The 100 most-cited articles in Nature Communications, 2023

Abstract Single cell and spatial technologies that profile gene expression across a whole tissue are revolutionizing the resolution of molecular states in clinical tissue samples. Commercially available methods that characterize either single cell or spatial gene expression are currently limited by low sample throughput and/or gene plexy, lack of on-instrument analysis, and the destruction of histological features and epitopes during the workflow. Here, we analyzed large, serial formalin-fixed, paraffin-embedded (FFPE) human breast cancer sections using a novel FFPE-compatible single cell gene expression workflow (Chromium Fixed RNA Profiling; scFFPE-seq), spatial transcriptomics (Visium CytAssist), and automated microscopy-based in situ technology using a 313-plex gene panel (Xenium In Situ). Whole transcriptome profiling of the FFPE tissue using scFFPE-seq and Visium facilitated the identification of 17 different cell types. Xenium allowed us to spatially resolve these cell types and their gene expression profiles with single cell resolution. Due to the non-destructive nature of…

Abstract Although the closed pore structure plays a key role in contributing low-voltage plateau capacity of hard carbon anode for sodium-ion batteries, the formation mechanism of closed pores is still under debate. Here, we employ waste wood-derived hard carbon as a template to systematically establish the formation mechanisms of closed pores and their effect on sodium storage performance. We find that the high crystallinity cellulose in nature wood decomposes to long-range carbon layers as the wall of closed pore, and the amorphous component can hinder the graphitization of carbon layer and induce the crispation of long-range carbon layers. The optimized sample demonstrates a high reversible capacity of 430 mAh g −1 at 20 mA g −1 (plateau capacity of 293 mAh g −1 for the second cycle), as well as good rate and stable cycling performances (85.4% after 400 cycles at 500 mA g −1 ). Deep insights into the closed pore formation will greatly forward the rational design of hard carbon anode with high capacity.

In the field of lithium-based batteries, there is often a substantial divide between academic research and industrial market needs. This is in part driven by a lack of peer-reviewed publications from industry. Here we present a non-academic view on applied research in lithium-based batteries to sharpen the focus and help bridge the gap between academic and industrial research. We focus our discussion on key metrics and challenges to be considered when developing new technologies in this industry. We also explore the need to consider various performance aspects in unison when developing a new material/technology. Moreover, we also investigate the suitability of supply chains, sustainability of materials and the impact on system-level cost as factors that need to be accounted for when working on new technologies. With these considerations in mind, we then assess the latest developments in the lithium-based battery industry, providing our views on the challenges and prospects of various technologies.

Post-translational modifications (PTMs) can occur on specific amino acids localized within regulatory domains of target proteins, which control a protein's stability. These regions, called degrons, are often controlled by PTMs, which act as signals to expedite protein degradation (PTM-activated degrons) or to forestall degradation and stabilize a protein (PTM-inactivated degrons). We summarize current knowledge of the regulation of protein stability by various PTMs. We aim to display the variety and breadth of known mechanisms of regulation as well as highlight common themes in PTM-regulated degrons to enhance potential for identifying novel drug targets where druggable targets are currently lacking.

Mechanical metamaterials enable the creation of structural materials with unprecedented mechanical properties. However, thus far, research on mechanical metamaterials has focused on passive mechanical metamaterials and the tunability of their mechanical properties. Deep integration of multifunctionality, sensing, electrical actuation, information processing, and advancing data-driven designs are grand challenges in the mechanical metamaterials community that could lead to truly intelligent mechanical metamaterials. In this perspective, we provide an overview of mechanical metamaterials within and beyond their classical mechanical functionalities. We discuss various aspects of data-driven approaches for inverse design and optimization of multifunctional mechanical metamaterials. Our aim is to provide new roadmaps for design and discovery of next-generation active and responsive mechanical metamaterials that can interact with the surrounding environment and adapt to various conditions while inheriting all outstanding mechanical features of classical mechanical metamaterials. Next, we…

ABSTRACT Spatial Transcriptomics is an emerging technology that adds spatial dimensionality and tissue morphology to the genome-wide transcriptional profile of cells in an undissociated tissue. Integrating these three types of data creates a vast potential for deciphering novel biology of cell types in their native morphological context. Here we developed innovative integrative analysis approaches to utilise all three data types to first find cell types, then reconstruct cell type evolution within a tissue, and search for tissue regions with high cell-to-cell interactions. First, for normalisation of gene expression, we compute a distance measure using morphological similarity and neighbourhood smoothing. The normalised data is then used to find clusters that represent transcriptional profiles of specific cell types and cellular phenotypes. Clusters are further sub-clustered if cells are spatially separated. Analysing anatomical regions in three mouse brain sections and 12 human brain datasets, we found the spatial clustering method more accurate and sensitive than other methods.…

Abstract Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO 3 − adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH 3 yield rate of 1.08 mmol h −1 mg −1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO 3 − and Fe/Cu promotes the adsorption and discharge of NO 3 − anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate…

Abstract Advances in spatial transcriptomics technologies have enabled the gene expression profiling of tissues while retaining its spatial context. Effective exploitation of this data combination requires spatially informed analysis tools to perform three key tasks, spatial clustering, multi-sample integration, and cell type deconvolution. Here, we present GraphST, a novel graph self-supervised contrastive learning method that incorporates spatial location information and gene expression profiles to accomplish all three tasks in a streamlined process while outperforming existing methods in each task. GraphST combines graph neural networks with self-supervised contrastive learning to learn informative and discriminative spot representations by minimizing the embedding distance between spatially adjacent spots and vice versa. With GraphST, we achieved 10% higher clustering accuracy on multiple datasets than competing methods, and better delineated the fine-grained structures in tissues such as the brain and embryo. Moreover, GraphST is the only method that can jointly analyze…

A simultaneously accurate and computationally efficient parametrization of the potential energy surface of molecules and materials is a long-standing goal in the natural sciences. While atom-centered message passing neural networks (MPNNs) have shown remarkable accuracy, their information propagation has limited the accessible length-scales. Local methods, conversely, scale to large simulations but have suffered from inferior accuracy. This work introduces Allegro, a strictly local equivariant deep neural network interatomic potential architecture that simultaneously exhibits excellent accuracy and scalability. Allegro represents a many-body potential using iterated tensor products of learned equivariant representations without atom-centered message passing. Allegro obtains improvements over state-of-the-art methods on QM9 and revMD17. A single tensor product layer outperforms existing deep MPNNs and transformers on QM9. Furthermore, Allegro displays remarkable generalization to out-of-distribution data. Molecular simulations using Allegro recover structural and kinetic properties…

Nanozymes with superoxide dismutase (SOD)-like activity have attracted increasing interest due to their ability to scavenge superoxide anion, the origin of most reactive oxygen species in vivo. However, SOD nanozymes reported thus far have yet to approach the activity of natural enzymes. Here, we report a carbon dot (C-dot) SOD nanozyme with a catalytic activity of over 10,000 U/mg, comparable to that of natural enzymes. Through selected chemical modifications and theoretical calculations, we show that the SOD-like activity of C-dots relies on the hydroxyl and carboxyl groups for binding superoxide anions and the carbonyl groups conjugated with the π-system for electron transfer. Moreover, C-dot SOD nanozymes exhibit intrinsic targeting ability to oxidation-damaged cells and effectively protect neuron cells in the ischemic stroke male mice model. Together, our study sheds light on the structure-activity relationship of C-dot SOD nanozymes, and demonstrates their potential for treating of oxidation stress related diseases.

Abstract Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na + ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational…

Non-fullerene acceptors based organic solar cells represent the frontier of the field, owing to both the materials and morphology manipulation innovations. Non-radiative recombination loss suppression and performance boosting are in the center of organic solar cell research. Here, we developed a non-monotonic intermediate state manipulation strategy for state-of-the-art organic solar cells by employing 1,3,5-trichlorobenzene as crystallization regulator, which optimizes the film crystallization process, regulates the self-organization of bulk-heterojunction in a non-monotonic manner, i.e., first enhancing and then relaxing the molecular aggregation. As a result, the excessive aggregation of non-fullerene acceptors is avoided and we have achieved efficient organic solar cells with reduced non-radiative recombination loss. In PM6:BTP-eC9 organic solar cell, our strategy successfully offers a record binary organic solar cell efficiency of 19.31% (18.93% certified) with very low non-radiative recombination loss of 0.190 eV. And lower non-radiative recombination loss of 0.168 eV is…

Abstract Extreme weather events lead to significant adverse societal costs. Extreme Event Attribution (EEA), a methodology that examines how anthropogenic greenhouse gas emissions had changed the occurrence of specific extreme weather events, allows us to quantify the climate change-induced component of these costs. We collect data from all available EEA studies, combine these with data on the socio-economic costs of these events and extrapolate for missing data to arrive at an estimate of the global costs of extreme weather attributable to climate change in the last twenty years. We find that US $$\$$$ $ 143 billion per year of the costs of extreme events is attributable to climatic change. The majority (63%), of this is due to human loss of life. Our results suggest that the frequently cited estimates of the economic costs of climate change arrived at by using Integrated Assessment Models may be substantially underestimated.

