The 100 most-cited articles in Nature Communications, 2024

Medical image segmentation is a critical component in clinical practice, facilitating accurate diagnosis, treatment planning, and disease monitoring. However, existing methods, often tailored to specific modalities or disease types, lack generalizability across the diverse spectrum of medical image segmentation tasks. Here we present MedSAM, a foundation model designed for bridging this gap by enabling universal medical image segmentation. The model is developed on a large-scale medical image dataset with 1,570,263 image-mask pairs, covering 10 imaging modalities and over 30 cancer types. We conduct a comprehensive evaluation on 86 internal validation tasks and 60 external validation tasks, demonstrating better accuracy and robustness than modality-wise specialist models. By delivering accurate and efficient segmentation across a wide spectrum of tasks, MedSAM holds significant potential to expedite the evolution of diagnostic tools and the personalization of treatment plans.

Accurate state-of-health (SOH) estimation is critical for reliable and safe operation of lithium-ion batteries. However, reliable and stable battery SOH estimation remains challenging due to diverse battery types and operating conditions. In this paper, we propose a physics-informed neural network (PINN) for accurate and stable estimation of battery SOH. Specifically, we model the attributes that affect the battery degradation from the perspective of empirical degradation and state space equations, and utilize neural networks to capture battery degradation dynamics. A general feature extraction method is designed to extract statistical features from a short period of data before the battery is fully charged, enabling our method applicable to different battery types and charge/discharge protocols. Additionally, we generate a comprehensive dataset consisting of 55 lithium-nickel-cobalt-manganese-oxide (NCM) batteries. Combined with three other datasets from different manufacturers, we use a total of 387 batteries with 310,705 samples to validate our method. The mean absolute…

Silicon photonics has developed into a mainstream technology driven by advances in optical communications. The current generation has led to a proliferation of integrated photonic devices from thousands to millions-mainly in the form of communication transceivers for data centers. Products in many exciting applications, such as sensing and computing, are around the corner. What will it take to increase the proliferation of silicon photonics from millions to billions of units shipped? What will the next generation of silicon photonics look like? What are the common threads in the integration and fabrication bottlenecks that silicon photonic applications face, and which emerging technologies can solve them? This perspective article is an attempt to answer such questions. We chart the generational trends in silicon photonics technology, drawing parallels from the generational definitions of CMOS technology. We identify the crucial challenges that must be solved to make giant strides in CMOS-foundry-compatible devices, circuits, integration, and packaging. We identify challenges…

Extracting structured knowledge from scientific text remains a challenging task for machine learning models. Here, we present a simple approach to joint named entity recognition and relation extraction and demonstrate how pretrained large language models (GPT-3, Llama-2) can be fine-tuned to extract useful records of complex scientific knowledge. We test three representative tasks in materials chemistry: linking dopants and host materials, cataloging metal-organic frameworks, and general composition/phase/morphology/application information extraction. Records are extracted from single sentences or entire paragraphs, and the output can be returned as simple English sentences or a more structured format such as a list of JSON objects. This approach represents a simple, accessible, and highly flexible route to obtaining large databases of structured specialized scientific knowledge extracted from research papers.

Abstract Water security is at stake today. While climate changes influence water availability, urbanization and agricultural activities have led to increasing water demand as well as pollution, limiting safe water use. We conducted a global assessment of future clean-water scarcity for 2050s by adding the water pollution aspect to the classical water quantity-induced scarcity assessments. This was done for >10,000 sub-basins focusing on nitrogen pollution in rivers by integrating land-system, hydrological and water quality models. We found that water pollution aggravates water scarcity in >2000 sub-basins worldwide. The number of sub-basins with water scarcity triples due to future nitrogen pollution worldwide. In 2010, 984 sub-basins are classified as water scarce when considering only quantity-induced scarcity, while 2517 sub-basins are affected by quantity & quality-induced scarcity. This number even increases to 3061 sub-basins in the worst case scenario in 2050. This aggravation means an extra 40 million km 2 of basin area and 3 billion more people that may potentially face…

Artificial Intelligence (AI) is currently experiencing a bloom driven by deep learning (DL) techniques, which rely on networks of connected simple computing units operating in parallel. The low communication bandwidth between memory and processing units in conventional von Neumann machines does not support the requirements of emerging applications that rely extensively on large sets of data. More recent computing paradigms, such as high parallelization and near-memory computing, help alleviate the data communication bottleneck to some extent, but paradigm- shifting concepts are required. Memristors, a novel beyond-complementary metal-oxide-semiconductor (CMOS) technology, are a promising choice for memory devices due to their unique intrinsic device-level properties, enabling both storing and computing with a small, massively-parallel footprint at low power. Theoretically, this directly translates to a major boost in energy efficiency and computational throughput, but various practical challenges remain. In this work we review the latest efforts for achieving hardware-based…

Hypersonic vehicles must withstand extreme conditions during flights that exceed five times the speed of sound. These systems have the potential to facilitate rapid access to space, bolster defense capabilities, and create a new paradigm for transcontinental earth-to-earth travel. However, extreme aerothermal environments create significant challenges for vehicle materials and structures. This work addresses the critical need to develop resilient refractory alloys, composites, and ceramics. We will highlight key design principles for critical vehicle areas such as primary structures, thermal protection, and propulsion systems; the role of theory and computation; and strategies for advancing laboratory-scale materials to manufacturable flight-ready components.

Abstract Global food production faces challenges in balancing the need for increased yields with environmental sustainability. This study presents a six-year field experiment in the North China Plain, demonstrating the benefits of diversifying traditional cereal monoculture (wheat–maize) with cash crops (sweet potato) and legumes (peanut and soybean). The diversified rotations increase equivalent yield by up to 38%, reduce N 2 O emissions by 39%, and improve the system’s greenhouse gas balance by 88%. Furthermore, including legumes in crop rotations stimulates soil microbial activities, increases soil organic carbon stocks by 8%, and enhances soil health (indexed with the selected soil physiochemical and biological properties) by 45%. The large-scale adoption of diversified cropping systems in the North China Plain could increase cereal production by 32% when wheat–maize follows alternative crops in rotation and farmer income by 20% while benefiting the environment. This study provides an example of sustainable food production practices, emphasizing the significance of crop…

Abstract Constructing S-scheme heterojunctions proves proficient in achieving the spatial separation of potent photogenerated charge carriers for their participation in photoreactions. Nonetheless, the restricted contact areas between two phases within S-scheme heterostructures lead to inefficient interfacial charge transport, resulting in low photocatalytic efficiency from a kinetic perspective. Here, In 2 O 3 /Nb 2 O 5 S-scheme heterojunctions are fabricated through a straightforward one-step electrospinning technique, enabling intimate contact between the two phases and thereby fostering ultrafast interfacial electron transfer (<10 ps), as analyzed via femtosecond transient absorption spectroscopy. As a result, powerful photo-electrons and holes accumulate in the Nb 2 O 5 conduction band and In 2 O 3 valence band, respectively, exhibiting extended long lifetimes and facilitating their involvement in subsequent photoreactions. Combined with the efficient chemisorption and activation of stable CO 2 on the Nb 2 O 5 , the resulting In 2 O 3 /Nb 2 O 5 hybrid nanofibers demonstrate…

Abstract The Sabatier principle is widely explored in heterogeneous catalysis, graphically depicted in volcano plots. The most desirable activity is located at the peak of the volcano, and further advances in activity past this optimum are possible only by designing a catalyst that circumvents the limitations entailed by the Sabatier principle. In this work, by density functional theory calculations, we found that high entropy alloy (HEA) surface with spatially varying adsorption free energy of hydrogen (ΔGH*), where the active sites with strong adsorption adsorb hydrogen (H*) and other sites with weak adsorption release H* to produce H2, was against the “just right” (ΔGH* = 0 eV) in the Sabatier principle of hydrogen evolution reaction (HER). The Gaussian distribution [X ~ N(µ, σ2)] of ΔGH* on HEA was proposed as a descriptor, deriving an anomalous Sabatier principle, where a larger σ value results with µ = 0 eV results in a higher catalytic activity for HER. As a proof-of-concept, we synthesized a series of alloy systems, the PtFeCoNiCu HEA catalyst has the best catalytic…

Abstract Exploring an active and cost-effective electrocatalyst alternative to carbon-supported platinum nanoparticles for alkaline hydrogen evolution reaction (HER) have remained elusive to date. Here, we report a catalyst based on platinum single atoms (SAs) doped into the hetero-interfaced Ru/RuO 2 support (referred to as Pt-Ru/RuO 2 ), which features a low HER overpotential, an excellent stability and a distinctly enhanced cost-based activity compared to commercial Pt/C and Ru/C in 1 M KOH. Advanced physico-chemical characterizations disclose that the sluggish water dissociation is accelerated by RuO 2 while Pt SAs and the metallic Ru facilitate the subsequent H* combination. Theoretical calculations correlate with the experimental findings. Furthermore, Pt-Ru/RuO 2 only requires 1.90 V to reach 1 A cm −2 and delivers a high price activity in the anion exchange membrane water electrolyzer, outperforming the benchmark Pt/C. This research offers a feasible guidance for developing the noble metal-based catalysts with high performance and low cost toward practical H 2 production.

