials as efficient catalysts were extensively used in the catalytic oxidation VOCs field due to their synergistic effect, manifold compositions, and electron configurations. However, most of the pollutants are complex, consisting of multiple VOCs, water vapor, CO 2, SO 2 and other substances, which presents a significant challenge in constructing highly active and stable catalysts. To meet the future demand for efficient catalysts capable of removing various types of VOCs, it is urgent to rationally design and scientifically prepare spinel catalysts based on existing knowledge. This work reviews the research and development of various…

Amidst tightening regulations, the proliferation of next-generation per- and polyfluoroalkyl substances (PFAS) necessitates a deeper understanding of their environmental fate and potential risks. Here, we conducted a comprehensive assessment of PFAS in the water and sediment of Taihu Lake, incorporating both nontarget and target screening, seasonal and geographical variation analysis, and risk prioritization. A total of 58 PFAS from 13 classes were identified, revealing complex PFAS contamination. In addition to short-chain perfluoroalkyl carboxylates (PFCAs) and sulfonates (PFSAs), bis(trifluoromethanesulfonyl)imide (Ntf2) and perfluoro-2,5-dimethyl-3,6-dioxo-heptanoic acid (C7 HFPO-TA) exhibited relatively high concentrations in water, with median values of 21.7 and 5.72 ng/L, respectively. Seasonal and geographical variation analysis revealed elevated levels of C7 HFPO-TA, Ntf2, and perfluorohexanoic acid (PFHxA) in the northeastern areas, suggesting transport via water diversion project. Multicriteria risk prioritization identified four high priority PFAS (Ntf2, C7 HFPO-TA,…

Further reducing total nitrogen (TN) and total phosphorus (TP) in the secondary effluent needs to be realized effectively and in an eco-friendly manner. Herein, four pyrite/sawdust composite-based biofilters were established to treat simulated secondary effluent for 304 days. The results demonstrated that effluent TN and TP concentrations from biofilters under the optimal hydraulic retention time (HRT) of 3.5 h were stable at <2.0 and 0.1 mg/L, respectively, and no significant differences were observed between inoculated sludge sources. The pyrite/sawdust composite-based biofilters had low N 2 O, CH 4, and CO 2 emissions, and the effluent’s DOM was mainly composed of five fluorescence components. Moreover, mixotrophic denitrifiers ( Thiothrix ) and sulfate-reducing bacteria ( Desulfosporosinus ) contributing to microbial nitrogen and sulfur cycles were enriched in the biofilm. Co-occurrence network analysis deciphered that Chlorobaculum and Desulfobacterales were key genera, which formed an obvious sulfur cycle process that strengthened the denitrification capacity. The higher…

Plastic waste has emerged as a serious issue due to its impact on environmental degradation and resource scarcity. Plastic recycling, especially of halogen-containing plastics, presents challenges due to potential secondary pollution and lower-value implementations. Chemical recycling via pyrolysis is the most versatile and robust approach for combating plastic waste. In this Review, we present recent advancements in halogen-plastic pyrolysis for resource utilization and the potential pathways from "reducing to recycling to upcycling" halogens. We emphasize the advanced management of halogen-plastics through copyrolysis with solid wastes (waste polymers, biomass, coal, etc.), which is an efficient method for dealing with mixed wastes to obtain high-value products while reducing undesirable substances. Innovations in catalyst design and reaction configurations for catalytic pyrolysis are comprehensively evaluated. In particular, a tandem catalysis system is a promising route for halogen removal and selective conversion of targeted products. Furthermore, we propose novel insights…

Microplastics are routinely ingested and inhaled by humans and other organisms. Despite the frequency of plastic exposure, little is known about its health consequences. Of particular concern are plastic additives─chemical compounds that are intentionally or unintentionally added to plastics to improve functionality or as residual components of plastic production. Additives are often loosely bound to the plastic polymer and may be released during plastic exposures. To better understand the health effects of plastic additives, we performed a comprehensive literature search to compile a list of 2,712 known plastic additives. Then, we performed an integrated toxicogenomic analysis of these additives, utilizing cancer classifications and carcinogenic expression pathways as a primary focus. Screening these substances across two chemical databases revealed two key observations: (1) over 150 plastic additives have known carcinogenicity and (2) the majority (∼90%) of plastic additives lack data on carcinogenic end points. Analyses of additive usage patterns pinpointed specific polymers,…

High Resolution Image Download MS PowerPoint Slide Methane is a major contributor to anthropogenic greenhouse gas emissions. Identifying large sources of methane, particularly from the oil and gas sectors, will be essential for mitigating climate change. Aircraft-based methane sensing platforms can rapidly detect and quantify methane point-source emissions across large geographic regions, and play an increasingly important role in industrial methane management and greenhouse gas inventory. We independently evaluate the performance of five major methane-sensing aircraft platforms: Carbon Mapper, GHGSat-AV, Insight M, MethaneAIR, and Scientific Aviation. Over a 6 week period, we released metered gas for over 700 single-blind measurements across all five platforms to evaluate their ability to detect and quantify emissions that range from 1 to over 1,500 kg(CH 4 )/h. Aircraft consistently quantified releases above 10 kg(CH 4 )/h, and GHGSat-AV and Insight M detected emissions below 5 kg(CH 4 )/h. Fully blinded quantification estimates for platforms using downward-facing imaging…