Abstract Rational design efficient transition metal-based electrocatalysts for oxygen evolution reaction (OER) is critical for water splitting. However, industrial water-alkali electrolysis requires large current densities at low overpotentials, always limited by intrinsic activity. Herein, we report hierarchical bimetal nitride/hydroxide (NiMoN/NiFe LDH) array as model catalyst, regulating the electronic states and tracking the relationship of structure-activity. As-activated NiMoN/NiFe LDH exhibits the industrially required current density of 1000 mA cm −2 at overpotential of 266 mV with 250 h stability for OER. Especially, in-situ electrochemical spectroscopic reveals that heterointerface facilitates dynamic structure evolution to optimize electronic structure. Operando electrochemical impedance spectroscopy implies accelerated OER kinetics and intermediate evolution due to fast charge transport. The OER mechanism is revealed by the combination of theoretical and experimental studies, indicating as-activated NiMoN/NiFe LDH follows lattice oxygen oxidation mechanism with…

Abstract Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance for H 2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy of Rh doping and surface oxygen vacancies to precisely regulate unconventional OER reaction path via the Ru–O–Rh active sites of Rh-RuO 2 , simultaneously boosting intrinsic activity and stability. The stabilized low-valent catalyst exhibits a remarkable performance, with an overpotential of 161 mV at 10 mA cm −2 and activity retention of 99.2% exceeding 700 h at 50 mA cm −2 . Quasi in situ/operando characterizations demonstrate the recurrence of reversible oxygen species under working potentials for enhanced activity and durability. It is theoretically revealed that Rh-RuO 2 passes through a more optimal reaction path of lattice oxygen mediated mechanism-oxygen vacancy site mechanism induced by the synergistic interaction of defects and Ru–O–Rh active sites with the rate-determining step of *O…

Blood lipids and metabolites are markers of current health and future disease risk. Here, we describe plasma nuclear magnetic resonance (NMR) biomarker data for 118,461 participants in the UK Biobank. The biomarkers cover 249 measures of lipoprotein lipids, fatty acids, and small molecules such as amino acids, ketones, and glycolysis metabolites. We provide an atlas of associations of these biomarkers to prevalence, incidence, and mortality of over 700 common diseases ( nightingalehealth.com/atlas ). The results reveal a plethora of biomarker associations, including susceptibility to infectious diseases and risk of various cancers, joint disorders, and mental health outcomes, indicating that abundant circulating lipids and metabolites are risk markers beyond cardiometabolic diseases. Clustering analyses indicate similar biomarker association patterns across different disease types, suggesting latent systemic connectivity in the susceptibility to a diverse set of diseases. This work highlights the value of NMR based metabolic biomarker profiling in large biobanks for public health…

Air pollution is one of the leading causes of health complications and mortality worldwide, especially affecting lower-income groups, who tend to be more exposed and vulnerable. This study documents the relationship between ambient air pollution exposure and poverty in 211 countries and territories. Using the World Health Organization's (WHO) 2021 revised fine particulate matter (PM2.5) thresholds, we show that globally, 7.3 billion people are directly exposed to unsafe average annual PM2.5 concentrations, 80 percent of whom live in low- and middle-income countries. Moreover, 716 million of the world's lowest income people (living on less than $1.90 per day) live in areas with unsafe levels of air pollution, especially in Sub-Saharan Africa. Air pollution levels are particularly high in lower-middle-income countries, where economies tend to rely more heavily on polluting industries and technologies. These findings are based on high-resolution air pollution and population maps with global coverage, as well as subnational poverty estimates based on harmonized household surveys.

Abstract Direct seawater electrolysis is promising for sustainable hydrogen gas (H 2 ) production. However, the chloride ions in seawater lead to side reactions and corrosion, which result in a low efficiency and poor stability of the electrocatalyst and hinder the use of seawater electrolysis technology. Here we report a corrosion-resistant RuMoNi electrocatalyst, in which the in situ-formed molybdate ions on its surface repel chloride ions. The electrocatalyst works stably for over 3000 h at a high current density of 500 mA cm −2 in alkaline seawater electrolytes. Using the RuMoNi catalyst in an anion exchange membrane electrolyzer, we report an energy conversion efficiency of 77.9% and a current density of 1000 mA cm −2 at 1.72 V. The calculated price per gallon of gasoline equivalent (GGE) of the H 2 produced is $ 0.85, which is lower than the 2026 technical target of $ 2.0/GGE set by the United Stated Department of Energy, thus, suggesting practicability of the technology.

Abstract There is an urgent need to develop effective and sustainable solutions to reduce water pollution. Heterogeneous Fenton-like catalysts are frequently used to eliminate contaminants from water. However, the applicability of these catalysts is limited due to low availability of the reactive species (RS). Herein, nanoconfinement strategy was applied to encapsulate short-lived RS at nanoscale to boost the utilization efficiency of the RS in Fenton-like reactions. The nanoconfined catalyst was fabricated by assembling Co 3 O 4 nanoparticles in carbon nanotube nanochannels to achieve exceptional reaction rate and excellent selectivity. Experiments collectively suggested that the degradation of contaminants was attributed to singlet oxygen ( 1 O 2 ). Density functional theory calculations demonstrated the nanoconfined space contributes to quantum mutation and alters the transition state to lower activation energy barriers. Simulation results revealed that the enrichment of contaminant on the catalyst reduced the migration distance and enhanced the utilization of 1 O 2 . The synergy…

Abstract The recycling of spent lithium-ion batteries is an effective approach to alleviating environmental concerns and promoting resource conservation. LiFePO 4 batteries have been widely used in electric vehicles and energy storage stations. Currently, lithium loss, resulting in formation of Fe(III) phase, is mainly responsible for the capacity fade of LiFePO 4 cathode. Another factor is poor electrical conductivity that limits its rate capability. Here, we report the use of a multifunctional organic lithium salt (3,4-dihydroxybenzonitrile dilithium) to restore spent LiFePO 4 cathode by direct regeneration. The degraded LiFePO 4 particles are well coupled with the functional groups of the organic lithium salt, so that lithium fills vacancies and cyano groups create a reductive atmosphere to inhibit Fe(III) phase. At the same time, pyrolysis of the salt produces an amorphous conductive carbon layer that coats the LiFePO 4 particles, which improves Li-ion and electron transfer kinetics. The restored LiFePO 4 cathode shows good cycling stability and rate performance (a high capacity…

Abstract Cuproptosis, caused by excessively high copper concentrations, is urgently exploited as a potential cancer therapeutic. However, the mechanisms underlying the initiation, propagation, and ultimate execution of cuproptosis in tumors remain unknown. Here, we show that copper content is significantly elevated in gastric cancer (GC), especially in malignant tumors. Screening reveals that METTL16, an atypical methyltransferase, is a critical mediator of cuproptosis through the m 6 A modification on FDX1 mRNA. Furthermore, copper stress promotes METTL16 lactylation at site K229 followed by cuproptosis. The process of METTL16 lactylation is inhibited by SIRT2. Elevated METTL16 lactylation significantly improves the therapeutic efficacy of the copper ionophore– elesclomol. Combining elesclomol with AGK2, a SIRT2-specific inhibitor, induce cuproptosis in gastric tumors in vitro and in vivo. These results reveal the significance of non-histone protein METTL16 lactylation on cuproptosis in tumors. Given the high copper and lactate concentrations in GC, cuproptosis induction becomes a…

Abstract Photocatalytic two-electron oxygen reduction to produce high-value hydrogen peroxide (H 2 O 2 ) is gaining popularity as a promising avenue of research. However, structural evolution mechanisms of catalytically active sites in the entire photosynthetic H 2 O 2 system remains unclear and seriously hinders the development of highly-active and stable H 2 O 2 photocatalysts. Herein, we report a high-loading Ni single-atom photocatalyst for efficient H 2 O 2 synthesis in pure water, achieving an apparent quantum yield of 10.9% at 420 nm and a solar-to-chemical conversion efficiency of 0.82%. Importantly, using in situ synchrotron X-ray absorption spectroscopy and Raman spectroscopy we directly observe that initial Ni-N 3 sites dynamically transform into high-valent O 1 -Ni-N 2 sites after O 2 adsorption and further evolve to form a key *OOH intermediate before finally forming HOO-Ni-N 2 . Theoretical calculations and experiments further reveal that the evolution of the active sites structure reduces the formation energy barrier of *OOH and suppresses the O=O bond dissociation,…

Covalent organic frameworks (COFs) represent an emerging class of organic photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry to construct a family of isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties and local pore characteristics of the COFs modulated using different linkers. The excited state electronic distribution and transport pathways in the COFs are probed using a host of experimental methods and theoretical calculations at a molecular level. One of our developed COFs (denoted as COF-4) exhibits a remarkable excited state electron utilization efficiency and charge transfer properties, achieving a record-high photocatalytic uranium extraction performance of ~6.84 mg/g/day in natural seawater among all techniques reported so far. This study brings a new understanding about the operation of COF-based photocatalysts, guiding the design of improved COF photocatalysts for many applications.

Photodetectors based on two-dimensional (2D) materials have been the focus of intensive research and development over the past decade. However, a gap has long persisted between fundamental research and mature applications. One of the main reasons behind this gap has been the lack of a practical and unified approach for the characterization of their figures of merit, which should be compatible with the traditional performance evaluation system of photodetectors. This is essential to determine the degree of compatibility of laboratory prototypes with industrial technologies. Here we propose general guidelines for the characterization of the figures of merit of 2D photodetectors and analyze common situations when the specific detectivity, responsivity, dark current, and speed can be misestimated. Our guidelines should help improve the standardization and industrial compatibility of 2D photodetectors.

Abstract The poor stability of Ru-based acidic oxygen evolution (OER) electrocatalysts has greatly hampered their application in polymer electrolyte membrane electrolyzers (PEMWEs). Traditional understanding of performance degradation centered on influence of bias fails in describing the stability trend, calling for deep dive into the essential origin of inactivation. Here we uncover the decisive role of reaction route (including catalytic mechanism and intermediates binding strength) on operational stability of Ru-based catalysts. Using MRuO x (M = Ce 4+ , Sn 4+ , Ru 4+ , Cr 4+ ) solid solution as structure model, we find the reaction route, thereby stability, can be customized by controlling the Ru charge. The screened SnRuO x thus exhibits orders of magnitude lifespan extension. A scalable PEMWE single cell using SnRuO x anode conveys an ever-smallest degradation rate of 53 μV h −1 during a 1300 h operation at 1 A cm −2 .

Abstract Constructing photocatalytically active and stable covalent organic frameworks containing both oxidative and reductive reaction centers remain a challenge. In this study, benzotrithiophene-based covalent organic frameworks with spatially separated redox centers are rationally designed for the photocatalytic production of hydrogen peroxide from water and oxygen without sacrificial agents. The triazine-containing framework demonstrates high selectivity for H 2 O 2 photogeneration, with a yield rate of 2111 μM h −1 (21.11 μmol h −1 and 1407 μmol g −1 h −1 ) and a solar-to-chemical conversion efficiency of 0.296%. Codirectional charge transfer and large energetic differences between linkages and linkers are verified in the double donor-acceptor structures of periodic frameworks. The active sites are mainly concentrated on the electron-acceptor fragments near the imine bond, which regulate the electron distribution of adjacent carbon atoms to optimally reduce the Gibbs free energy of O 2 * and OOH* intermediates during the formation of H 2 O 2 .

Abstract The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (Au SA -MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm −2 and high mass activity of 732.925 A g −1 at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm −2 . Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2 p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity.