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spin-integrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the significance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to…

The nanoscale fibrillar morphology, featuring long-range structural order, provides abundant interfaces for efficient exciton dissociation and high-quality pathways for effective charge transport, is a promising morphology for high performance organic solar cells. Here, we synthesize a thiophene terminated non-fullerene acceptor, L8-ThCl, to induce the fibrillization of both polymer donor and host acceptor, that surpasses the 20% efficiency milestone of organic solar cells. After adding L8-ThCl, the original weak and less continuous nanofibrils of polymer donors, i.e. PM6 or D18, are well enlarged and refined, whilst the host acceptor L8-BO also assembles into nanofibrils with enhanced structural order. By adapting the layer-by-layer deposition method, the enhanced structural order can be retained to significantly boost the power conversion efficiency, with specific values of 19.4% and 20.1% for the PM6:L8-ThCl/L8-BO:L8-ThCl and D18:L8-ThCl/L8-BO:L8-ThCl devices, with the latter being certified 20.0%, which is the highest certified efficiency reported so far for single-junction…

Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d-band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding…

Chronic wounds are often infected with biofilm bacteria and characterized by high oxidative stress. Current dressings that promote chronic wound healing either require additional processes such as photothermal irradiation or leave behind gross amounts of undesirable residues. We report a dual-functionality hydrogel dressing with intrinsic antibiofilm and antioxidative properties that are synergistic and low-leaching. The hydrogel is a crosslinked network with tethered antibacterial cationic polyimidazolium and antioxidative N-acetylcysteine. In a murine diabetic wound model, the hydrogel accelerates the closure of wounds infected with methicillin-resistant Staphylococcus aureus or carbapenem-resistant Pseudomonas aeruginosa biofilm. Furthermore, a three-dimensional ex vivo human skin equivalent model shows that N-acetylcysteine promotes the keratinocyte differentiation and accelerates the re-epithelialization process. Our hydrogel dressing can be made into different formats for the healing of both flat and deep infected chronic wounds without contamination of the wound or needing…

The development of vascular networks in microfluidic chips is crucial for the long-term culture of three-dimensional cell aggregates such as spheroids, organoids, tumoroids, or tissue explants. Despite rapid advancement in microvascular network systems and organoid technologies, vascularizing organoids-on-chips remains a challenge in tissue engineering. Most existing microfluidic devices poorly reflect the complexity of in vivo flows and require complex technical set-ups. Considering these constraints, we develop a platform to establish and monitor the formation of endothelial networks around mesenchymal and pancreatic islet spheroids, as well as blood vessel organoids generated from pluripotent stem cells, cultured for up to 30 days on-chip. We show that these networks establish functional connections with the endothelium-rich spheroids and vascular organoids, as they successfully provide intravascular perfusion to these structures. We find that organoid growth, maturation, and function are enhanced when cultured on-chip using our vascularization method. This microphysiological…

Abstract Precisely modulating the Ru-O covalency in RuO x for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d -valence electrons, which were doped into or alloyed with RuO x , are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5 s /5 p orbitals. Theoretical calculations confirm that the durability of Ln-RuO x following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuO x , Er-RuO x is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO 2 . Particularly, the Er-RuO x -based device requires only 1.837 V to reach 3 A cm −2 and shows a long-term stability at 500 mA cm −2 for 100 h with a degradation rate of mere 37 μV h −1 .

Abstract Ruthenium dioxide is presently the most active catalyst for the oxygen evolution reaction (OER) in acidic media but suffers from severe Ru dissolution resulting from the high covalency of Ru-O bonds triggering lattice oxygen oxidation. Here, we report an interstitial silicon-doping strategy to stabilize the highly active Ru sites of RuO 2 while suppressing lattice oxygen oxidation. The representative Si-RuO 2 −0.1 catalyst exhibits high activity and stability in acid with a negligible degradation rate of ~52 μV h −1 in an 800 h test and an overpotential of 226 mV at 10 mA cm −2 . Differential electrochemical mass spectrometry (DEMS) results demonstrate that the lattice oxygen oxidation pathway of the Si-RuO 2 −0.1 was suppressed by ∼95% compared to that of commercial RuO 2 , which is highly responsible for the extraordinary stability. This work supplied a unique mentality to guide future developments on Ru-based oxide catalysts’ stability in an acidic environment.

Abstract Most tough hydrogels are reinforced by introducing energy dissipation mechanisms, but simultaneously realizing a high toughness and low hysteresis is challenging because the energy dissipation structure cannot recover rapidly. In this work, high mechanical performance highly entangled double network hydrogels without energy dissipation structure are fabricated, in which physical entanglements act as the primary effective crosslinking in the first network. This sliding entanglement structure allows the hydrogel network to form a highly uniform oriented structure during stretching, resulting in a high tensile strength of ~3 MPa, a fracture energy of 8340 J m −2 and a strain-stiffening capability of 47.5 in 90% water content. Moreover, almost 100% reversibility is obtained in this hydrogel via energy storage based on entropy loss. The highly entangled double network structure not only overcomes the typical trade-off between the high toughness and low hysteresis of hydrogels, but more importantly, it provides an insight into the application of entanglement structures in…

There has been a growing effort to replace manual extraction of data from research papers with automated data extraction based on natural language processing, language models, and recently, large language models (LLMs). Although these methods enable efficient extraction of data from large sets of research papers, they require a significant amount of up-front effort, expertise, and coding. In this work, we propose the ChatExtract method that can fully automate very accurate data extraction with minimal initial effort and background, using an advanced conversational LLM. ChatExtract consists of a set of engineered prompts applied to a conversational LLM that both identify sentences with data, extract that data, and assure the data's correctness through a series of follow-up questions. These follow-up questions largely overcome known issues with LLMs providing factually inaccurate responses. ChatExtract can be applied with any conversational LLMs and yields very high quality data extraction. In tests on materials data, we find precision and recall both close to 90% from the best…

A subgroup of patients infected with SARS-CoV-2 remain symptomatic over three months after infection. A distinctive symptom of patients with long COVID is post-exertional malaise, which is associated with a worsening of fatigue- and pain-related symptoms after acute mental or physical exercise, but its underlying pathophysiology is unclear. With this longitudinal case-control study (NCT05225688), we provide new insights into the pathophysiology of post-exertional malaise in patients with long COVID. We show that skeletal muscle structure is associated with a lower exercise capacity in patients, and local and systemic metabolic disturbances, severe exercise-induced myopathy and tissue infiltration of amyloid-containing deposits in skeletal muscles of patients with long COVID worsen after induction of post-exertional malaise. This study highlights novel pathways that help to understand the pathophysiology of post-exertional malaise in patients suffering from long COVID and other post-infectious diseases.

Macroautophagy decreases with age, and this change is considered a hallmark of the aging process. It remains unknown whether mitophagy, the essential selective autophagic degradation of mitochondria, also decreases with age. In our analysis of mitophagy in multiple organs in the mito-QC reporter mouse, mitophagy is either increased or unchanged in old versus young mice. Transcriptomic analysis shows marked upregulation of the type I interferon response in the retina of old mice, which correlates with increased levels of cytosolic mtDNA and activation of the cGAS/STING pathway. Crucially, these same alterations are replicated in primary human fibroblasts from elderly donors. In old mice, pharmacological induction of mitophagy with urolithin A attenuates cGAS/STING activation and ameliorates deterioration of neurological function. These findings point to mitophagy induction as a strategy to decrease age-associated inflammation and increase healthspan.

Simultaneously activating metal and lattice oxygen sites to construct a compatible multi-mechanism catalysis is expected for the oxygen evolution reaction (OER) by providing highly available active sites and mediate catalytic activity/stability, but significant challenges remain. Herein, Fe and S dually modulated NiFe oxyhydroxide (R-NiFeOOH@SO4) is conceived by complete reconstruction of NiMoO4·xH2O@Fe,S during OER, and achieves compatible adsorbate evolution mechanism and lattice oxygen oxidation mechanism with simultaneously optimized metal/oxygen sites, as substantiated by in situ spectroscopy/mass spectrometry and chemical probe. Further theoretical analyses reveal that Fe promotes the OER kinetics under adsorbate evolution mechanism, while S excites the lattice oxygen activity under lattice oxygen oxidation mechanism, featuring upshifted O 2p band centers, enlarged d-d Coulomb interaction, weakened metal-oxygen bond and optimized intermediate adsorption free energy. Benefiting from the compatible multi-mechanism, R-NiFeOOH@SO4 only requires overpotentials of 251 ± 5/291 ± 1 mV…

Reservoir computing originates in the early 2000s, the core idea being to utilize dynamical systems as reservoirs (nonlinear generalizations of standard bases) to adaptively learn spatiotemporal features and hidden patterns in complex time series. Shown to have the potential of achieving higher-precision prediction in chaotic systems, those pioneering works led to a great amount of interest and follow-ups in the community of nonlinear dynamics and complex systems. To unlock the full capabilities of reservoir computing towards a fast, lightweight, and significantly more interpretable learning framework for temporal dynamical systems, substantially more research is needed. This Perspective intends to elucidate the parallel progress of mathematical theory, algorithm design and experimental realizations of reservoir computing, and identify emerging opportunities as well as existing challenges for large-scale industrial adoption of reservoir computing, together with a few ideas and viewpoints on how some of those challenges might be resolved with joint efforts by academic and industrial…

The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites and the intensive oxidant consumption still severely restrict the decontamination performance. While nanoconfinement of SACs allows drastically enhanced decontamination reaction kinetics, the detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment of reactants, the catalytic pathway shift is also an important cause for the reactivity enhancement of nanoconfined SACs. The surface electronic structure of cobalt site is altered by confining it within the nanopores of mesostructured silica particles, which triggers a fundamental transition from singlet oxygen to electron transfer pathway for 4-chlorophenol oxidation. The changed pathway and accelerated interfacial mass transfer render the nanoconfined system up to 34.7-fold higher pollutant degradation rate and drastically raised peroxymonosulfate utilization efficiency (from 61.8% to 96.6%) relative…

Abstract Gold-based co-catalysts are a promising class of materials with potential applications in photocatalytic H 2 O 2 production. However, current approaches with Au co-catalysts show limited H 2 O 2 production due to intrinsically weak O 2 adsorption at the Au site. We report an approach to strengthen O 2 adsorption at Au sites, and to improve H 2 O 2 production, through the formation of electron-deficient Au δ+ sites by modifying the electronic structure. In this case, we report the synthesis of TiO 2 /MoS x -Au, following selective deposition of Au onto a MoS x surface which is then further anchored onto TiO 2 . We further show that the catalyst achieves a significantly increased H 2 O 2 production rate of 30.44 mmol g −1 h −1 in O 2 -saturated solution containing ethanol. Density functional theory calculations and X-ray photoelectron spectroscopy analysis reveal that the MoS x mediator induces the formation of electron-deficient Au δ+ sites thereby decreasing the antibonding-orbital occupancy of Au-O ads and subsequently enhancing O 2 adsorption. This strategy may be useful…

Abstract The combination between macroscopic structure designs and microscopic material designs offers tremendous possibilities for the development of advanced electromagnetic wave (EMW) absorbers. Herein, we propose a metamaterial design to address persistent challenges in this field, including narrow bandwidth, low–frequency bottlenecks, and, particularly, the urgent issue of robustness (i.e., oblique, and polarized incidence). Our absorber features a semiconductive metal-organic framework/iron 2D/2D assembly (CuHT–FCIP) with abundant crystal/crystal heterojunctions and strong magneto-electric coupling networks. This design achieves remarkable EMW absorption across a broad range (2 to 40 GHz) at a thickness of just 9.3 mm. Notably, it maintains stable performance against oblique incidence (within 75°) and polarizations (both transverse electric and transverse magnetic). Furthermore, the absorber demonstrates high specific compressive strength (201.01 MPa·cm 3 ·g −1 ) and low density (0.89 g·cm −3 ). This advancement holds promise for developing robust EMW absorbers with superior…

Abstract Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. The key to achieving high selectivity lies in the on-demand design of NF membrane pores in accordance with the size difference between Li+ and Mg2+ ions, but this poses a huge challenge for traditional NF membranes and difficult to be realized. In this work, we report the fabrication of polyamide (PA) NF membranes with ultra-high Li+/Mg2+ selectivity by modifying the interfacial polymerization (IP) process between piperazine (PIP) and trimesoyl chloride (TMC) with an oil-soluble surfactant that forms a monolayer at oil/water interface, referred to as OSARIP. The OSARIP benefits to regulate the membrane pores so that all of them are smaller than Mg2+ ions. Under the solely size sieving effect, an unprecedentedly high Mg2+ rejection rate of 99.96% and Li+/Mg2+ selectivity over 4000 are achieved. This value is one to two orders of magnitude higher than all the currently reported…

For organic solar cells to be competitive, the light-absorbing molecules should simultaneously satisfy multiple key requirements, including weak-absorption charge transfer state, high dielectric constant, suitable surface energy, proper crystallinity, etc. However, the systematic design rule in molecules to achieve the abovementioned goals is rarely studied. In this work, guided by theoretical calculation, we present a rational design of non-fullerene acceptor o-BTP-eC9, with distinct photoelectric properties compared to benchmark BTP-eC9. o-BTP-eC9 based device has uplifted charge transfer state, therefore significantly reducing the energy loss by 41 meV and showing excellent power conversion efficiency of 18.7%. Moreover, the new guest acceptor o-BTP-eC9 has excellent miscibility, crystallinity, and energy level compatibility with BTP-eC9, which enables an efficiency of 19.9% (19.5% certified) in PM6:BTP-C9:o-BTP-eC9 based ternary system with enhanced operational stability.