Ecological role of the viral community on the fate of antibiotic resistance genes (ARGs) (reduction vs proliferation) remains unclear in anaerobic digestion (AD). Metagenomics revealed a dominance of Siphoviridae and Podoviridae among 13,895 identified viral operational taxonomic units (vOTUs) within AD, and only 21 of the vOTUs carried ARGs, which only accounted for 0.57 ± 0.43% of AD antibiotic resistome. Conversely, ARGs locating on plasmids and integrative and conjugative elements accounted for above 61.0%, indicating a substantial potential for conjugation in driving horizontal gene transfer of ARGs within AD. Virus-host prediction based on CRISPR spacer, tRNA, and homology matches indicated that most viruses (80.2%) could not infect across genera. Among 480 high-quality metagenome assembly genomes, 95 carried ARGs and were considered as putative antibiotic-resistant bacteria (pARB). Furthermore, lytic phages of 66 pARBs were identified and devoid of ARGs, and virus/host abundance ratios with an average value of 71.7 indicated extensive viral activity and lysis. The infectivity…

Tire wear particles (TWPs), generated from tire abrasion, contribute significantly to environmental contamination. The toxicity of TWPs to organisms has raised significant concerns, yet their effects on terrestrial plants remain unclear. Here, we investigated the long-term impact of pristine and naturally aged TWPs on water spinach ( Ipomoea aquatica ) and its rhizospheric soil. The results indicated that natural aging reduced the toxicity of TWPs, as evidenced by decreased levels of polycyclic aromatic hydrocarbons (PAHs) in soil and TWPs themselves. Consequently, aged TWPs were found to enhance the plant growth and chlorophyll content, whereas pristine TWPs increased the plant stress. Furthermore, aged TWPs improved soil organic matter (SOM) and total organic carbon (TOC), thereby boosting the microbial enzymes involved in nitrogen cycling. Metabolomic analysis revealed that aged TWPs upregulated key pathways related to carbon and nitrogen metabolism, enhancing plant growth and stress responses. Additionally, rhizosphere bacterial diversity was higher under aged TWPs, favoring…

Previous studies have detected microplastics (MPs) in human biological samples, such as lungs, alveolar lavage fluid, and thrombus. However, whether MPs induce health effects after inhalation are unclear. In this study, fluorescent polystyrene microplastics (PS-MPs) were found in the thymus, spleen, testes, liver, kidneys, and brain on day 1 or day 3 after one intratracheal instillation. Furthermore, mice showed inflammation in multiple organs, manifested as obvious infiltration of neutrophils and macrophages, increased Toll-like receptors (TLRs), myeloid differentiation primary response protein 88 (MyD88) and nuclear factor-κB (NF-κB), as well as proinflammatory cytokines (tumor necrosis factor (TNF)-α and interleukin (IL)-1β) in the lungs, thymus, spleen, liver, and kidneys after four intratracheal instillations of PS-MPs at once every 2 weeks. Hepatic and renal function indexes were also increased. Subsequently, the inflammatory response in multiple murine organs was significantly alleviated by TLR2 and TLR4 inhibitors. Unexpectedly, we did not find any elevated secretion of…

As regulatory standards for per- and polyfluoroalkyl substances (PFAS) become increasingly stringent, innovative water treatment technologies are urgently demanded for effective PFAS removal. Reported sorbents often exhibit limited affinity for PFAS and are frequently hindered by competitive background substances. Recently, fluorinated sorbents (abbreviated as fluorosorbents) have emerged as a potent solution by leveraging fluorine-fluorine (F···F) interactions to enhance selectivity and efficiency in PFAS removal. This review delves into the designs and applications of fluorosorbents, emphasizing how F···F interactions improve PFAS binding affinity. Specifically, the existence of F···F interactions results in removal efficiencies orders of magnitude higher than other counterpart sorbents, particularly under competitive conditions. Furthermore, we provide a detailed analysis of the fundamental principles underlying F···F interactions and elucidate their synergistic effects with other sorption forces, which contribute to the enhanced efficacy and selectivity. Subsequently, we examine…

Short carbon chain alkanes, as typical volatile organic compounds (VOCs), have molecular structural stability and low molecular polarity, leading to an enormous challenge in the catalytic oxidation of propane. Although Ru-based catalysts exhibit a surprisingly high activity for the catalytic oxidation of propane to CO 2 and H 2 O, active RuO x species are partially oxidized and sintered during the oxidation reaction, leading to a decrease in catalytic activity and significantly inhibiting their application in industrial processes. Herein, the Ru/Ce@Co catalyst is synthesized with a specific structure, in which cerium dioxide is dispersed in a thin layer on the surface of Co 3 O 4, and Ru nanoparticles fall preferentially on cerium oxide with high dispersity. Compared with the Ru/CeO 2 and Ru/Co 3 O 4 catalysts, the Ru/Ce@Co catalyst demonstrates excellent catalytic activity and stability for the oxidation of propane, even under severe operating conditions, such as recycling reaction, high space velocity, a certain degree of moisture, and high temperature. Benefiting from this…

Volatile organic compounds (VOCs) are considered to be the most recalcitrant gaseous pollutants due to their high toxicity, diversity, complexity, and stability. Gas-solid catalytic oxidation methods have been intensively studied for VOC treatment while being greatly hampered by energy consumption, catalyst deactivation, and byproduct formation. Recently, aqueous advanced oxidation processes (AOPs) have attracted increasing interest for the deep oxidation of VOCs at room temperature, owing to the generation of abundant reactive oxygen species (ROS). However, current reviews mainly focus on VOC degradation performance and have not clarified the specific reaction process, degradation products, and paths of VOCs in different AOPs. This study systematically reviews recent advances in the application of aqueous AOPs for gaseous VOC removal. First, the VOC gas-liquid mass transfer and chemical oxidation processes are presented. Second, the latest research progress of VOC removal by various ROS is reviewed to study their degradation performances, pathways, and mechanisms. Finally, the…