Solid polymer electrolytes (SPEs) and hydrogel electrolytes were developed as electrolytes for zinc ion batteries (ZIBs). Hydrogels can retain water molecules and provide high ionic conductivities; however, they contain many free water molecules, inevitably causing side reactions on the zinc anode. SPEs can enhance the stability of anodes, but they typically possess low ionic conductivities and result in high impedance. Here, we develop a lean water hydrogel electrolyte, aiming to balance ion transfer, anode stability, electrochemical stability window and resistance. This hydrogel is equipped with a molecular lubrication mechanism to ensure fast ion transportation. Additionally, this design leads to a widened electrochemical stability window and highly reversible zinc plating/ stripping. The full cell shows excellent cycling stability and capacity retentions at high and low current rates, respectively. Moreover, superior adhesion ability can be achieved, meeting the needs of flexible devices.

Anthropogenic activities profoundly impact soil organic carbon (SOC), affecting its contribution to ecosystem services such as climate regulation. Here, we conducted a thorough review of the impacts of land-use change, land management, and climate change on SOC. Using second-order meta-analysis, we synthesized findings from 230 first-order meta-analyses comprising over 25,000 primary studies. We show that (i) land conversion for crop production leads to high SOC loss, that can be partially restored through land management practices, particularly by introducing trees and incorporating exogenous carbon in the form of biochar or organic amendments, (ii) land management practices that are implemented in forests generally result in depletion of SOC, and (iii) indirect effects of climate change, such as through wildfires, have a greater impact on SOC than direct climate change effects (e.g., from rising temperatures). The findings of our study provide strong evidence to assist decision-makers in safeguarding SOC stocks and promoting land management practices for SOC restoration.…

Much research focuses on increasing carbon storage in mineral-associated organic matter (MAOM), in which carbon may persist for centuries to millennia. However, MAOM-targeted management is insufficient because the formation pathways of persistent soil organic matter are diverse and vary with environmental conditions. Effective management must also consider particulate organic matter (POM). In many soils, there is potential for enlarging POM pools, POM can persist over long time scales, and POM can be a direct precursor of MAOM. We present a framework for context-dependent management strategies that recognizes soils as complex systems in which environmental conditions constrain POM and MAOM formation.

Abstract Metallic zinc anodes of aqueous zinc ion batteries suffer from severe dendrite and side reaction issues, resulting in poor cycling stability, especially at high rates and capacities. Herein, we develop two three-dimensional hierarchical graphene matrices consisting of nitrogen-doped graphene nanofibers clusters anchored on vertical graphene arrays of modified multichannel carbon. The graphene matrix with radial direction carbon channels possesses high surface area and porosity, which effectively minimizes the surface local current density, manipulates the Zn 2+ ions concentration gradient, and homogenizes the electric field distribution to regulate Zn deposition. As a result, the engineered matrices achieve a superior coulombic efficiency of 99.67% over 3000 cycles at 120 mA cm −2 , the symmetric cells with the composite zinc anode demonstrates 2600 h dendrite-free cycles at 80 mA cm −2 and 80 mAh cm −2 . The as-designed full cell exhibits an inspiring capacity of 16.91 mAh cm −2 . The Zn capacitor matched with activated carbon shows a superior long-term cycle performance…

Abstract The strong excitonic effects widely exist in polymer-semiconductors and the large exciton binding energy (Eb) seriously limits their photocatalysis. Herein, density functional theory (DFT) calculations are conducted to assess band alignment and charge transfer feature of potential donor-acceptor (D-A) covalent organic frameworks (COFs), using 1,3,5-tris(4-aminophenyl)triazine (TAPT) or 1,3,5-tris(4-aminophenyl)benzene (TAPB) as acceptors and tereph-thaldehydes functionalized diverse groups as donors. Given the discernable D-A interaction strengths in the D-A pairs, their Eb can be systematically regulated with minimum Eb in TAPT-OMe. Guided by these results, the corresponding D-A COFs are synthesized, where TAPT-OMe-COF possesses the best activity in photocatalytic H2 production and the activity trend of other COFs is associated with that of calculated Eb for the D-A pairs. In addition, further alkyne cycloaddition for the imine linkage in the COFs greatly improves the stability and the resulting TAPT-OMe-alkyne-COF with a substantially smaller Eb exhibits ~20 times higher…

Abstract The mitigation scenarios database of the Intergovernmental Panel on Climate Change’s Sixth Assessment Report is an important resource for informing policymaking on energy transitions. However, there is a large variety of models, scenario designs, and resulting outputs. Here we analyse the scenarios consistent with limiting warming to 2 °C or below regarding the speed, trajectory, and feasibility of different fossil fuel reduction pathways. In scenarios limiting warming to 1.5 °C with no or limited overshoot, global coal, oil, and natural gas supply (intended for all uses) decline on average by 95%, 62%, and 42%, respectively, from 2020 to 2050, but the long-term role of gas is highly variable. Higher-gas pathways are enabled by higher carbon capture and storage (CCS) and carbon dioxide removal (CDR), but are likely associated with inadequate model representation of regional CO 2 storage capacity and technology adoption, diffusion, and path-dependencies. If CDR is constrained by limits derived from expert consensus, the respective modelled coal, oil, and gas reductions…

Abstract The fitness effects of all possible mutations available to an organism largely shape the dynamics of evolutionary adaptation. Yet, whether and how this adaptive landscape changes over evolutionary times, especially upon ecological diversification and changes in community composition, remains poorly understood. We sought to fill this gap by analyzing a stable community of two closely related ecotypes (“L” and “S”) shortly after they emerged within the E. coli Long-Term Evolution Experiment (LTEE). We engineered genome-wide barcoded transposon libraries to measure the invasion fitness effects of all possible gene knockouts in the coexisting strains as well as their ancestor, for many different, ecologically relevant conditions. We find consistent statistical patterns of fitness effect variation across both genetic background and community composition, despite the idiosyncratic behavior of individual knockouts. Additionally, fitness effects are correlated with evolutionary outcomes for a number of conditions, possibly revealing shifting patterns of adaptation. Together, our…

Abstract Achieving low-carbon development of the cement industry in the developing countries is fundamental to global emissions abatement, considering the local construction industry’s rapid growth. However, there is currently a lack of systematic and accurate accounting and projection of cement emissions in developing countries, which are characterized with lower basic economic country condition. Here, we provide bottom-up quantifications of emissions from global cement production and reveal a regional shift in the main contributors to global cement CO 2 emissions. The study further explores cement emissions over 2020-2050 that correspond to different housing and infrastructure conditions and emissions mitigation options for all developing countries except China. We find that cement emissions in developing countries except China will reach 1.4-3.8 Gt in 2050 (depending on different industrialization trajectories), compared to their annual emissions of 0.7 Gt in 2018. The optimal combination of low-carbon measures could contribute to reducing annual emissions by around 65% in 2050…

In late June 2021 a heatwave of unprecedented magnitude impacted the Pacific Northwest region of Canada and the United States. Many locations broke all-time maximum temperature records by more than 5 °C, and the Canadian national temperature record was broken by 4.6 °C, with a new record temperature of 49.6 °C. Here, we provide a comprehensive summary of this event and its impacts. Upstream diabatic heating played a key role in the magnitude of this anomaly. Weather forecasts provided advanced notice of the event, while sub-seasonal forecasts showed an increased likelihood of a heat extreme with lead times of 10-20 days. The impacts of this event were catastrophic, including hundreds of attributable deaths across the Pacific Northwest, mass-mortalities of marine life, reduced crop and fruit yields, river flooding from rapid snow and glacier melt, and a substantial increase in wildfires-the latter contributing to landslides in the months following. These impacts provide examples we can learn from and a vivid depiction of how climate change can be so devastating.

Abstract Aqueous Zn-ion batteries have attracted increasing research interest; however, the development of these batteries has been hindered by several challenges, including dendrite growth, Zn corrosion, cathode material degradation, limited temperature adaptability and electrochemical stability window, which are associated with water activity and the solvation structure of electrolytes. Here we report that water activity is suppressed by increasing the electron density of the water protons through interactions with highly polar dimethylacetamide and trimethyl phosphate molecules. Meanwhile, the Zn corrosion in the hybrid electrolyte is mitigated, and the electrochemical stability window and the operating temperature of the electrolyte are extended. The dimethylacetamide alters the surface energy of Zn, guiding the (002) plane dominated deposition of Zn. Molecular dynamics simulation evidences Zn 2+ ions are solvated with fewer water molecules, resulting in lower lattice strain in the NaV 3 O 8 ·1.5H 2 O cathode during the insertion of hydrated Zn 2+ ions, boosting the lifespan of…

Abstract Progress towards the integration of technology into living organisms requires power devices that are biocompatible and mechanically flexible. Aqueous zinc ion batteries that use hydrogel biomaterials as electrolytes have emerged as a potential solution that operates within biological constraints; however, most of these batteries feature inferior electrochemical properties. Here, we propose a biocompatible hydrogel electrolyte by utilising hyaluronic acid, which contains ample hydrophilic functional groups. The gel-based electrolyte offers excellent anti-corrosion ability for zinc anodes and regulates zinc nucleation/growth. Also, the gel electrolyte provides high battery performance, including a 99.71% Coulombic efficiency, over 5500 hours of long-term stability, improved cycle life of 250 hours under a high zinc utilization rate of 80%, and high biocompatibility. Importantly, the Zn//LiMn 2 O 4 pouch cell exhibits 82% capacity retention after 1000 cycles at 3 C. This work presents a promising gel chemistry that controls zinc behaviour, offering great potential in…

Before the debut of lithium-ion batteries (LIBs) in the commodity market, solid-state lithium metal batteries (SSLMBs) were considered promising high-energy electrochemical energy storage systems before being almost abandoned in the late 1980s because of safety concerns. However, after three decades of development, LIB technologies are now approaching their energy content and safety limits imposed by the rocking chair chemistry. These aspects are prompting the revival of research activities in SSLMB technologies at both academic and industrial levels. In this perspective article, we present a personal reflection on solid polymer electrolytes (SPEs), spanning from early development to their implementation in SSLMBs, highlighting key milestones. In particular, we discuss the SPEs' characteristics taking into account the concept of coupled and decoupled SPEs proposed by C. Austen Angell in the early 1990s. Possible remedies to improve the physicochemical and electrochemical properties of SPEs are also examined. With this article, we also aim to highlight the missing blocks in building…

The Atlantic meridional overturning circulation (AMOC) is a major tipping element in the climate system and a future collapse would have severe impacts on the climate in the North Atlantic region. In recent years weakening in circulation has been reported, but assessments by the Intergovernmental Panel on Climate Change (IPCC), based on the Climate Model Intercomparison Project (CMIP) model simulations suggest that a full collapse is unlikely within the 21st century. Tipping to an undesired state in the climate is, however, a growing concern with increasing greenhouse gas concentrations. Predictions based on observations rely on detecting early-warning signals, primarily an increase in variance (loss of resilience) and increased autocorrelation (critical slowing down), which have recently been reported for the AMOC. Here we provide statistical significance and data-driven estimators for the time of tipping. We estimate a collapse of the AMOC to occur around mid-century under the current scenario of future emissions.