Abstract Structure deterioration and side reaction, which originated from the solvated H 2 O, are the main constraints for the practical deployment of both cathode and anode in aqueous Zn-ion batteries. Here we formulate a weakly solvating electrolyte to reduce the solvating power of H 2 O and strengthen the coordination competitiveness of SO 4 2− to Zn 2+ over H 2 O. Experiment results and theoretical simulations demonstrate that the water-poor solvation structure of Zn 2+ is achieved, which can (i) substantially eliminate solvated-H 2 O-mediated undesirable side reactions on the Zn anode. (ii) boost the desolvation kinetics of Zn 2+ and suppress Zn dendrite growth as well as structure aberration of the cathode. Remarkably, the synergy of these two factors enables long-life full cells including Zn/NaV 3 O 8 ·1.5H 2 O, Zn/MnO 2 and Zn/CoFe(CN) 6 cells. More importantly, practical rechargeable AA-type Zn/NVO cells are assembled, which present a capacity of 101.7 mAh and stability of 96.1% capacity retention after 30 cycles at 0.66 C.

Abstract Computational design of therapeutic peptides that enables fast exploration of a combinatorial number of amino acid possibilities has emerged as a popular strategy in antibiotics discovery but identifying peptide inhibitors targeting specific protein-protein interactions (PPIs) still faces significant challenges. Here, we present a new approach for de novo design of target-specific peptides, which combines a Gated Recurrent Unit (GRU) based variational autoencoder (VAE) with Rosetta FlexPepDock for peptide sequence generation and potency assessment, followed by the refinement with all-atom molecular dynamics (MD) simulations. We have utilized the computational protocol to design eight peptide inhibitors specifically disrupting the interaction of β-catenin with TCF/LEF family transcription factors. Four of these peptide inhibitor candidates were synthesized and experimentally tested, of which two displayed enhanced binding affinities for β-catenin compared to the best-known peptide made of all natural amino acids. We also constructed a random peptide library of 710,000 unique…

The 2023 wildfire season in Canada was unprecedented in its scale and intensity, spanning from mid-April to late October and across much of the forested regions of Canada. Here, we summarize the main causes and impacts of this exceptional season. The record-breaking total area burned (~15 Mha) can be attributed to several environmental factors that converged early in the season: early snowmelt, multiannual drought conditions in western Canada, and the rapid transition to drought in eastern Canada. Anthropogenic climate change enabled sustained extreme fire weather conditions, as the mean May-October temperature over Canada in 2023 was 2.2 °C warmer than the 1991-2020 average. The impacts were profound with more than 200 communities evacuated, millions exposed to hazardous air quality from smoke, and unmatched demands on fire-fighting resources. The 2023 wildfire season in Canada not only set new records, but highlights the increasing challenges posed by wildfires in Canada.

Abstract Coupling high capacity cathode and Li metal anode with the solid-state electrolyte has been demonstrated as an effective strategy for increasing the energy density and enhancing the safety of rechargeable batteries. However, the limited ion conductivity of the solid-state electrolyte, the large interfacial resistance of electrode/electrolyte, and the unconstrained dendrite growth of the Li metal anode are still the main challenges hindering the applications of the solid-state Li-metal batteries (SSLMB). Herein, a poly(ether-urethane) based solid-state polymer electrolyte (SPE) with self-healing property are designed to reduce the interface impedance and achieve high performance SSLMB. Benefiting from the dynamic covalent disulfide bonds rearrangement and the hydrogen bonds between urethane groups, the proposed SPE exhibits excellent interfacial self-healing ability, which can help to constantly maintain well interfacial contact between solid-state electrolyte and cathode/anode electrodes during the whole cycling life. By casting the designed SPE directly on the sulfur-based…

Commensal bacteria generate immensely diverse active metabolites to maintain gut homeostasis, however their fundamental role in establishing an immunotolerogenic microenvironment in the intestinal tract remains obscure. Here, we demonstrate that an understudied murine commensal bacterium, Dubosiella newyorkensis, and its human homologue Clostridium innocuum, have a probiotic immunomodulatory effect on dextran sulfate sodium-induced colitis using conventional, antibiotic-treated and germ-free mouse models. We identify an important role for the D. newyorkensis in rebalancing Treg/Th17 responses and ameliorating mucosal barrier injury by producing short-chain fatty acids, especially propionate and L-Lysine (Lys). We further show that Lys induces the immune tolerance ability of dendritic cells (DCs) by enhancing Trp catabolism towards the kynurenine (Kyn) pathway through activation of the metabolic enzyme indoleamine-2,3-dioxygenase 1 (IDO1) in an aryl hydrocarbon receptor (AhR)-dependent manner. This study identifies a previously unrecognized metabolic communication by which…

Abstract Chronic diabetic wounds are at lifelong risk of developing diabetic foot ulcers owing to severe hypoxia, excessive reactive oxygen species (ROS), a complex inflammatory microenvironment, and the potential for bacterial infection. Here we develop a programmed treatment strategy employing live Haematococcus (HEA). By modulating light intensity, HEA can be programmed to perform a variety of functions, such as antibacterial activity, oxygen supply, ROS scavenging, and immune regulation, suggesting its potential for use in programmed therapy. Under high light intensity (658 nm, 0.5 W/cm 2 ), green HEA (GHEA) with efficient photothermal conversion mediate wound surface disinfection. By decreasing the light intensity (658 nm, 0.1 W/cm 2 ), the photosynthetic system of GHEA can continuously produce oxygen, effectively resolving the problems of hypoxia and promoting vascular regeneration. Continuous light irradiation induces astaxanthin (AST) accumulation in HEA cells, resulting in a gradual transformation from a green to red hue (RHEA). RHEA effectively scavenges excess ROS,…

Abstract Oxygen evolution reaction (OER) is critical to renewable energy conversion technologies, but the structure-activity relationships and underlying catalytic mechanisms in catalysts are not fully understood. We herein demonstrate a strategy to promote OER with simultaneously achieved lattice oxygen activation and enhanced local electric field by dual doping of cations and anions. Rough arrays of Fe and F co-doped CoO nanoneedles are constructed, and a low overpotential of 277 mV at 500 mA cm −2 is achieved. The dually doped Fe and F could cooperatively tailor the electronic properties of CoO, leading to improved metal-oxygen covalency and stimulated lattice oxygen activation. Particularly, Fe doping induces a synergetic effect of tip enhancement and proximity effect, which effectively concentrates OH − ions, optimizes reaction energy barrier and promotes O 2 desorption. This work demonstrates a conceptual strategy to couple lattice oxygen and local electric field for effective electrocatalytic water oxidation.

Abstract Improving the absorption of electromagnetic waves at low-frequency bands (2-8 GHz) is crucial for the increasing electromagnetic (EM) pollution brought about by the innovation of the fifth generation (5G) communication technology. However, the poor impedance matching and intrinsic attenuation of material in low-frequency bands hinders the development of low-frequency electromagnetic wave absorbing (EMWA) materials. Here we propose an interface-induced dual-pinning mechanism and establish a magnetoelectric bias interface by constructing bilayer core-shell structures of NiFe 2 O 4 (NFO)@BiFeO 3 (BFO)@polypyrrole (PPy). Such heterogeneous interface could induce distinct magnetic pinning of the magnetic moment in the ferromagnetic NFO and dielectric pinning of the dipole rotation in PPy. The establishment of the dual-pinning effect resulted in optimized impedance and enhanced attenuation at low-frequency bands, leading to better EMWA performance. The minimum reflection loss (RL min ) at thickness of 4.43 mm reaches -65.30 dB (the optimal absorption efficiency of 99.99997%), and…

Abstract Amorphous semiconductors without perfect crystalline lattice structures are usually considered to be unfavorable for photocatalysis due to the presence of enriched trap states and defects. Here we demonstrate that breaking long-range atomic order in an amorphous ZnCdS photocatalyst can induce dipole moments and generate strong electric fields within the particles which facilitates charge separation and transfer. Loading 1 wt.% of low-cost Co-MoSx cocatalysts to the ZnCdS material increases the H2 evolution rate to 70.13 mmol g−1 h−1, which is over 5 times higher than its crystalline counterpart and is stable over the long-term up to 160 h. A flexible 20 cm × 20 cm Co-MoSx/ZnCdS film is prepared by a facile blade-coating technique and can generate numerous observable H2 bubbles under natural sunlight, exhibiting potential for scale-up solar H2 production.