Abstract Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg −1 . Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF 4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions’ decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO 2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg −1 with 80% capacity retention after 100 cycles.

ABSTRACT Highly pathogenic avian influenza (HPAI) A/H5N1 viruses (lineage 2.3.4.4b) are rapidly invading the Americas, threatening wildlife, poultry, and potentially evolving into the next global pandemic. In November 2022, HPAI arrived in Peru, where massive pelican and sea lion die-offs are still underway. We report complete genomic characterization of HPAI/H5N1 viruses in five species of marine mammals and seabirds (dolphins, sea lions, sanderlings, pelicans and cormorants) sampled since November 2022. All Peruvian viruses belong to the HPAI A/H5N1 lineage 2.3.4.4b, but they are 4:4 reassortants where 4 genomic segments (PA, HA, NA and MP) position within the Eurasian lineage that initially entered North America from Eurasia, while the other 4 genomic segments (PB2, PB1, NP and NS) position within the American lineage (clade C) that was already circulating in North America. These viruses are rapidly accruing mutations as they spread south. Peruvian viruses do not contain PB2 E627K or D701N mutations linked to mammalian host adaptation and enhanced transmission, but at least 8…

State of health is a critical state which evaluates the degradation level of batteries. However, it cannot be measured directly but requires estimation. While accurate state of health estimation has progressed markedly, the time- and resource-consuming degradation experiments to generate target battery labels hinder the development of state of health estimation methods. In this article, we design a deep-learning framework to enable the estimation of battery state of health in the absence of target battery labels. This framework integrates a swarm of deep neural networks equipped with domain adaptation to produce accurate estimation. We employ 65 commercial batteries from 5 different manufacturers to generate 71,588 samples for cross-validation. The validation results indicate that the proposed framework can ensure absolute errors of less than 3% for 89.4% of samples (less than 5% for 98.9% of samples), with a maximum absolute error of less than 8.87% in the absence of target labels. This work emphasizes the power of deep learning in precluding degradation experiments and highlights…

Cancer-associated fibroblasts (CAFs) are a diverse cell population within the tumour microenvironment, where they have critical effects on tumour evolution and patient prognosis. To define CAF phenotypes, we analyse a single-cell RNA sequencing (scRNA-seq) dataset of over 16,000 stromal cells from tumours of 14 breast cancer patients, based on which we define and functionally annotate nine CAF phenotypes and one class of pericytes. We validate this classification system in four additional cancer types and use highly multiplexed imaging mass cytometry on matched breast cancer samples to confirm our defined CAF phenotypes at the protein level and to analyse their spatial distribution within tumours. This general CAF classification scheme will allow comparison of CAF phenotypes across studies, facilitate analysis of their functional roles, and potentially guide development of new treatment strategies in the future.

Polydopamine is a biomimetic self-adherent polymer, which can be easily deposited on a wide variety of materials. Despite the rapidly increasing interest in polydopamine-based coatings, the polymerization mechanism and the key intermediate species formed during the deposition process are still controversial. Herein, we report a systematic investigation of polydopamine formation on halloysite nanotubes; the negative charge and high surface area of halloysite nanotubes favour the capture of intermediates that are involved in polydopamine formation and decelerate the kinetics of the process, to unravel the various polymerization steps. Data from X-ray photoelectron and solid-state nuclear magnetic resonance spectroscopies demonstrate that in the initial stage of polydopamine deposition, oxidative coupling reaction of the dopaminechrome molecules is the main reaction pathway that leads to formation of polycatecholamine oligomers as an intermediate and the post cyclization of the linear oligomers occurs subsequently. Furthermore, TRIS molecules are incorporated into the initially formed…

Abstract Heteroatom-doping is a practical means to boost RuO2 for acidic oxygen evolution reaction (OER). However, a major drawback is conventional dopants have static electron redistribution. Here, we report that Re dopants in Re0.06Ru0.94O2 undergo a dynamic electron accepting-donating that adaptively boosts activity and stability, which is different from conventional dopants with static dopant electron redistribution. We show Re dopants during OER, (1) accept electrons at the on-site potential to activate Ru site, and (2) donate electrons back at large overpotential and prevent Ru dissolution. We confirm via in situ characterizations and first-principle computation that the dynamic electron-interaction between Re and Ru facilitates the adsorbate evolution mechanism and lowers adsorption energies for oxygen intermediates to boost activity and stability of Re0.06Ru0.94O2. We demonstrate a high mass activity of 500 A gcata.−1 (7811 A gRe-Ru−1) and a high stability number of S-number = 4.0 × 106 noxygen nRu−1 to outperform most electrocatalysts. We conclude that dynamic dopants can…

Operando monitoring of complex physical and chemical activities inside rechargeable lithium-ion batteries during thermal runaway is critical to understanding thermal runaway mechanisms and giving early warning of safety-related failure. However, most existing sensors cannot survive during such extremely hazardous thermal runaway processes (temperature up to 500 °C accompanied by fire and explosion). To address this, we develop a compact and multifunctional optical fiber sensor (12 mm in length and 125 µm in diameter) capable of insertion into commercial 18650 cells to continuously monitor internal temperature and pressure effects during cell thermal runaway. We observe a stable and reproducible correlation between the cell thermal runaway and the optical response. The sensor's signal shows two internal pressure peaks corresponding to safety venting and initiation of thermal runaway. Further analysis reveals that a scalable solution for predicting imminent thermal runaway is the detection of the abrupt turning range of the differential curves of cell temperature and pressure, which…

Early cancer detection has significant clinical value, but there remains no single method that can comprehensively identify multiple types of early-stage cancer. Here, we report the diagnostic accuracy of simultaneous detection of 6 types of early-stage cancers (lung, breast, colon, liver, pancreas, and stomach) by analyzing surface-enhanced Raman spectroscopy profiles of exosomes using artificial intelligence in a retrospective study design. It includes classification models that recognize signal patterns of plasma exosomes to identify both their presence and tissues of origin. Using 520 test samples, our system identified cancer presence with an area under the curve value of 0.970. Moreover, the system classified the tumor organ type of 278 early-stage cancer patients with a mean area under the curve of 0.945. The final integrated decision model showed a sensitivity of 90.2% at a specificity of 94.4% while predicting the tumor organ of 72% of positive patients. Since our method utilizes a non-specific analysis of Raman signatures, its diagnostic scope could potentially be expanded…

Recently it has become possible to de novo design high affinity protein binding proteins from target structural information alone. There is, however, considerable room for improvement as the overall design success rate is low. Here, we explore the augmentation of energy-based protein binder design using deep learning. We find that using AlphaFold2 or RoseTTAFold to assess the probability that a designed sequence adopts the designed monomer structure, and the probability that this structure binds the target as designed, increases design success rates nearly 10-fold. We find further that sequence design using ProteinMPNN rather than Rosetta considerably increases computational efficiency.

Abstract Despite the extensive developments of flexible capacitive pressure sensors, it is still elusive to simultaneously achieve excellent linearity over a broad pressure range, high sensitivity, and ultrahigh pressure resolution under large pressure preloads at low cost. This work presents a facile and low-cost fabrication method to integrate an ultrathin ionic layer with gradient microstructures with programmable profiles and heights created by a simple CO2 laser. The coupled electrical and mechanical simulations provide a route to optimize the design of iontronic pressure sensors based on the electric double layer to address the existing challenges for significantly improved pressure sensing performance. The resulting optimized sensor exhibits a high sensitivity of 33 kPa− 1 over an ultra-board linear sensing range of 1700 kPa, an ultralow detection limit of 0.36 Pa, and a pressure resolution of 0.00725% under ultrahigh pressure of 2000 kPa. Taken together with a rapid response/recovery time of 4/16 ms and excellent repeatability over 4,500 cycles, the sensor has been applied…

Decarbonisation plans across the globe require zero-carbon energy sources to be widely deployed by 2050 or 2060. Solar energy is the most widely available energy resource on Earth, and its economic attractiveness is improving fast in a cycle of increasing investments. Here we use data-driven conditional technology and economic forecasting modelling to establish which zero carbon power sources could become dominant worldwide. We find that, due to technological trajectories set in motion by past policy, a global irreversible solar tipping point may have passed where solar energy gradually comes to dominate global electricity markets, without any further climate policies. Uncertainties arise, however, over grid stability in a renewables-dominated power system, the availability of sufficient finance in underdeveloped economies, the capacity of supply chains and political resistance from regions that lose employment. Policies resolving these barriers may be more effective than price instruments to accelerate the transition to clean energy.