Climate warming disproportionately impacts countries in the Global South by increasing extreme heat exposure. However, geographic disparities in adaptation capacity are unclear. Here, we assess global inequality in green spaces, which urban residents critically rely on to mitigate outdoor heat stress. We use remote sensing data to quantify daytime cooling by urban greenery in the warm seasons across the ~500 largest cities globally. We show a striking contrast, with Global South cities having ~70% of the cooling capacity of cities in the Global North (2.5 ± 1.0 °C vs. 3.6 ± 1.7 °C). A similar gap occurs for the cooling adaptation benefits received by an average resident in these cities (2.2 ± 0.9 °C vs. 3.4 ± 1.7 °C). This cooling adaptation inequality is due to discrepancies in green space quantity and quality between cities in the Global North and South, shaped by socioeconomic and natural factors. Our analyses further suggest a vast potential for enhancing cooling adaptation while reducing global inequality. A 1.5-fold gap exists in green space cooling adaptation between cities…

Abstract The nitrate (NO3−) electroreduction into ammonia (NH3) represents a promising approach for sustainable NH3 synthesis. However, the variation of adsorption configurations renders great difficulties in the simultaneous optimization of binding energy for the intermediates. Though the extensively reported Cu-based electrocatalysts benefit NO3− adsorption, one of the key issues lies in the accumulation of nitrite (NO2−) due to its weak adsorption, resulting in the rapid deactivation of catalysts and sluggish kinetics of subsequent hydrogenation steps. Here we report a tandem electrocatalyst by combining Cu single atoms catalysts with adjacent Co3O4 nanosheets to boost the electroreduction of NO3− to NH3. The obtained tandem catalyst exhibits a yield rate for NH3 of 114.0 mg $${}_{{{{{{\rm{NH}}}}}}_3}$$ NH 3 h−1 cm−2, which exceeds the previous values for the reported Cu-based catalysts. Mechanism investigations unveil that the combination of Co3O4 regulates the adsorption configuration of NO2− and strengthens the binding with NO2−, thus accelerating the electroreduction of NO3−…

The rapid recombination of photoinduced charge carriers in semiconductors fundamentally limits their application in photocatalysis. Herein, we report that a superlattice interface and S-scheme heterojunction based on Mn0.5Cd0.5S nanorods can significantly promote ultrafast charge separation and transfer. Specifically, the axially distributed zinc blende/wurtzite superlattice interfaces in Mn0.5Cd0.5S nanorods can redistribute photoinduced charge carriers more effectively when boosted by homogeneous internal electric fields and promotes bulk separation. Accordingly, S-scheme heterojunctions between the Mn0.5Cd0.5S nanorods and MnWO4 nanoparticles can further accelerate the surface separation of charge carriers via a heterogeneous internal electric field. Subsequent capture of the photoelectrons by adsorbed H2O is as fast as several picoseconds which results in a photocatalytic H2 evolution rate of 54.4 mmol·g−1·h−1 without any cocatalyst under simulated solar irradiation. The yields are increased by a factor of ~5 times relative to control samples and an apparent quantum efficiency…

The wide applications of liquid chromatography - mass spectrometry (LC-MS) in untargeted metabolomics demand an easy-to-use, comprehensive computational workflow to support efficient and reproducible data analysis. However, current tools were primarily developed to perform specific tasks in LC-MS based metabolomics data analysis. Here we introduce MetaboAnalystR 4.0 as a streamlined pipeline covering raw spectra processing, compound identification, statistical analysis, and functional interpretation. The key features of MetaboAnalystR 4.0 includes an auto-optimized feature detection and quantification algorithm for LC-MS1 spectra processing, efficient MS2 spectra deconvolution and compound identification for data-dependent or data-independent acquisition, and more accurate functional interpretation through integrated spectral annotation. Comprehensive validation studies using LC-MS1 and MS2 spectra obtained from standards mixtures, dilution series and clinical metabolomics samples have shown its excellent performance across a wide range of common tasks such as peak picking, spectral…

Abstract Single-atom catalysts, especially those with metal−N 4 moieties, hold great promise for facilitating the oxygen reduction reaction. However, the symmetrical distribution of electrons within the metal−N 4 moiety results in unsatisfactory adsorption strength of intermediates, thereby limiting their performance improvements. Herein, we present atomically coordination-regulated Co single-atom catalysts that comprise a symmetry-broken Cl−Co−N 4 moiety, which serves to break the symmetrical electron distribution. In situ characterizations reveal the dynamic evolution of the symmetry-broken Cl−Co−N 4 moiety into a coordination-reduced Cl−Co−N 2 structure, effectively optimizing the 3 d electron filling of Co sites toward a reduced d -band electron occupancy ( d 5.8 → d 5.28 ) under reaction conditions for a fast four-electron oxygen reduction reaction process. As a result, the coordination-regulated Co single-atom catalysts deliver a large half-potential of 0.93 V and a mass activity of 5480 A g metal −1 . Importantly, a Zn-air battery using the coordination-regulated Co…

Nutrient enrichment is a major global change component that often disrupts the relationship between aboveground biodiversity and ecosystem functions by promoting species dominance, altering trophic interactions, and reducing ecosystem stability. Emerging evidence indicates that nutrient enrichment also reduces soil biodiversity and weakens the relationship between belowground biodiversity and ecosystem functions, but the underlying mechanisms remain largely unclear. Here, we explore the effects of nutrient enrichment on soil properties, soil biodiversity, and multiple ecosystem functions through a 13-year field experiment. We show that soil acidification induced by nutrient enrichment, rather than changes in mineral nutrient and carbon (C) availability, is the primary factor negatively affecting the relationship between soil diversity and ecosystem multifunctionality. Nitrogen and phosphorus additions significantly reduce soil pH, diversity of bacteria, fungi and nematodes, as well as an array of ecosystem functions related to C and nutrient cycling. Effects of nutrient enrichment…

Patient recruitment is challenging for clinical trials. We introduce TrialGPT, an end-to-end framework for zero-shot patient-to-trial matching with large language models. TrialGPT comprises three modules: it first performs large-scale filtering to retrieve candidate trials (TrialGPT-Retrieval); then predicts criterion-level patient eligibility (TrialGPT-Matching); and finally generates trial-level scores (TrialGPT-Ranking). We evaluate TrialGPT on three cohorts of 183 synthetic patients with over 75,000 trial annotations. TrialGPT-Retrieval can recall over 90% of relevant trials using less than 6% of the initial collection. Manual evaluations on 1,015 patient-criterion pairs show that TrialGPT-Matching achieves an accuracy of 87.3% with faithful explanations, close to the expert performance. The TrialGPT-Ranking scores are highly correlated with human judgments and outperform the best-competing models by 43.8% in ranking and excluding trials. Furthermore, our user study reveals that TrialGPT can reduce the screening time by 42.6% in patient recruitment. Overall, these results have…

Abstract The demand for lithium extraction from salt-lake brines is increasing to address the lithium supply shortage. Nanofiltration separation technology with high Mg 2+ /Li + separation efficiency has shown great potential for lithium extraction. However, it usually requires diluting the brine with a large quantity of freshwater and only yields Li + -enriched solution. Inspired by the process of selective ion uptake and salt secretion in mangroves, we report here the direct extraction of lithium from salt-lake brines by utilizing the synergistic effect of ion separation membrane and solar-driven evaporator. The ion separation membrane-based solar evaporator is a multilayer structure consisting of an upper photothermal layer to evaporate water, a hydrophilic porous membrane in the middle to generate capillary pressure as the driving force for water transport, and an ultrathin ion separation membrane at the bottom to allow Li + to pass through and block other multivalent ions. This process exhibits excellent lithium extraction capability. When treating artificial salt-lake brine…

Electrocatalytic H2 production from seawater, recognized as a promising technology utilizing offshore renewables, faces challenges from chloride-induced reactions and corrosion. Here, We introduce a catalytic surface where OH– dominates over Cl– in adsorption and activation, which is crucial for O2 production. Our NiFe-based anode, enhanced by nearby Cr sites, achieves low overpotentials and selective alkaline seawater oxidation. It outperforms the RuO2 counterpart in terms of lifespan in scaled-up stacks, maintaining stability for over 2500 h in three-electrode tests. Ex situ/in situ analyses reveal that Cr(III) sites enrich OH–, while Cl– is repelled by Cr(VI) sites, both of which are well-dispersed and close to NiFe, enhancing charge transfer and overall electrode performance. Such multiple effects fundamentally boost the activity, selectively, and chemical stability of the NiFe-based electrode. This development marks a significant advance in creating durable, noble-metal-free electrodes for alkaline seawater electrolysis, highlighting the importance of well-distributed catalytic…

Abstract Transition metal chalcogenides have been identified as low-cost and efficient electrocatalysts to promote the hydrogen evolution reaction in alkaline media. However, the identification of active sites and the underlying catalytic mechanism remain elusive. In this work, we employ operando X-ray absorption spectroscopy and near-ambient pressure X-ray photoelectron spectroscopy to elucidate that NiS undergoes an in-situ phase transition to an intimately mixed phase of Ni 3 S 2 and NiO, generating highly active synergistic dual sites at the Ni 3 S 2 /NiO interface. The interfacial Ni is the active site for water dissociation and OH* adsorption while the interfacial S acts as the active site for H* adsorption and H 2 evolution. Accordingly, the in-situ formation of Ni 3 S 2 /NiO interfaces enables NiS electrocatalysts to achieve an overpotential of only 95 ± 8 mV at a current density of 10 mA cm −2 . Our work highlighted that the chemistry of transition metal chalcogenides is highly dynamic, and a careful control of the working conditions may lead to the in-situ formation of…

Toll-like receptor 9 (TLR9) recognizes self-DNA and plays intricate roles in systemic lupus erythematosus (SLE). However, the molecular mechanism regulating the endosomal TLR9 response is incompletely understood. Here, we report that palmitoyl-protein thioesterase 1 (PPT1) regulates systemic autoimmunity by removing S-palmitoylation from TLR9 in lysosomes. PPT1 promotes the secretion of IFNα by plasmacytoid dendritic cells (pDCs) and TNF by macrophages. Genetic deficiency in or chemical inhibition of PPT1 reduces anti-nuclear antibody levels and attenuates nephritis in B6.Sle1yaa mice. In healthy volunteers and patients with SLE, the PPT1 inhibitor, HDSF, reduces IFNα production ex vivo. Mechanistically, biochemical and mass spectrometry analyses demonstrated that TLR9 is S-palmitoylated at C258 and C265. Moreover, the protein acyltransferase, DHHC3, palmitoylates TLR9 in the Golgi, and regulates TLR9 trafficking to endosomes. Subsequent depalmitoylation by PPT1 facilitates the release of TLR9 from UNC93B1. Our results reveal a posttranslational modification cycle that controls TLR9…

Wound healing is an obvious clinical concern that can be hindered by inadequate angiogenesis, inflammation, and chronic hypoxia. While exosomes derived from adipose tissue-derived stem cells have shown promise in accelerating healing by carrying therapeutic growth factors and microRNAs, intracellular cargo delivery is compromised in hypoxic tissues due to activated hypoxia-induced endocytic recycling. To address this challenge, we have developed a strategy to coat oxygen nanobubbles with exosomes and incorporate them into a polyvinyl alcohol/gelatin hybrid hydrogel. This approach not only alleviates wound hypoxia but also offers an efficient means of delivering exosome-coated nanoparticles in hypoxic conditions. The self-healing properties of the hydrogel, along with its component, gelatin, aids in hemostasis, while its crosslinking bonds facilitate hydrogen peroxide decomposition, to ameliorate wound inflammation. Here, we show the potential of this multifunctional hydrogel for enhanced healing, promoting angiogenesis, facilitating exosome delivery, mitigating hypoxia, and…