Designing and printing metamaterials with customizable architectures enables the realization of unprecedented mechanical behaviors that transcend those of their constituent materials. These behaviors are recorded in the form of response curves, with stress-strain curves describing their quasi-static footprint. However, existing inverse design approaches are yet matured to capture the full desired behaviors due to challenges stemmed from multiple design objectives, nonlinear behavior, and process-dependent manufacturing errors. Here, we report a rapid inverse design methodology, leveraging generative machine learning and desktop additive manufacturing, which enables the creation of nearly all possible uniaxial compressive stress‒strain curve cases while accounting for process-dependent errors from printing. Results show that mechanical behavior with full tailorability can be achieved with nearly 90% fidelity between target and experimentally measured results. Our approach represents a starting point to inverse design materials that meet prescribed yet complex behaviors and…

Abstract Solar-driven photosynthesis is a sustainable process for the production of hydrogen peroxide, the efficiency of which is plagued by side reactions. Metal-free covalent organic frameworks (COFs) that can form suitable intermediates and inhibit side reactions show great promise to photo-synthesize H 2 O 2 . However, the insufficient formation and separation/transfer of photogenerated charges in such materials restricts the efficiency of H 2 O 2 production. Herein, we provide a strategy for the design of donor-acceptor COFs to greatly boost H 2 O 2 photosynthesis. We demonstrate that the optimal intramolecular polarity of COFs, achieved by using suitable amounts of phenyl groups as electron donors, can maximize the free charge generation, which leads to high H 2 O 2 yield rates (605 μmol g −1 h −1 ) from water, oxygen and visible light without sacrificial agents. Combining in-situ characterization with computational calculations, we describe how the triazine N-sites with optimal N 2p states play a crucial role in H 2 O activation and selective oxidation into H 2 O 2 . We…

Protein-based therapeutics have led to new paradigms in disease treatment. Projected to be half of the top ten selling drugs in 2023, proteins have emerged as rivaling and, in some cases, superior alternatives to historically used small molecule-based medicines. This review chronicles both well-established and emerging design strategies that have enabled this paradigm shift by transforming protein-based structures that are often prone to denaturation, degradation, and aggregation in vitro and in vivo into highly effective therapeutics. In particular, we discuss strategies for creating structures with increased affinity and targetability, enhanced in vivo stability and pharmacokinetics, improved cell permeability, and reduced amounts of undesired immunogenicity.

Abstract Oxygen evolution reaction catalysts capable of working efficiently in acidic media are highly demanded for the commercialization of proton exchange membrane water electrolysis. Herein, we report a Zn-doped RuO 2 nanowire array electrocatalyst with outstanding catalytic performance for the oxygen evolution reaction under acidic conditions. Overpotentials as low as 173, 304, and 373 mV are achieved at 10, 500, and 1000 mA cm −2 , respectively, with robust stability reaching to 1000 h at 10 mA cm −2 . Experimental and theoretical investigations establish a clear synergistic effect of Zn dopants and oxygen vacancies on regulating the binding configurations of oxygenated adsorbates on the active centers, which then enables an alternative Ru−Zn dual-site oxide path of the reaction. Due to the change of reaction pathways, the energy barrier of rate-determining step is reduced, and the over-oxidation of Ru active sites is alleviated. As a result, the catalytic activity and stability are significantly enhanced.

Abstract The slow redox kinetics of polysulfides and the difficulties in decomposition of Li2S during the charge and discharge processes are two serious obstacles to the practical application of lithium-sulfur batteries. Herein, we construct the Fe-Co diatomic catalytic materials supported by hollow carbon spheres to achieve high-efficiency catalysis for the conversion of polysulfides and the decomposition of Li2S simultaneously. The Fe atom center is beneficial to accelerate the discharge reaction process, and the Co atom center is favorable for charging process. Theoretical calculations combined with experiments reveal that this excellent bifunctional catalytic activity originates from the diatomic synergy between Fe and Co atom. As a result, the assembled cells exhibit the high rate performance (the discharge specific capacity achieves 688 mAh g−1 at 5 C) and the excellent cycle stability (the capacity decay rate is 0.018% for 1000 cycles at 1 C).

The standard primitives of quantum computing include deterministic unitary entangling gates, which are not natural operations in many systems including photonics. Here, we present fusion-based quantum computation, a model for fault tolerant quantum computing constructed from physical primitives readily accessible in photonic systems. These are entangling measurements, called fusions, which are performed on the qubits of small constant sized entangled resource states. Probabilistic photonic gates as well as errors are directly dealt with by the quantum error correction protocol. We show that this computational model can achieve a higher threshold than schemes reported in literature. We present a ballistic scheme which can tolerate a 10.4% probability of suffering photon loss in each fusion, which corresponds to a 2.7% probability of loss of each individual photon. The architecture is also highly modular and has reduced classical processing requirements compared to previous photonic quantum computing architectures.

Incorporating mixed ion is a frequently used strategy to stabilize black-phase formamidinum lead iodide perovskite for high-efficiency solar cells. However, these devices commonly suffer from photoinduced phase segregation and humidity instability. Herein, we find that the underlying reason is that the mixed halide perovskites generally fail to grow into homogenous and high-crystalline film, due to the multiple pathways of crystal nucleation originating from various intermediate phases in the film-forming process. Therefore, we design a multifunctional fluorinated additive, which restrains the complicated intermediate phases and promotes orientated crystallization of α-phase of perovskite. Furthermore, the additives in-situ polymerize during the perovskite film formation and form a hydrogen-bonded network to stabilize α-phase. Remarkably, the polymerized additives endow a strongly hydrophobic effect to the bare perovskite film against liquid water for 5 min. The unencapsulated devices achieve 24.10% efficiency and maintain >95% of the initial efficiency for 1000 h under continuous…

Pancreatic cancer is characterized by abundant desmoplasia, a dense stroma composed of extra-cellular and cellular components, with cancer associated fibroblasts (CAFs) being the major cellular component. However, the tissue(s) of origin for CAFs remains controversial. Here we determine the tissue origin of pancreatic CAFs through comprehensive lineage tracing studies in mice. We find that the splanchnic mesenchyme, the fetal cell layer surrounding the endoderm from which the pancreatic epithelium originates, gives rise to the majority of resident fibroblasts in the normal pancreas. In a genetic mouse model of pancreatic cancer, resident fibroblasts expand and constitute the bulk of CAFs. Single cell RNA profiling identifies gene expression signatures that are shared among the fetal splanchnic mesenchyme, adult fibroblasts and CAFs, suggesting a persistent transcriptional program underlies splanchnic lineage differentiation. Together, this study defines the phylogeny of the mesenchymal component of the pancreas and provides insights into pancreatic morphogenesis and tumorigenesis.

Abstract The remarkable advantages of heterointerface and defect engineering and their unique electromagnetic characteristics inject infinite vitality into the design of advanced carbon-matrix electromagnetic wave absorbers. However, understanding the interface and dipole effects based on microscopic and macroscopic perspectives, rather than semi-empirical rules, can facilitate the design of heterointerfaces and defects to adjust the impedance matching and electromagnetic wave absorption of the material, which is currently lacking. Herein, CuCo 2 S 4 @Expanded Graphite heterostructure with multiple heterointerfaces and cation defects are reported, and the morphology, interfaces and defects of component are regulated by varying the concentration of metal ions. The results show that the 3D flower-honeycomb morphology, the crystal-crystal/amorphous heterointerfaces and the abundant cation defects can effectively adjust the conductive and polarization losses, achieve the impedance matching balance of carbon materials, and improve the absorption of electromagnetic wave. For the sample…

Abstract Electrochemical CO 2 reduction (CO 2 R) to ethylene and ethanol enables the long-term storage of renewable electricity in valuable multi-carbon (C 2+ ) chemicals. However, carbon–carbon (C–C) coupling, the rate-determining step in CO 2 R to C 2+ conversion, has low efficiency and poor stability, especially in acid conditions. Here we find that, through alloying strategies, neighbouring binary sites enable asymmetric CO binding energies to promote CO 2 -to-C 2+ electroreduction beyond the scaling-relation-determined activity limits on single-metal surfaces. We fabricate experimentally a series of Zn incorporated Cu catalysts that show increased asymmetric CO* binding and surface CO* coverage for fast C–C coupling and the consequent hydrogenation under electrochemical reduction conditions. Further optimization of the reaction environment at nanointerfaces suppresses hydrogen evolution and improves CO 2 utilization under acidic conditions. We achieve, as a result, a high 31 ± 2% single-pass CO 2 -to-C 2+ yield in a mild-acid pH 4 electrolyte with >80% single-pass CO 2…

Abstract Photochemical conversion of CO 2 into high-value C 2+ products is difficult to achieve due to the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for the conversion of CO 2 into C 3 H 8 is prepared by implanting Cu single atoms on Ti 0.91 O 2 atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (V O s) in Ti 0.91 O 2 matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-V O unit in Ti 0.91 O 2 matrix. A high electron-based selectivity of 64.8% for C 3 H 8 (product-based selectivity of 32.4%), and 86.2% for total C 2+ hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-V O unit may stabilize the key *CHOCO and *CH 2 OCOCO intermediates and reduce their energy levels, tuning both C 1 -C 1 and C 1 -C 2 couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are…

Abstract Achieving long-term stable zinc anodes at high currents/capacities remains a great challenge for practical rechargeable zinc-ion batteries. Herein, we report an imprinted gradient zinc electrode that integrates gradient conductivity and hydrophilicity for long-term dendrite-free zinc-ion batteries. The gradient design not only effectively prohibits side reactions between the electrolyte and the zinc anode, but also synergistically optimizes electric field distribution, zinc ion flux and local current density, which induces preferentially deposited zinc in the bottom of the microchannels and suppresses dendrite growth even under high current densities/capacities. As a result, the imprinted gradient zinc anode can be stably cycled for 200 h at a high current density/capacity of 10 mA cm −2 /10 mAh cm −2 , with a high cumulative capacity of 1000 mAh cm −2 , which outperforms the none-gradient counterparts and bare zinc. The imprinted gradient design can be easily scaled up, and a high-performance large-area pouch cell (4*5 cm 2 ) is also demonstrated.

The dendrite growth of zinc and the side reactions including hydrogen evolution often degrade performances of zinc-based batteries. These issues are closely related to the desolvation process of hydrated zinc ions. Here we show that the efficient regulation on the solvation structure and chemical properties of hydrated zinc ions can be achieved by adjusting the coordination micro-environment with zinc phenolsulfonate and tetrabutylammonium 4-toluenesulfonate as a family of electrolytes. The theoretical understanding and in-situ spectroscopy analysis revealed that the favorable coordination of conjugated anions involved in hydrogn bond network minimizes the activate water molecules of hydrated zinc ion, thus improving the zinc/electrolyte interface stability to suppress the dendrite growth and side reactions. With the reversibly cycling of zinc electrode over 2000 h with a low overpotential of 17.7 mV, the full battery with polyaniline cathode demonstrated the impressive cycling stability for 10000 cycles. This work provides inspiring fundamental principles to design advanced…

Abstract The cystine transporter solute carrier family 7 member 11 (SLC7A11; also called xCT) protects cancer cells from oxidative stress and is overexpressed in many cancers. Here we report a surprising finding that, whereas moderate overexpression of SLC7A11 is beneficial for cancer cells treated with H 2 O 2 , a common oxidative stress inducer, its high overexpression dramatically increases H 2 O 2 -induced cell death. Mechanistically, high cystine uptake in cancer cells with high overexpression of SLC7A11 in combination with H 2 O 2 treatment results in toxic buildup of intracellular cystine and other disulfide molecules, NADPH depletion, redox system collapse, and rapid cell death (likely disulfidptosis). We further show that high overexpression of SLC7A11 promotes tumor growth but suppresses tumor metastasis, likely because metastasizing cancer cells with high expression of SLC7A11 are particularly susceptible to oxidative stress. Our findings reveal that SLC7A11 expression level dictates cancer cells’ sensitivity to oxidative stress and suggests a context-dependent role for…

Bacteria from the Turicibacter genus are prominent members of the mammalian gut microbiota and correlate with alterations in dietary fat and body weight, but the specific connections between these symbionts and host physiology are poorly understood. To address this knowledge gap, we characterize a diverse set of mouse- and human-derived Turicibacter isolates, and find they group into clades that differ in their transformations of specific bile acids. We identify Turicibacter bile salt hydrolases that confer strain-specific differences in bile deconjugation. Using male and female gnotobiotic mice, we find colonization with individual Turicibacter strains leads to changes in host bile acid profiles, generally aligning with those produced in vitro. Further, colonizing mice with another bacterium exogenously expressing bile-modifying genes from Turicibacter strains decreases serum cholesterol, triglycerides, and adipose tissue mass. This identifies genes that enable Turicibacter strains to modify host bile acids and lipid metabolism, and positions Turicibacter bacteria as modulators of…

Abstract The electrochemical stability window of the electrolyte solution limits the energy content of non-aqueous lithium metal batteries. In particular, although electrolytes comprising fluorinated solvents show good oxidation stability against high-voltage positive electrode active materials such as LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), the ionic conductivity is adversely affected and, thus, the battery cycling performance at high current rates and low temperatures. To address these issues, here we report the design and synthesis of a monofluoride ether as an electrolyte solvent with Li-F and Li-O tridentate coordination chemistries. The monofluoro substituent (-CH 2 F) in the solvent molecule, differently from the difluoro (-CHF 2 ) and trifluoro (-CF 3 ) counterparts, improves the electrolyte ionic conductivity without narrowing the oxidation stability. Indeed, the electrolyte solution with the monofluoride ether solvent demonstrates good compatibility with positive and negative electrodes in a wide range of temperatures (i.e., from −60 °C to +60 °C) and at high charge/discharge…

Materials with phototunable full-color circularly polarized luminescence (CPL) have a large storage density, high-security level, and enormous prospects in the field of information encryption and decryption. In this work, device-friendly solid films with color tunability are prepared by constructing Förster resonance energy transfer (FRET) platforms with chiral donors and achiral molecular switches in liquid crystal photonic capsules (LCPCs). These LCPCs exhibit photoswitchable CPL from initial blue emission to RGB trichromatic signals under UV irradiation due to the synergistic effect of energy and chirality transfer and show strong time dependence because of the different FRET efficiencies at each time node. Based on these phototunable CPL and time response characteristics, the concept of multilevel data encryption by using LCPC films is demonstrated.

Osteoarthritis affects millions of people worldwide but current treatments using analgesics or anti-inflammatory drugs only alleviate symptoms of this disease. Here, we present an injectable, biodegradable piezoelectric hydrogel, made of short electrospun poly-L-lactic acid nanofibers embedded inside a collagen matrix, which can be injected into the joints and self-produce localized electrical cues under ultrasound activation to drive cartilage healing. In vitro, data shows that the piezoelectric hydrogel with ultrasound can enhance cell migration and induce stem cells to secrete TGF-β1, which promotes chondrogenesis. In vivo, the rabbits with osteochondral critical-size defects receiving the ultrasound-activated piezoelectric hydrogel show increased subchondral bone formation, improved hyaline-cartilage structure, and good mechanical properties, close to healthy native cartilage. This piezoelectric hydrogel is not only useful for cartilage healing but also potentially applicable to other tissue regeneration, offering a significant impact on the field of regenerative tissue…

Abstract The emergence of parallel convolution-operation technology has substantially powered the complexity and functionality of optical neural networks (ONN) by harnessing the dimension of optical wavelength. However, this advanced architecture faces remarkable challenges in high-level integration and on-chip operation. In this work, convolution based on time-wavelength plane stretching approach is implemented on a microcomb-driven chip-based photonic processing unit (PPU). To support the operation of this processing unit, we develop a dedicated control and operation protocol, leading to a record high weight precision of 9 bits. Moreover, the compact architecture and high data loading speed enable a preeminent photonic-core compute density of over 1 trillion of operations per second per square millimeter (TOPS mm −2 ). Two proof-of-concept experiments are demonstrated, including image edge detection and handwritten digit recognition, showing comparable processing capability compared to that of a digital computer. Due to the advanced performance and the great scalability, this…

Abstract Ga 2 O 3 -based solar blind avalanche photodetectors exhibit low voltage operation, optical filter-free and monolithic integration of photodetector arrays, and therefore they are promising to be an alternative to the bulky and fragile photomultiplier tubes for weak signal detection in deep-ultraviolet region. Here, by deliberate lattice and band engineering, we construct an n-Barrier-n unipolar barrier avalanche photodetector consisting of β -Ga 2 O 3 /MgO/Nb:SrTiO 3 heterostructure, in which the enlarged conduction band offsets fortify the reverse breakdown and suppress the dark current while the negligible valance band offsets faciliate minority carrier flow across the heterojunction. The developed devices exhibit record-high avalanche gain up to 5.9 × 10 5 and detectivity of 2.33 × 10 16 Jones among the reported wafer-scale grown Ga 2 O 3 -based photodetectors, which are even comparable to the commercial photomultiplier tubes. These findings provide insights into precise manipulation of band alignment in avalanche photodetectors, and also offer exciting opportunities for…

Abstract Electrocatalytic urea synthesis is an emerging alternative technology to the traditional energy-intensive industrial urea synthesis protocol. Novel strategies are urgently needed to promote the electrocatalytic C–N coupling process and inhibit the side reactions. Here, we report a CuWO 4 catalyst with native bimetallic sites that achieves a high urea production rate (98.5 ± 3.2 μg h −1 mg −1 cat ) for the co-reduction of CO 2 and NO 3 − with a high Faradaic efficiency (70.1 ± 2.4%) at −0.2 V versus the reversible hydrogen electrode. Mechanistic studies demonstrated that the combination of stable intermediates of *NO 2 and *CO increases the probability of C–N coupling and reduces the potential barrier, resulting in high Faradaic efficiency and low overpotential. This study provides a new perspective on achieving efficient urea electrosynthesis by stabilizing the key reaction intermediates, which may guide the design of other electrochemical systems for high-value C–N bond-containing chemicals.

Abstract Stable operation of batteries at low temperatures is critical for applications in cold-climates; however, low-temperature operations are plagued by low ionic conductivity of electrolytes, slow interfacial kinetics and unstable solid–electrolyte interphases (SEIs). We report a polymer electrolyte with an ionic conductivity of 2.2⋅10− 4 S cm− 1 and an ionic transference number of 0.8 at − 20 °C; the electrolyte is synthesized by in-situ polymerizing 1,3,5-trioxane (TXE), 2-2-2-trifluoro-N, N-dimethylacetamide (FDMA), fluoroethylene carbonate (FEC) and lithium difluoro(oxalate)borate (LiDFOB). The polymer electrolyte enables a dual-layered SEI on the Li metal anode and strongly stabilizes the LiNi0.8Co0.1Mn0.1O2 cathode, thus defining fast interfacial charge-transfer at low temperatures. Consequently, the galvanic Li corrosion and the dendritic growth are suppressed, stable Li metal anode and LiNi0.8Co0.1Mn0.1O2 cathode are achieved, and the operation temperatures of polymer-based batteries are decreased to below − 30°C. From − 30°C to room temperature, the…

Effective reprogramming of chronic wound healing remains challenging due to the limited drug delivery efficacy hindered by physiological barriers, as well as the inappropriate dosing timing in distinct healing stages. Herein, a core-shell structured microneedle array patch with programmed functions (PF-MNs) is designed to dynamically modulate the wound immune microenvironment according to the varied healing phases. Specifically, PF-MNs combat multidrug-resistant bacterial biofilm at the early stage via generating reactive oxygen species (ROS) under laser irradiation. Subsequently, the ROS-sensitive MN shell gradually degrades to expose the MN core component, which neutralizes various inflammatory factors and promotes the phase transition from inflammation to proliferation. In addition, the released verteporfin inhibits scar formation by blocking Engrailed-1 (En1) activation in fibroblasts. Our experiments demonstrate that PF-MNs promote scarless wound repair in mouse models of both acute and chronic wounds, and inhibit the formation of hypertrophic scar in rabbit ear models.

Mapping tumor metabolic remodeling and their spatial crosstalk with surrounding non-tumor cells can fundamentally improve our understanding of tumor biology, facilitates the designing of advanced therapeutic strategies. Here, we present an integration of mass spectrometry imaging-based spatial metabolomics and lipidomics with microarray-based spatial transcriptomics to hierarchically visualize the intratumor metabolic heterogeneity and cell metabolic interactions in same gastric cancer sample. Tumor-associated metabolic reprogramming is imaged at metabolic-transcriptional levels, and maker metabolites, lipids, genes are connected in metabolic pathways and colocalized in the heterogeneous cancer tissues. Integrated data from spatial multi-omics approaches coherently identify cell types and distributions within the complex tumor microenvironment, and an immune cell-dominated "tumor-normal interface" region where tumor cells contact adjacent tissues are characterized with distinct transcriptional signatures and significant immunometabolic alterations. Our approach for mapping tissue…

Abstract Cobalt coordinated covalent organic frameworks have attracted increasing interest in the field of CO 2 photoreduction to CO, owing to their high electron affinity and predesigned structures. However, achieving high conversion efficiency is challenging since most Co related coordination environments facilitate fast recombination of photogenerated electron-hole pairs. Here, we design two kinds of Co-COF catalysts with oxygen coordinated Co atoms and find that after tuning of coordination environment, the reported Co framework catalyst with Co-O 4 sites exhibits a high CO production rate of 18000 µmol g −1 h −1 with selectivity as high as 95.7% under visible light irradiation. From in/ex-situ spectral characterizations and theoretical calculations, it is revealed that the predesigned Co-O 4 sites significantly facilitate the carrier migration in framework matrixes and inhibit the recombination of photogenerated electron-hole pairs in the photocatalytic process. This work opens a way for the design of high-performance catalysts for CO 2 photoreduction.