Abstract Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive and yet remains to be understood. Here, an efficient hierarchically porous Fe single atom catalyst (Fe SAs-HP) is prepared with Fe atoms densely resided at micropores and mesopores. Fe SAs-HP exhibits robust ORR performance with half-wave potential of 0.94 V and turnover frequency of 5.99 e −1 s −1 site −1 at 0.80 V. Theoretical simulations unravel a structural heterogeneity induced optimization, where mesoporous Fe-N 4 acts as real active centers as a result of long-range electron regulation by adjacent microporous sites, facilitating O 2 activation and desorption of key intermediate *OH. Multilevel operando characterization results identify active Fe sites undergo a dynamic evolution from basic Fe-N 4 to active Fe-N 3 under working conditions. Our findings reveal the structural origin of…

Abstract Hard carbons are emerging as the most viable anodes to support the commercialization of sodium-ion (Na-ion) batteries due to their competitive performance. However, the hard carbon anode suffers from low initial Coulombic efficiency (ICE), and the ambiguous Na-ion (Na+) storage mechanism and interfacial chemistry fail to give a reasonable interpretation. Here, we have identified the time-dependent ion pre-desolvation on the nanopore of hard carbons, which significantly affects the Na+ storage efficiency by altering the solvation structure of electrolytes. Consummating the pre-desolvation by extending the aging time, generates a highly aggregated electrolyte configuration inside the nanopore, resulting in negligible reductive decomposition of electrolytes. When applying the above insights, the hard carbon anodes achieve a high average ICE of 98.21% in the absence of any Na supplementation techniques. Therefore, the negative-to-positive capacity ratio can be reduced to 1.02 for full cells, which enables an improved energy density. The insight into hard carbons and related…

Abstract Seawater electroreduction is attractive for future H 2 production and intermittent energy storage, which has been hindered by aggressive Mg 2+ /Ca 2+ precipitation at cathodes and consequent poor stability. Here we present a vital microscopic bubble/precipitate traffic system (MBPTS) by constructing honeycomb-type 3D cathodes for robust anti-precipitation seawater reduction (SR), which massively/uniformly release small-sized H 2 bubbles to almost every corner of the cathode to repel Mg 2+ /Ca 2+ precipitates without a break. Noticeably, the optimal cathode with built-in MBPTS not only enables state-of-the-art alkaline SR performance (1000-h stable operation at –1 A cm −2 ) but also is highly specialized in catalytically splitting natural seawater into H 2 with the greatest anti-precipitation ability. Low precipitation amounts after prolonged tests under large current densities reflect genuine efficacy by our MBPTS. Additionally, a flow-type electrolyzer based on our optimal cathode stably functions at industrially-relevant 500 mA cm −2 for 150 h in natural seawater while…

Abstract Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause an inert oxygen production, which remains a huge obstacle to overall water-splitting. Here, a distortion-evoked cation-site oxygen doping of ZnIn2S4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S1 sites being electron-rich and S2 sites being electron-deficient in the local structure of S1–S2–O sites. The strong charge redistribution character activates stable oxygen reactions at S2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S1 sites favor the adsorption/desorption of hydrogen. Consequently, an overall water-splitting reaction has been realized in D-O-ZIS with a remarkable solar-to-hydrogen conversion efficiency of 0.57%, accompanying a ~ 91% retention rate after 120 h photocatalytic…

Fully targeted mRNA therapeutics necessitate simultaneous organ-specific accumulation and effective translation. Despite some progress, delivery systems are still unable to fully achieve this. Here, we reformulate lipid nanoparticles (LNPs) through adjustments in lipid material structures and compositions to systematically achieve the pulmonary and hepatic (respectively) targeted mRNA distribution and expression. A combinatorial library of degradable-core based ionizable cationic lipids is designed, following by optimisation of LNP compositions. Contrary to current LNP paradigms, our findings demonstrate that cholesterol and phospholipid are dispensable for LNP functionality. Specifically, cholesterol-removal addresses the persistent challenge of preventing nanoparticle accumulation in hepatic tissues. By modulating and simplifying intrinsic LNP components, concurrent mRNA accumulation and translation is achieved in the lung and liver, respectively. This targeting strategy is applicable to existing LNP systems with potential to expand the progress of precise mRNA therapy for diverse…

The unceasing circulation of SARS-CoV-2 leads to the continuous emergence of novel viral sublineages. Here, we isolate and characterize XBB.1, XBB.1.5, XBB.1.9.1, XBB.1.16.1, EG.5.1.1, EG.5.1.3, XBF, BA.2.86.1 and JN.1 variants, representing >80% of circulating variants in January 2024. The XBB subvariants carry few but recurrent mutations in the spike, whereas BA.2.86.1 and JN.1 harbor >30 additional changes. These variants replicate in IGROV-1 but no longer in Vero E6 and are not markedly fusogenic. They potently infect nasal epithelial cells, with EG.5.1.3 exhibiting the highest fitness. Antivirals remain active. Neutralizing antibody (NAb) responses from vaccinees and BA.1/BA.2-infected individuals are markedly lower compared to BA.1, without major differences between variants. An XBB breakthrough infection enhances NAb responses against both XBB and BA.2.86 variants. JN.1 displays lower affinity to ACE2 and higher immune evasion properties compared to BA.2.86.1. Thus, while distinct, the evolutionary trajectory of these variants combines increased fitness and antibody evasion.

Photothermal superhydrophobic coatings are supposed promising to prevent ice accumulation on infrastructures but often experience significant performance degradation in real icing conditions and lack mechanical robustness. Here, we report design of robust photothermal superhydrophobic coatings with three-tier hierarchical micro-/nano-/nanostructures by deposition of nanosized MOFs on natural attapulgite nanorods, fluorination, controlled phase separation of a hydrophobic adhesive and spraying assembly. Phase separation degree and adhesive content significantly influence the coatings' properties by regulating the structural parameters and morphology. In simulated/real icing environments, the coatings simultaneously show (i) high superhydrophobicity and stable Cassie-Baxter states due to their low-surface-energy, three-tier micro-/nano-/nanostructure, (ii) excellent photothermal effect primarily due to nanosized MOFs, and (iii) good mechanical robustness by the phase-separated adhesive, reinforcement with attapulgite and the coatings' self-similar structure. Accordingly, combined with…

Lysine lactylation (Kla) links metabolism and gene regulation and plays a key role in multiple biological processes. However, the regulatory mechanism and functional consequence of Kla remain to be explored. Here, we report that HBO1 functions as a lysine lactyltransferase to regulate transcription. We show that HBO1 catalyzes the addition of Kla in vitro and intracellularly, and E508 is a key site for the lactyltransferase activity of HBO1. Quantitative proteomic analysis further reveals 95 endogenous Kla sites targeted by HBO1, with the majority located on histones. Using site-specific antibodies, we find that HBO1 may preferentially catalyze histone H3K9la and scaffold proteins including JADE1 and BRPF2 can promote the enzymatic activity for histone Kla. Notably, CUT&Tag assays demonstrate that HBO1 is required for histone H3K9la on transcription start sites (TSSs). Besides, the regulated Kla can promote key signaling pathways and tumorigenesis, which is further supported by evaluating the malignant behaviors of HBO1- knockout (KO) tumor cells, as well as the level of histone…

Abstract Continuous and effective hydrogen evolution under high current densities remains a challenge for water electrolysis owing to the rapid performance degradation under continuous large-current operation. In this study, theoretical calculations, operando Raman spectroscopy, and CO stripping experiments confirm that Ru nanocrystals have a high resistance against deactivation because of the synergistic adsorption of OH intermediates (OH ad ) on the Ru and single atoms. Based on this conceptual model, we design the Ni single atoms modifying ultra-small Ru nanoparticle with defect carbon bridging structure (UP-RuNi SAs /C) via a unique unipolar pulse electrodeposition (UPED) strategy. As a result, the UP-RuNi SAs /C is found capable of running steadily for 100 h at 3 A cm −2 , and shows a low overpotential of 9 mV at a current density of 10 mA cm −2 under alkaline conditions. Moreover, the UP-RuNi SAs /C allows an anion exchange membrane (AEM) electrolyzer to operate stably at 1.95 V cell for 250 h at 1 A cm −2 .

Abstract Cobalt oxyhydroxide (CoOOH) is a promising catalytic material for oxygen evolution reaction (OER). In the traditional CoOOH structure, Co 3+ exhibits a low-spin state configuration ( $${t}_{2{{{{{\rm{g}}}}}}}^{6}{e}_{{{{{{\rm{g}}}}}}}^{0}$$ t 2 g 6 e g 0 ), with electron transfer occurring in face-to-face $${t}_{2{{{{{\rm{g}}}}}}}^{*}$$ t 2 g * orbitals. In this work, we report the successful synthesis of high-spin state Co 3+ CoOOH structure, by introducing coordinatively unsaturated Co atoms. As compared to the low-spin state CoOOH, electron transfer in the high-spin state CoOOH occurs in apex-to-apex $${e}_{{{{{{\rm{g}}}}}}}^{*}$$ e g * orbitals, which exhibits faster electron transfer ability. As a result, the high-spin state CoOOH performs superior OER activity with an overpotential of 226 mV at 10 mA cm −2 , which is 148 mV lower than that of the low-spin state CoOOH. This work emphasizes the effect of the spin state of Co 3+ on OER activity of CoOOH based electrocatalysts for water splitting, and thus provides a new strategy for designing highly efficient…

Abstract Structure-based virtual screening is a key tool in early drug discovery, with growing interest in the screening of multi-billion chemical compound libraries. However, the success of virtual screening crucially depends on the accuracy of the binding pose and binding affinity predicted by computational docking. Here we develop a highly accurate structure-based virtual screen method, RosettaVS, for predicting docking poses and binding affinities. Our approach outperforms other state-of-the-art methods on a wide range of benchmarks, partially due to our ability to model receptor flexibility. We incorporate this into a new open-source artificial intelligence accelerated virtual screening platform for drug discovery. Using this platform, we screen multi-billion compound libraries against two unrelated targets, a ubiquitin ligase target KLHDC2 and the human voltage-gated sodium channel Na V 1.7. For both targets, we discover hit compounds, including seven hits (14% hit rate) to KLHDC2 and four hits (44% hit rate) to Na V 1.7, all with single digit micromolar binding affinities.…

Abstract Exploring new near-room-temperature thermoelectric materials is significant for replacing current high-cost Bi 2 Te 3 . This study highlights the potential of Ag 2 Se for wearable thermoelectric electronics, addressing the trade-off between performance and flexibility. A record-high ZT of 1.27 at 363 K is achieved in Ag 2 Se-based thin films with 3.2 at.% Te doping on Se sites, realized by a new concept of doping-induced orientation engineering. We reveal that Te-doping enhances film uniformity and (00 l )-orientation and in turn carrier mobility by reducing the (00 l ) formation energy, confirmed by solid computational and experimental evidence. The doping simultaneously widens the bandgap, resulting in improved Seebeck coefficients and high power factors, and introduces Te Se point defects to effectively reduce the lattice thermal conductivity. A protective organic-polymer-based composite layer enhances film flexibility, and a rationally designed flexible thermoelectric device achieves an output power density of 1.5 mW cm −2 for wearable power generation under a 20 K…

Abstract In-depth comprehension and modulation of the electronic structure of the active metal sites is crucial to enhance their intrinsic activity of electrocatalytic oxygen evolution reaction (OER) toward anion exchange membrane water electrolyzers (AEMWEs). Here, we elaborate a series of amorphous metal oxide catalysts (FeCrO x , CoCrO x and NiCrO x ) with high performance AEMWEs by high-valent chromium dopant. We discover that the positive effect of the transition from low to high valence of the Co site on the adsorption energy of the intermediate and the lower oxidation barrier is the key factor for its increased activity by synchrotron radiation in-situ techniques. Particularly, the CoCrO x anode catalyst achieves the high current density of 1.5 A cm −2 at 2.1 V and maintains for over 120 h with attenuation less than 4.9 mV h −1 in AEMWE testing. Such exceptional performance demonstrates a promising prospect for industrial application and providing general guidelines for the design of high-efficiency AEMWEs systems.

Commercial wearable piezoelectric sensors possess excellent anti-interference stability due to their electronic packaging. However, this packaging renders them barely breathable and compromises human comfort. To address this issue, we develop a PVDF piezoelectric nanoyarns with an ultrahigh strength of 313.3 MPa, weaving them with different yarns to form three-dimensional piezoelectric fabric (3DPF) sensor using the advanced 3D textile technology. The tensile strength (46.0 MPa) of 3DPF exhibits the highest among the reported flexible piezoelectric sensors. The 3DPF features anti-gravity unidirectional liquid transport that allows sweat to move from the inner layer near to the skin to the outer layer in 4 s, resulting in a comfortable and dry environment for the user. It should be noted that sweating does not weaken the piezoelectric properties of 3DPF, but rather enhances. Additionally, the durability and comfortability of 3DPF are similar to those of the commercial cotton T-shirts. This work provides a strategy for developing comfortable flexible wearable electronic devices.

Abstract Inflammatory depression is a treatment-resistant subtype of depression. A causal role of the gut microbiota as a source of low-grade inflammation remains unclear. Here, as part of an observational trial, we first analyze the gut microbiota composition in the stool, inflammatory factors and short-chain fatty acids (SCFAs) in plasma, and inflammatory and permeability markers in the intestinal mucosa of patients with inflammatory depression (ChiCTR1900025175). Gut microbiota of patients with inflammatory depression exhibits higher Bacteroides and lower Clostridium , with an increase in SCFA-producing species with abnormal butanoate metabolism. We then perform fecal microbiota transplantation (FMT) and probiotic supplementation in animal experiments to determine the causal role of the gut microbiota in inflammatory depression. After FMT, the gut microbiota of the inflammatory depression group shows increased peripheral and central inflammatory factors and intestinal mucosal permeability in recipient mice with depressive and anxiety-like behaviors. Clostridium butyricum…

Abstract Two-dimensional (2D) transition metal nitrides and carbides (MXenes), represented by Ti 3 C 2 T x , have broad applications in flexible electronics, electromechanical devices, and structural membranes due to their unique physical and chemical properties. Despite the Young’s modulus of 2D Ti 3 C 2 T x has been theoretically predicted to be 0.502 TPa, which has not been experimentally confirmed so far due to the measurement is extremely restricted. Here, by optimizing the sample preparation, cutting, and transfer protocols, we perform the direct in-situ tensile tests on monolayer Ti 3 C 2 T x nanosheets using nanomechanical push-to-pull equipment under a scanning electron microscope. The effective Young’s modulus is 0.484 ± 0.013 TPa, which is much closer to the theoretical value of 0.502 TPa than the previously reported 0.33 TPa by the disputed nanoindentation method, and the measured elastic stiffness is ~948 N/m. Moreover, during the process of tensile loading, the monolayer Ti 3 C 2 T x shows an average elastic strain of ~3.2% and a tensile strength as large as ~15.4 GPa.…

Abstract Nitrate (NO 3 ‒ ) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO 3 ‒ reduction reaction (NO 3 RR) emerges as an attractive route for enabling NO 3 ‒ removal and sustainable ammonia (NH 3 ) synthesis. However, it suffers from insufficient proton (H + ) supply in high pH conditions, restricting NO 3 ‒ -to-NH 3 activity. Herein, we propose a halogen-mediated H + feeding strategy to enhance the alkaline NO 3 RR performance. Our platform achieves near-100% NH 3 Faradaic efficiency (pH = 14) with a current density of 2 A cm –2 and enables an over 99% NO 3 – -to-NH 3 conversion efficiency. We also convert NO 3 ‒ to high-purity NH 4 Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d -band center of Pd atoms to construct local H + -abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation…

Radiative cooling is a zero-energy technology that enables subambient cooling by emitting heat into outer space (~3 K) through the atmospheric transparent windows. However, existing designs typically focus only on the main atmospheric transparent window (8-13 μm) and ignore another window (16-25 μm), under-exploiting their cooling potential. Here, we show a dual-selective radiative cooling design based on a scalable thermal emitter, which exhibits selective emission in both atmospheric transparent windows and reflection in the remaining mid-infrared and solar wavebands. As a result, the dual-selective thermal emitter exhibits an ultrahigh subambient cooling capacity (~9 °C) under strong sunlight, surpassing existing typical thermal emitters (≥3 °C cooler) and commercial counterparts (as building materials). Furthermore, the dual-selective sample also exhibits high weather resistance and color compatibility, indicating a high practicality. This work provides a scalable and practical radiative cooling design for sustainable thermal management.

Reuse and recycling of retired electric vehicle (EV) batteries offer a sustainable waste management approach but face decision-making challenges. Based on the process-based life cycle assessment method, we present a strategy to optimize pathways of retired battery treatments economically and environmentally. The strategy is applied to various reuse scenarios with capacity configurations, including energy storage systems, communication base stations, and low-speed vehicles. Hydrometallurgical, pyrometallurgical, and direct recycling considering battery residual values are evaluated at the end-of-life stage. For the optimized pathway, lithium iron phosphate (LFP) batteries improve profits by 58% and reduce emissions by 18% compared to hydrometallurgical recycling without reuse. Lithium nickel manganese cobalt oxide (NMC) batteries boost profit by 19% and reduce emissions by 18%. Despite NMC batteries exhibiting higher immediate recycling returns, LFP batteries provide superior long-term benefits through reuse before recycling. Our strategy features an accessible evaluation framework…

Abstract Ionizable lipid nanoparticles (LNPs) are seeing widespread use in mRNA delivery, notably in SARS-CoV-2 mRNA vaccines. However, the expansion of mRNA therapies beyond COVID-19 is impeded by the absence of LNPs tailored for diverse cell types. In this study, we present the AI-Guided Ionizable Lipid Engineering (AGILE) platform, a synergistic combination of deep learning and combinatorial chemistry. AGILE streamlines ionizable lipid development with efficient library design, in silico lipid screening via deep neural networks, and adaptability to diverse cell lines. Using AGILE, we rapidly design, synthesize, and evaluate ionizable lipids for mRNA delivery, selecting from a vast library. Intriguingly, AGILE reveals cell-specific preferences for ionizable lipids, indicating tailoring for optimal delivery to varying cell types. These highlight AGILE’s potential in expediting the development of customized LNPs, addressing the complex needs of mRNA delivery in clinical practice, thereby broadening the scope and efficacy of mRNA therapies.

Abstract Soil organic carbon (SOC) persistence is predominantly governed by mineral protection, consequently, soil mineral-associated (MAOC) and particulate organic carbon (POC) turnovers have different impacts on the vulnerability of SOC to climate change. Here, we generate the global MAOC and POC maps using 8341 observations and then infer the turnover times of MAOC and POC by a data-model integration approach. Global MAOC and POC storages are $${975}_{964}^{987}$$ 975 964 987 Pg C (mean with 5% and 95% quantiles) and $${330}_{323}^{337}$$ 330 323 337 Pg C, while global mean MAOC and POC turnover times are $${129}_{45}^{383}$$ 129 45 383 yr and $${23}_{5}^{82}$$ 23 5 82 yr in the top meter, respectively. Climate warming-induced acceleration of MAOC and POC decomposition is greater in subsoil than that in topsoil. Overall, the global atlas of MAOC and POC turnover, together with the global distributions of MAOC and POC stocks, provide a benchmark for Earth system models to diagnose SOC-climate change feedback.