Factors driving microbial community composition and diversity are well established but the relationship with microbial functioning is poorly understood, especially at large scales. We analysed microbial biodiversity metrics and distribution of potential functional groups along a gradient of increasing land-use perturbation, detecting over 79,000 bacterial and 25,000 fungal OTUs in 715 sites across 24 European countries. We found the lowest bacterial and fungal diversity in less-disturbed environments (woodlands) compared to grasslands and highly-disturbed environments (croplands). Highly-disturbed environments contain significantly more bacterial chemoheterotrophs, harbour a higher proportion of fungal plant pathogens and saprotrophs, and have less beneficial fungal plant symbionts compared to woodlands and extensively-managed grasslands. Spatial patterns of microbial communities and predicted functions are best explained when interactions among the major determinants (vegetation cover, climate, soil properties) are considered. We propose guidelines for environmental policy actions…

In late 2022, SARS-CoV-2 Omicron subvariants have become highly diversified, and XBB is spreading rapidly around the world. Our phylogenetic analyses suggested that XBB emerged through the recombination of two cocirculating BA.2 lineages, BJ.1 and BM.1.1.1 (a progeny of BA.2.75), during the summer of 2022. XBB.1 is the variant most profoundly resistant to BA.2/5 breakthrough infection sera to date and is more fusogenic than BA.2.75. The recombination breakpoint is located in the receptor-binding domain of spike, and each region of the recombinant spike confers immune evasion and increases fusogenicity. We further provide the structural basis for the interaction between XBB.1 spike and human ACE2. Finally, the intrinsic pathogenicity of XBB.1 in male hamsters is comparable to or even lower than that of BA.2.75. Our multiscale investigation provides evidence suggesting that XBB is the first observed SARS-CoV-2 variant to increase its fitness through recombination rather than substitutions.

Proposals for achieving net-zero emissions by 2050 include scaling-up electrolytic hydrogen production, however, this poses technical, economic, and environmental challenges. One such challenge is for policymakers to ensure a sustainable future for the environment including freshwater and land resources while facilitating low-carbon hydrogen production using renewable wind and solar energy. We establish a country-by-country reference scenario for hydrogen demand in 2050 and compare it with land and water availability. Our analysis highlights countries that will be constrained by domestic natural resources to achieve electrolytic hydrogen self-sufficiency in a net-zero target. Depending on land allocation for the installation of solar panels or wind turbines, less than 50% of hydrogen demand in 2050 could be met through a local production without land or water scarcity. Our findings identify potential importers and exporters of hydrogen or, conversely, exporters or importers of industries that would rely on electrolytic hydrogen. The abundance of land and water resources in Southern…

Abstract Dynamic reconstruction of metal sulphides during electrocatalytic oxygen evolution reaction (OER) has hampered the acquisition of legible evidence for comprehensively understanding the phase-transition mechanism and electrocatalytic activity origin. Herein, modelling on a series of cobalt-nickel bimetallic sulphides, we for the first time establish an explicit and comprehensive picture of their dynamic phase evaluation pathway at the pre-catalytic stage before OER process. By utilizing the in-situ electrochemical transmission electron microscopy and electron energy loss spectroscopy, the lattice sulphur atoms of (NiCo)S1.33particles are revealed to be partially substituted by oxygen from electrolyte to form a lattice oxygen-sulphur coexisting shell surface before the generation of reconstituted active species. Such S-O exchange process is benefitted from the subtle modulation of metal-sulphur coordination form caused by the specific Ni and Co occupation. This unique oxygen-substitution behaviour produces an (NiCo)OxS1.33-xsurface to reduce the energy barrier of surface…

Ulcerative colitis and Crohn's disease are chronic inflammatory intestinal diseases with perplexing heterogeneity in disease manifestation and response to treatment. While the molecular basis for this heterogeneity remains uncharacterized, single-cell technologies allow us to explore the transcriptional states within tissues at an unprecedented resolution which could further understanding of these complex diseases. Here, we apply single-cell RNA-sequencing to human inflamed intestine and show that the largest differences among patients are present within the myeloid compartment including macrophages and neutrophils. Using spatial transcriptomics in human tissue at single-cell resolution (CosMx Spatial Molecular Imaging) we spatially localize each of the macrophage and neutrophil subsets identified by single-cell RNA-sequencing and unravel further macrophage diversity based on their tissue localization. Finally, single-cell RNA-sequencing combined with single-cell spatial analysis reveals a strong communication network involving macrophages and inflammatory fibroblasts. Our data…

Even though the perovskite solar cell has been so popular for its skyrocketing power conversion efficiency, its further development is still roadblocked by its overall performance, in particular long-term stability, large-area fabrication and stable module efficiency. In essence, the soft component and ionic-electronic nature of metal halide perovskites usually chaperonage large number of anion vacancy defects that act as recombination centers to decrease both the photovoltaic efficiency and operational stability. Herein, we report a one-stone-for-two-birds strategy in which both anion-fixation and associated undercoordinated-Pb passivation are in situ achieved during crystallization by using a single amidino-based ligand, namely 3-amidinopyridine, for metal-halide perovskite to overcome above challenges. The resultant devices attain a power conversion efficiency as high as 25.3% (certified at 24.8%) with substantially improved stability. Moreover, the device without encapsulation retained 92% of its initial efficiency after 5000 h exposure in ambient and the device with…

Abstract The development of Zn-free anodes to inhibit Zn dendrite formation and modulate high-capacity Zn batteries is highly applauded yet very challenging. Here, we design a robust two-dimensional antimony/antimony-zinc alloy heterostructured interface to regulate Zn plating. Benefiting from the stronger adsorption and homogeneous electric field distribution of the Sb/Sb 2 Zn 3 -heterostructured interface in Zn plating, the Zn anode enables an ultrahigh areal capacity of 200 mAh cm −2 with an overpotential of 112 mV and a Coulombic efficiency of 98.5%. An anode-free Zn-Br 2 battery using the Sb/Sb 2 Zn 3 -heterostructured interface@Cu anode shows an attractive energy density of 274 Wh kg −1 with a practical pouch cell energy density of 62 Wh kg −1 . The scaled-up Zn-Br 2 battery in a capacity of 500 mAh exhibits over 400 stable cycles. Further, the Zn-Br 2 battery module in an energy of 9 Wh (6 V, 1.5 Ah) is integrated with a photovoltaic panel to demonstrate the practical renewable energy storage capabilities. Our superior anode-free Zn batteries enabled by the heterostructured…

T cell exhaustion is a hallmark of cancer and persistent infections, marked by inhibitory receptor upregulation, diminished cytokine secretion, and impaired cytolytic activity. Terminally exhausted T cells are steadily replenished by a precursor population (Tpex), but the metabolic principles governing Tpex maintenance and the regulatory circuits that control their exhaustion remain incompletely understood. Using a combination of gene-deficient mice, single-cell transcriptomics, and metabolomic analyses, we show that mitochondrial insufficiency is a cell-intrinsic trigger that initiates the functional exhaustion of T cells. At the molecular level, we find that mitochondrial dysfunction causes redox stress, which inhibits the proteasomal degradation of hypoxia-inducible factor 1α (HIF-1α) and promotes the transcriptional and metabolic reprogramming of Tpex cells into terminally exhausted T cells. Our findings also bear clinical significance, as metabolic engineering of chimeric antigen receptor (CAR) T cells is a promising strategy to enhance the stemness and functionality of Tpex…

Abstract Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of nitrate reduction under acidic conditions is rarely reported. In this work, we demonstrate the potential of TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity for selective and rapid nitrate reduction to ammonia under acidic conditions. Hybridized with iron phthalocyanine, the resulting catalyst displays remarkably improved efficiency toward ammonia formation owing to the enhanced nitrate adsorption, suppressed hydrogen evolution and lowered energy barrier for the rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed with high open-circuit voltage of 1.99 V and power density of 91.4 mW cm –2 . Further, the environmental sulfur recovery can be powered by above hybrid battery and the hydrazine-nitrate fuel cell can be developed for simultaneously hydrazine/nitrate conversion and electricity generation. This work demonstrates the attractive potential of acidic nitrate…

The spatial organization of the tumor microenvironment has a profound impact on biology and therapy response. Here, we perform an integrative single-cell and spatial transcriptomic analysis on HPV-negative oral squamous cell carcinoma (OSCC) to comprehensively characterize malignant cells in tumor core (TC) and leading edge (LE) transcriptional architectures. We show that the TC and LE are characterized by unique transcriptional profiles, neighboring cellular compositions, and ligand-receptor interactions. We demonstrate that the gene expression profile associated with the LE is conserved across different cancers while the TC is tissue specific, highlighting common mechanisms underlying tumor progression and invasion. Additionally, we find our LE gene signature is associated with worse clinical outcomes while TC gene signature is associated with improved prognosis across multiple cancer types. Finally, using an in silico modeling approach, we describe spatially-regulated patterns of cell development in OSCC that are predictably associated with drug response. Our work provides…

A comprehensive quantification of global forest fragmentation is urgently required to guide forest protection, restoration and reforestation policies. Previous efforts focused on the static distribution patterns of forest remnants, potentially neglecting dynamic changes in forest landscapes. Here, we map global distribution of forest fragments and their temporal changes between 2000 and 2020. We find that forest landscapes in the tropics were relatively intact, yet these areas experienced the most severe fragmentation over the past two decades. In contrast, 75.1% of the world's forests experienced a decrease in fragmentation, and forest fragmentation in most fragmented temperate and subtropical regions, mainly in northern Eurasia and South China, declined between 2000 and 2020. We also identify eight modes of fragmentation that indicate different recovery or degradation states. Our findings underscore the need to curb deforestation and increase connectivity among forest fragments, especially in tropical areas.