Self-assembled monolayers (SAMs) have become pivotal in achieving high-performance perovskite solar cells (PSCs) and organic solar cells (OSCs) by significantly minimizing interfacial energy losses. In this study, we propose a co-adsorb (CA) strategy employing a novel small molecule, 2-chloro-5-(trifluoromethyl)isonicotinic acid (PyCA-3F), introducing at the buried interface between 2PACz and the perovskite/organic layers. This approach effectively diminishes 2PACz's aggregation, enhancing surface smoothness and increasing work function for the modified SAM layer, thereby providing a flattened buried interface with a favorable heterointerface for perovskite. The resultant improvements in crystallinity, minimized trap states, and augmented hole extraction and transfer capabilities have propelled power conversion efficiencies (PCEs) beyond 25% in PSCs with a p-i-n structure (certified at 24.68%). OSCs employing the CA strategy achieve remarkable PCEs of 19.51% based on PM1:PTQ10:m-BTP-PhC6 photoactive system. Notably, universal improvements have also been achieved for the other two…

Engineering natural microbiomes for biotechnological applications remains challenging, as metabolic interactions within microbiomes are largely unknown, and practical principles and tools for microbiome engineering are still lacking. Here, we present a combinatory top-down and bottom-up framework to engineer natural microbiomes for the construction of function-enhanced synthetic microbiomes. We show that application of herbicide and herbicide-degrader inoculation drives a convergent succession of different natural microbiomes toward functional microbiomes (e.g., enhanced bioremediation of herbicide-contaminated soils). We develop a metabolic modeling pipeline, SuperCC, that can be used to document metabolic interactions within microbiomes and to simulate the performances of different microbiomes. Using SuperCC, we construct bioremediation-enhanced synthetic microbiomes based on 18 keystone species identified from natural microbiomes. Our results highlight the importance of metabolic interactions in shaping microbiome functions and provide practical guidance for engineering natural…

Beneficial gut bacteria are indispensable for developing colonic mucus and fully establishing its protective function against intestinal microorganisms. Low-fiber diet consumption alters the gut bacterial configuration and disturbs this microbe-mucus interaction, but the specific bacteria and microbial metabolites responsible for maintaining mucus function remain poorly understood. By using human-to-mouse microbiota transplantation and ex vivo analysis of colonic mucus function, we here show as a proof-of-concept that individuals who increase their daily dietary fiber intake can improve the capacity of their gut microbiota to prevent diet-mediated mucus defects. Mucus growth, a critical feature of intact colonic mucus, correlated with the abundance of the gut commensal Blautia, and supplementation of Blautia coccoides to mice confirmed its mucus-stimulating capacity. Mechanistically, B. coccoides stimulated mucus growth through the production of the short-chain fatty acids propionate and acetate via activation of the short-chain fatty acid receptor Ffar2, which could serve as a new…

Abstract Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe 1 −Ti pairs on monolithic titanium electrode that exhibits an attractive NH 3 yield rate of 272,000 μg h −1 mg Fe −1 and a high NH 3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe 1 −Ti pairs (51000 μg h –1 mg Fe –1 ) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH 3 recovery unit, the simultaneous nitrate reduction and NH 3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.

Abstract The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing for energy conversion, yet remains a grand challenge. Herein, we report a class of single-atom Mo-tailored PdPtNiCuZn high-entropy-alloy nanosheets with dilute Pt-Pt ensembles and intrinsic tensile strain (Mo 1 -PdPtNiCuZn) as efficient electrocatalysts for enhancing the methanol oxidation reaction catalysis. The as-made Mo 1 -PdPtNiCuZn delivers an extraordinary mass activity of 24.55 A mg Pt −1 and 11.62 A mg Pd+Pt −1 , along with impressive long-term durability. The planted oxophilic Mo single atoms as promoters modify the electronic structure of isolated Pt sites in the high-entropy-alloy host, suppressing the formation of CO adsorbates and steering the reaction towards the formate pathway. Meanwhile, Mo promoters and tensile strain synergistically optimize the adsorption behaviour of intermediates to achieve a more energetically favourable pathway and minimize the methanol oxidation reaction barrier. This work advances the design of…

Abstract CO 2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-O V -Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kg cat −1 ·h −1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO 2 with abundant oxygen vacancies can facilitate H 2 dissociation energetically and thus improve CO 2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.

Abstract Seawater electrolysis offers a renewable, scalable, and economic means for green hydrogen production. However, anode corrosion by Cl - pose great challenges for its commercialization. Herein, different from conventional catalysts designed to repel Cl - adsorption, we develop an atomic Ir catalyst on cobalt iron layered double hydroxide (Ir/CoFe-LDH) to tailor Cl - adsorption and modulate the electronic structure of the Ir active center, thereby establishing a unique Ir-OH/Cl coordination for alkaline seawater electrolysis. Operando characterizations and theoretical calculations unveil the pivotal role of this coordination state to lower OER activation energy by a factor of 1.93. The Ir/CoFe-LDH exhibits a remarkable oxygen evolution reaction activity (202 mV overpotential and TOF = 7.46 O 2 s −1 ) in 6 M NaOH+2.8 M NaCl, superior over Cl - -free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O 2 s −1 ), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm −2 ) for more than 1,000 h.

Gastric cancer (GC) represents a significant burden of cancer-related mortality worldwide, underscoring an urgent need for the development of early detection strategies and precise postoperative interventions. However, the identification of non-invasive biomarkers for early diagnosis and patient risk stratification remains underexplored. Here, we conduct a targeted metabolomics analysis of 702 plasma samples from multi-center participants to elucidate the GC metabolic reprogramming. Our machine learning analysis reveals a 10-metabolite GC diagnostic model, which is validated in an external test set with a sensitivity of 0.905, outperforming conventional methods leveraging cancer protein markers (sensitivity < 0.40). Additionally, our machine learning-derived prognostic model demonstrates superior performance to traditional models utilizing clinical parameters and effectively stratifies patients into different risk groups to guide precision interventions. Collectively, our findings reveal the metabolic landscape of GC and identify two distinct biomarker panels that enable early…

Abstract Developing eco-friendly catalysts for effective water purification with minimal oxidant use is imperative. Herein, we present a metal-free and nitrogen/fluorine dual-site catalyst, enhancing the selectivity and utilization of singlet oxygen (1O2) for water decontamination. Advanced theoretical simulations reveal that synergistic fluorine-nitrogen interactions modulate electron distribution and polarization, creating asymmetric surface electron configurations and electron-deficient nitrogen vacancies. These properties trigger the selective generation of 1O2 from peroxymonosulfate (PMS) and improve the utilization of neighboring reactive oxygen species, facilitated by contaminant enrichment at the fluorine-carbon Lewis-acid adsorption sites. Utilizing these insights, we synthesize the catalyst through montmorillonite (MMT)-assisted pyrolysis (NFC/M). This method leverages the role of MMT as an in-situ layer-stacked template, enabling controlled decomposition of carbon, nitrogen, and fluorine precursors and resulting in a catalyst with enhanced structural adaptability,…

ChatMOF is an artificial intelligence (AI) system that is built to predict and generate metal-organic frameworks (MOFs). By leveraging a large-scale language model (GPT-4, GPT-3.5-turbo, and GPT-3.5-turbo-16k), ChatMOF extracts key details from textual inputs and delivers appropriate responses, thus eliminating the necessity for rigid and formal structured queries. The system is comprised of three core components (i.e., an agent, a toolkit, and an evaluator) and it forms a robust pipeline that manages a variety of tasks, including data retrieval, property prediction, and structure generations. ChatMOF shows high accuracy rates of 96.9% for searching, 95.7% for predicting, and 87.5% for generating tasks with GPT-4. Additionally, it successfully creates materials with user-desired properties from natural language. The study further explores the merits and constraints of utilizing large language models (LLMs) in combination with database and machine learning in material sciences and showcases its transformative potential for future advancements.

Abstract Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm−2 across wide nitrate concentrations (1–100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm−2 at −1.4 V…

Abstract The rational design of efficient bifunctional single-atom electrocatalysts for industrial water splitting and the comprehensive understanding of its complex catalytic mechanisms remain challenging. Here, we report a Ni single atoms supported on oxygen-incorporated Mo 2 C via Ni-O-Mo bridge bonds, that gives high oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) bifunctional activity. By ex situ synchrotron X-ray absorption spectroscopy and electron microscopy, we found that after HER, the coordination number and bond lengths of Ni-O and Ni-Mo (Ni-O-Mo) were all altered, yet the Ni species still remain atomically dispersed. In contrast, after OER, the atomically dispersed Ni were agglomerated into very small clusters with new Ni-Ni (Ni-O-Ni) bonds appeared. Combining experimental results and DFT calculations, we infer the oxidation degree of Mo 2 C and the configuration of single-atom Ni are both vital for HER or OER. This study provides both a feasible strategy and model to rational design highly efficient electrocatalysts for water electrolysis.

While significant advances have been made in predicting static protein structures, the inherent dynamics of proteins, modulated by ligands, are crucial for understanding protein function and facilitating drug discovery. Traditional docking methods, frequently used in studying protein-ligand interactions, typically treat proteins as rigid. While molecular dynamics simulations can propose appropriate protein conformations, they're computationally demanding due to rare transitions between biologically relevant equilibrium states. In this study, we present DynamicBind, a deep learning method that employs equivariant geometric diffusion networks to construct a smooth energy landscape, promoting efficient transitions between different equilibrium states. DynamicBind accurately recovers ligand-specific conformations from unbound protein structures without the need for holo-structures or extensive sampling. Remarkably, it demonstrates state-of-the-art performance in docking and virtual screening benchmarks. Our experiments reveal that DynamicBind can accommodate a wide range of large…

Aqueous zinc batteries are currently being explored as potential alternatives to non-aqueous lithium-ion batteries. In this comment, the authors highlight zinc’s global supply chain resilience and lower material costs yet caution about its higher mass requirement for comparable charge storage.

Abstract Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrode is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0) and low Coulombic efficiency that plague development of lithium metal batteries. But it is not known how the Li+ transfer behavior in the SEI is coupled with mechanical properties. We demonstrate here a facile and scalable solution-processed approach to form a Li3N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+ across the SEI. Compared with a polycrystalline Li3N SEI obtained from conventional practice, our phase-pure/single crystalline Li3N-rich SEI constitutes an interphase of high mechanical strength and low Li+ diffusion barrier. We elucidate the correlation among Li+ transference number, diffusion behavior, concentration gradient, and the stability of the lithium metal electrode by integrating phase field simulations with experiments. We demonstrate extreme reversibility and ultra-stable charge/discharge cycling…

Abstract Aqueous zinc batteries possess intrinsic safety and cost-effectiveness, but dendrite growth and side reactions of zinc anodes hinder their practical application. Here, we propose the extended substrate screening strategy for stabilizing zinc anodes and verify its availability (d substrate : d Zn(002) = 1: 1→d substrate : d Zn(002) =n:1, n = 1, 2). From a series of calculated phyllosilicates satisfying d substrate ≈ 2d Zn(002) , we select vermiculite, which has the lowest lattice mismatch (0.38%) reported so far, as the model to confirm the effectiveness of “2d Zn(002) ” substrates for zinc anodes protection. Then, we develop a monolayer porous vermiculite through a large-scale and green preparation as a functional coating for zinc electrodes. Unique “planting Zn(002) seeds” mechanism for “2d Zn(002) ” substrates is revealed to induce the oriented growth of zinc deposits. Additionally, the coating effectively inhibits side reactions and promotes zinc ion transport. Consequently, the modified symmetric cells operate stably for over 300 h at a high current density of 50 mA cm…

Coordination engineering of high-valent Fe(IV)-oxo (FeIV=O) is expected to break the activity-selectivity trade-off of traditional reactive oxygen species, while attempts to regulate the oxidation behaviors of heterogeneous FeIV=O remain unexplored. Here, by coordination engineering of Fe-Nx single-atom catalysts (Fe-Nx SACs), we propose a feasible approach to regulate the oxidation behaviors of heterogeneous FeIV=O. The developed Fe-N2 SACs/peroxymonosulfate (PMS) system delivers boosted performance for FeIV=O generation, and thereby can selectively remove a range of pollutants within tens of seconds. In-situ spectra and theoretical simulations suggest that low-coordination Fe-Nx SACs favor the generation of FeIV=O via PMS activation as providing more electrons to facilitate the desorption of the key *SO4H intermediate. Due to their disparate attacking sites to sulfamethoxazole (SMX) molecules, Fe-N2 SACs mediated FeIV=O (FeIVN2=O) oxidize SMX to small molecules with less toxicity, while FeIVN4=O produces series of more toxic azo compounds through N-N coupling with more complex…

Abstract The optimization of crystalline orientation of a Zn metal substrate to expose more Zn(0002) planes has been recognized as an effective strategy in pursuit of highly reversible Zn metal anodes. However, the lattice mismatch between substrate and overgrowth crystals has hampered the epitaxial sustainability of Zn metal. Herein, we discover that the presence of crystal grains deviating from [0001] orientation within a Zn(0002) metal anode leads to the failure of epitaxial mechanism. The electrodeposited [0001]-uniaxial oriented Zn metal anodes with a single (0002) texture fundamentally eliminate the lattice mismatch and achieve ultra-sustainable homoepitaxial growth. Using high-angle angular dark-filed scanning transmission electron microscopy, we elucidate the homoepitaxial growth of the deposited Zn following the “~ABABAB~” arrangement on the Zn(0002) metal from an atomic-level perspective. Such consistently epitaxial behavior of Zn metal retards dendrite formation and enables improved cycling, even in Zn||NH 4 V 4 O 10 pouch cells, with a high capacity of 220 mAh g −1 for…

Signal processing is of critical importance for various science and technology fields. Analog optical processing can provide an effective solution to perform large-scale and real-time data processing, superior to its digital counterparts, which have the disadvantages of low operation speed and large energy consumption. As an important branch of modern optics, Fourier optics exhibits great potential for analog optical image processing, for instance for edge detection. While these operations have been commonly explored to manipulate the spatial content of an image, mathematical operations that act directly over the angular spectrum of an image have not been pursued. Here, we demonstrate manipulation of the angular spectrum of an image, and in particular its differentiation, using dielectric metasurfaces operating across the whole visible spectrum. We experimentally show that this technique can be used to enhance desired portions of the angular spectrum of an image. Our approach can be extended to develop more general angular spectrum analog meta-processors, and may open opportunities…

Predictive modeling has now become a central technique in neuroimaging to identify complex brain-behavior relationships and test their generalizability to unseen data. However, data leakage, which unintentionally breaches the separation between data used to train and test the model, undermines the validity of predictive models. Previous literature suggests that leakage is generally pervasive in machine learning, but few studies have empirically evaluated the effects of leakage in neuroimaging data. Although leakage is always an incorrect practice, understanding the effects of leakage on neuroimaging predictive models provides insight into the extent to which leakage may affect the literature. Here, we investigated the effects of leakage on machine learning models in two common neuroimaging modalities, functional and structural connectomes. Using over 400 different pipelines spanning four large datasets and three phenotypes, we evaluated five forms of leakage fitting into three broad categories: feature selection, covariate correction, and lack of independence between subjects. As…

The root-associated microbiota plays an important role in the response to environmental stress. However, the underlying mechanisms controlling the interaction between salt-stressed plants and microbiota are poorly understood. Here, by focusing on a salt-tolerant plant wild soybean (Glycine soja), we demonstrate that highly conserved microbes dominated by Pseudomonas are enriched in the root and rhizosphere microbiota of salt-stressed plant. Two corresponding Pseudomonas isolates are confirmed to enhance the salt tolerance of wild soybean. Shotgun metagenomic and metatranscriptomic sequencing reveal that motility-associated genes, mainly chemotaxis and flagellar assembly, are significantly enriched and expressed in salt-treated samples. We further find that roots of salt stressed plants secreted purines, especially xanthine, which induce motility of the Pseudomonas isolates. Moreover, exogenous application for xanthine to non-stressed plants results in Pseudomonas enrichment, reproducing the microbiota shift in salt-stressed root. Finally, Pseudomonas mutant analysis shows that the…

Rapid uptake of nanoparticles by mononuclear phagocyte system (MPS) significantly hampers their therapeutic efficacy. Temporal MPS blockade is one of the few ways to overcome this barrier - the approach rediscovered many times under different names but never extensively used in clinic. Using meta-analysis of the published data we prove the efficacy of this technique for enhancing particle circulation in blood and their delivery to tumours, describe a century of its evolution and potential combined mechanism behind it. Finally, we discuss future directions of the research focusing on the features essential for successful clinical translation of the method.

The ability to scale two-dimensional (2D) material thickness down to a single monolayer presents a promising opportunity to realize high-speed energy-efficient memristors. Here, we report an ultra-fast memristor fabricated using atomically thin sheets of 2D hexagonal Boron Nitride, exhibiting the shortest observed switching speed (120 ps) among 2D memristors and low switching energy (2pJ). Furthermore, we study the switching dynamics of these memristors using ultra-short (120ps-3ns) voltage pulses, a frequency range that is highly relevant in the context of modern complementary metal oxide semiconductor (CMOS) circuits. We employ statistical analysis of transient characteristics to gain insights into the memristor switching mechanism. Cycling endurance data confirms the ultra-fast switching capability of these memristors, making them attractive for next generation computing, storage, and Radio-Frequency (RF) circuit applications.

Prediction methods inputting embeddings from protein language models have reached or even surpassed state-of-the-art performance on many protein prediction tasks. In natural language processing fine-tuning large language models has become the de facto standard. In contrast, most protein language model-based protein predictions do not back-propagate to the language model. Here, we compare the fine-tuning of three state-of-the-art models (ESM2, ProtT5, Ankh) on eight different tasks. Two results stand out. Firstly, task-specific supervised fine-tuning almost always improves downstream predictions. Secondly, parameter-efficient fine-tuning can reach similar improvements consuming substantially fewer resources at up to 4.5-fold acceleration of training over fine-tuning full models. Our results suggest to always try fine-tuning, in particular for problems with small datasets, such as for fitness landscape predictions of a single protein. For ease of adaptability, we provide easy-to-use notebooks to fine-tune all models used during this work for per-protein (pooling) and per-residue…

Fire suppression is the primary management response to wildfires in many areas globally. By removing less-extreme wildfires, this approach ensures that remaining wildfires burn under more extreme conditions. Here, we term this the "suppression bias" and use a simulation model to highlight how this bias fundamentally impacts wildfire activity, independent of fuel accumulation and climate change. We illustrate how attempting to suppress all wildfires necessarily means that fires will burn with more severe and less diverse ecological impacts, with burned area increasing at faster rates than expected from fuel accumulation or climate change. Over a human lifespan, the modeled impacts of the suppression bias exceed those from fuel accumulation or climate change alone, suggesting that suppression may exert a significant and underappreciated influence on patterns of fire globally. Managing wildfires to safely burn under low and moderate conditions is thus a critical tool to address the growing wildfire crisis.

Abstract Reducing interface nonradiative recombination is important for realizing highly efficient perovskite solar cells. In this work, we develop a synergistic bimolecular interlayer (SBI) strategy via 4-methoxyphenylphosphonic acid (MPA) and 2-phenylethylammonium iodide (PEAI) to functionalize the perovskite interface. MPA induces an in-situ chemical reaction at the perovskite surface via forming strong P-O-Pb covalent bonds that diminish the surface defect density and upshift the surface Fermi level. PEAI further creates an additional negative surface dipole so that a more n-type perovskite surface is constructed, which enhances electron extraction at the top interface. With this cooperative surface treatment, we greatly minimize interface nonradiative recombination through both enhanced defect passivation and improved energetics. The resulting p-i-n device achieves a stabilized power conversion efficiency of 25.53% and one of the smallest nonradiative recombination induced Voc loss of only 59 mV reported to date. We also obtain a certified efficiency of 25.05%. This work sheds…

Abstract Establishing appropriate metal-support interactions is imperative for acquiring efficient and corrosion-resistant catalysts for water splitting. Herein, the interaction mechanism between Ru nanoparticles and a series of titanium oxides, including TiO, Ti 4 O 7 and TiO 2, designed via facile non-stoichiometric engineering is systematically studied. Ti 4 O 7, with the unique band structure, high conductivity and chemical stability, endows with ingenious metal-support interaction through interfacial Ti–O–Ru units, which stabilizes Ru species during OER and triggers hydrogen spillover to accelerate HER kinetics. As expected, Ru/Ti 4 O 7 displays ultralow overpotentials of 8 mV and 150 mV for HER and OER with a long operation of 500 h at 10 mA cm −2 in acidic media, which is expanded in pH-universal environments. Benefitting from the excellent bifunctional performance, the proton exchange membrane and anion exchange membrane electrolyzer assembled with Ru/Ti 4 O 7 achieves superior performance and robust operation. The work paves the way for efficient energy conversion devices.

The impact of microplastics on antibiotic resistance has attracted widespread attention. However, previous studies primarily focused on the effects of individual microplastics. In reality, diverse microplastic types accumulate in soil, and it remains less well studied whether microplastic diversity (i.e., variations in color, shape or polymer type) can be an important driver of increased antibiotic resistance gene (ARG) abundance. Here, we employed microcosm studies to investigate the effects of microplastic diversity on soil ARG dynamics through metagenomic analysis. Additionally, we evaluated the associated potential health risks by profiling virulence factor genes (VFGs) and mobile genetic elements (MGEs). Our findings reveal that as microplastic diversity increases, there is a corresponding rise in the abundance of soil ARGs, VFGs and MGEs. We further identified microbial adaptive strategies involving genes (changed genetic diversity), community (increased specific microbes), and functions (enriched metabolic pathways) that correlate with increased ARG abundance and may thus…

Abstract Machine-learned potentials (MLPs) trained against quantum-mechanical reference data have demonstrated remarkable accuracy, surpassing empirical potentials. However, the absence of readily available general-purpose MLPs encompassing a broad spectrum of elements and their alloys hampers the applications of MLPs in materials science. In this study, we present a feasible approach for constructing a unified general-purpose MLP for numerous elements and showcase its capability by developing a model (UNEP-v1) for 16 elemental metals (Ag, Al, Au, Cr, Cu, Mg, Mo, Ni, Pb, Pd, Pt, Ta, Ti, V, W, Zr) and their diverse alloys. To achieve a complete representation of the chemical space, we demonstrate that employing 16 one-component and 120 two-component systems suffices, thereby avoiding the enumeration of all 65535 possible combinations for training data generation. Furthermore, we illustrate that systems with more components can be adequately represented as interpolation points in the descriptor space. Our unified MLP exhibits superior performance across various physical properties as…