Glacial lake outburst floods (GLOFs) represent a major hazard and can result in significant loss of life. Globally, since 1990, the number and size of glacial lakes has grown rapidly along with downstream population, while socio-economic vulnerability has decreased. Nevertheless, contemporary exposure and vulnerability to GLOFs at the global scale has never been quantified. Here we show that 15 million people globally are exposed to impacts from potential GLOFs. Populations in High Mountains Asia (HMA) are the most exposed and on average live closest to glacial lakes with ~1 million people living within 10 km of a glacial lake. More than half of the globally exposed population are found in just four countries: India, Pakistan, Peru, and China. While HMA has the highest potential for GLOF impacts, we highlight the Andes as a region of concern, with similar potential for GLOF impacts to HMA but comparatively few published research studies.

Antibodies have the capacity to bind a diverse set of antigens, and they have become critical therapeutics and diagnostic molecules. The binding of antibodies is facilitated by a set of six hypervariable loops that are diversified through genetic recombination and mutation. Even with recent advances, accurate structural prediction of these loops remains a challenge. Here, we present IgFold, a fast deep learning method for antibody structure prediction. IgFold consists of a pre-trained language model trained on 558 million natural antibody sequences followed by graph networks that directly predict backbone atom coordinates. IgFold predicts structures of similar or better quality than alternative methods (including AlphaFold) in significantly less time (under 25 s). Accurate structure prediction on this timescale makes possible avenues of investigation that were previously infeasible. As a demonstration of IgFold's capabilities, we predicted structures for 1.4 million paired antibody sequences, providing structural insights to 500-fold more antibodies than have experimentally…

Abstract One of unsolved puzzles about water lies in how ion-water interplay affects its freezing point. Here, we report the direct link between tetrahedral entropy and the freezing behavior of water in Zn 2+ -based electrolytes by analyzing experimental spectra and molecular simulation results. A higher tetrahedral entropy leads to lower freezing point, and the freezing temperature is directly related to the entropy value. By tailoring the entropy of water using different anions, we develop an ultralow temperature aqueous polyaniline| |Zn battery that exhibits a high capacity (74.17 mAh g −1 ) at 1 A g −1 and −80 °C with ~85% capacity retention after 1200 cycles due to the high electrolyte ionic conductivity (1.12 mS cm −1 ). Moreover, an improved cycling life is achieved with ~100% capacity retention after 5000 cycles at −70 °C. The fabricated battery delivers appreciably enhanced performance in terms of frost resistance and stability. This work serves to provide guidance for the design of ultralow temperature aqueous batteries by precisely tuning the water structure within…

Abstract Electrochemical coupling of biomass valorization with carbon dioxide (CO 2 ) conversion provides a promising approach to generate value-added chemicals on both sides of the electrolyzer. Herein, oxygen-vacancy-rich indium oxyhydroxide (InOOH-O V ) is developed as a bifunctional catalyst for CO 2 reduction to formate and 5-hydroxymethylfurfural electrooxidation to 2,5-furandicarboxylic acid with faradaic efficiencies for both over 90.0% at optimized potentials. Atomic-scale electron microscopy images and density functional theory calculations reveal that the introduction of oxygen vacancy sites causes lattice distortion and charge redistribution. Operando Raman spectra indicate oxygen vacancies could protect the InOOH-O V from being further reduced during CO 2 conversion and increase the adsorption competitiveness for 5-hydroxymethylfurfural over hydroxide ions in alkaline electrolytes, making InOOH-O V a main-group p-block metal oxide electrocatalyst with bifunctional activities. Based on the catalytic performance of InOOH-O V , a pH-asymmetric integrated cell is fabricated…

Abstract Catalysts capable of electrochemical overall water splitting in acidic, neutral, and alkaline solution are important materials. This work develops bifunctional catalysts with single atom active sites through a pyrolysis-free route. Starting with a conjugated framework containing Fe sites, the addition of Ni atoms is used to weaken the adsorption of electrochemically generated intermediates, thus leading to more optimized energy level sand enhanced catalytic performance. The pyrolysis-free synthesis also ensured the formation of well-defined active sites within the framework structure, providing ideal platforms to understand the catalytic processes. The as-prepared catalyst exhibits efficient catalytic capability for electrochemical water splitting in both acidic and alkaline electrolytes. At a current density of 10 mA cm −2 , the overpotential for hydrogen evolution and oxygen evolution is 23/201 mV and 42/194 mV in 0.5 M H 2 SO 4 and 1 M KOH, respectively. Our work not only develops a route towards efficient catalysts applicable across a wide range of pH values, it also…

Abstract Electrocatalytic hydrogen peroxide (H 2 O 2 ) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H 2 O 2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e − oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H 2 O 2 production. Consequently, the H 2 O 2 yield approaches 30 mol g −1 h −1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H 2 O 2 concentration of 7.2 g L −1 . This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy…

While marine kelp forests have provided valuable ecosystem services for millennia, the global ecological and economic value of those services is largely unresolved. Kelp forests are diminishing in many regions worldwide, and efforts to manage these ecosystems are hindered without accurate estimates of the value of the services that kelp forests provide to human societies. Here, we present a global estimate of the ecological and economic potential of three key ecosystem services - fisheries production, nutrient cycling, and carbon removal provided by six major forest forming kelp genera (Ecklonia, Laminaria, Lessonia, Macrocystis, Nereocystis, and Saccharina). Each of these genera creates a potential value of between $64,400 and $147,100/hectare each year. Collectively, they generate between $465 and $562 billion/year worldwide, with an average of $500 billion. These values are primarily driven by fisheries production (mean $29,900, 904 Kg/Ha/year) and nitrogen removal ($73,800, 657 Kg N/Ha/year), though kelp forests are also estimated to sequester 4.91 megatons of carbon from the…

Quantifying the resilience of vegetated ecosystems is key to constraining both present-day and future global impacts of anthropogenic climate change. Here we apply both empirical and theoretical resilience metrics to remotely-sensed vegetation data in order to examine the role of water availability and variability in controlling vegetation resilience at the global scale. We find a concise global relationship where vegetation resilience is greater in regions with higher water availability. We also reveal that resilience is lower in regions with more pronounced inter-annual precipitation variability, but find less concise relationships between vegetation resilience and intra-annual precipitation variability. Our results thus imply that the resilience of vegetation responds differently to water deficits at varying time scales. In view of projected increases in precipitation variability, our findings highlight the risk of ecosystem degradation under ongoing climate change.

Abstract Designing electrochemically active, stable, and earth-abundant electrocatalysts is essential for boosting oxygen evolution reaction (OER) rates for sustainable hydrogen production. High entropy oxides (HEOs) consist of five or more metal cations, offering ample opportunities to tune their catalytic properties toward high OER efficiency. In this work, we combine theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Our density functional theory calculations unequivocally confirm that randomly mixed metal sites are more thermodynamically stable, while we also show that adsorption energies of the intermediates display widening distributions accompanied by the equatorial strain of active metal-oxygen bonds under mixing. The rapid sol-flame method was successfully employed to synthesize spinel oxides up to five third-row metal cations (Co, Fe, Ni, Cr, and Mn) with high degree of entropy. Such catalyst exhibits the highest OER activity of 309 mV at 10 mA cm− 2 and prolonged durability up to 168 hours under alkaline conditions over…

Abstract High entropy oxides (HEOs) with chemically disordered multi-cation structure attract intensive interest as negative electrode materials for battery applications. The outstanding electrochemical performance has been attributed to the high-entropy stabilization and the so-called ‘cocktail effect’. However, the configurational entropy of the HEO, which is thermodynamically only metastable at room-temperature, is insufficient to drive the structural reversibility during conversion-type battery reaction, and the ‘cocktail effect’ has not been explained thus far. This work unveils the multi-cations synergy of the HEO Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 O at atomic and nanoscale during electrochemical reaction and explains the ‘cocktail effect’. The more electronegative elements form an electrochemically inert 3-dimensional metallic nano-network enabling electron transport. The electrochemical inactive cation stabilizes an oxide nanophase, which is semi-coherent with the metallic phase and accommodates Li + ions. This self-assembled nanostructure enables stable cycling of…

Abstract The detrimental parasitic reactions and uncontrolled deposition behavior derived from inherently unstable interface have largely impeded the practical application of aqueous zinc batteries. So far, tremendous efforts have been devoted to tailoring interfaces, while stabilization of grain boundaries has received less attention. Here, we demonstrate that preferential distribution of intermetallic compounds at grain boundaries via an alloying strategy can substantially suppress intergranular corrosion. In-depth morphology analysis reveals their thermodynamic stability, ensuring sustainable potency. Furthermore, the hybrid nucleation and growth mode resulting from reduced Gibbs free energy contributes to the spatially uniform distribution of Zn nuclei, promoting the dense Zn deposition. These integrated merits enable a high Zn reversibility of 99.85% for over 4000 cycles, steady charge-discharge at 10 mA cm−2, and impressive cyclability for roughly 3500 cycles in Zn-Ti//NH4V4O10 full cell. Notably, the multi-layer pouch cell of 34 mAh maintains stable cycling for 500 cycles.…

Abstract The current lithium-ion battery (LIB) electrode fabrication process relies heavily on the wet coating process, which uses the environmentally harmful and toxic N-methyl-2-pyrrolidone (NMP) solvent. In addition to being unsustainable, the use of this expensive organic solvent substantially increases the cost of battery production, as it needs to be dried and recycled throughout the manufacturing process. Herein, we report an industrially viable and sustainable dry press-coating process that uses the combination of multiwalled carbon nanotubes (MWNTs) and polyvinylidene fluoride (PVDF) as a dry powder composite and etched Al foil as a current collector. Notably, the mechanical strength and performance of the fabricated LiNi 0.7 Co 0.1 Mn 0.2 O 2 (NCM712) dry press-coated electrodes (DPCEs) far exceed those of conventional slurry-coated electrodes (SCEs) and give rise to high loading (100 mg cm −2 , 17.6 mAh cm −2 ) with impressive specific energy and volumetric energy density of 360 Wh kg −1 and 701 Wh L −1 , respectively.

Abstract Direct hydrogen peroxide (H 2 O 2 ) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to the traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain to be challenging, partially due to insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches to identify transition-metal single-site catalysts for two-electron oxygen reduction using the *OOH binding energy as a descriptor. The theoretical predictions are then used as guidance to synthesize the desired cobalt single-site catalyst with a O-modified Co-(pyrrolic N) 4 configuration that can achieve industrial-relevant current densities up to 300 mA cm − 2 with 96–100% Faradaic efficiencies for H 2 O 2 production at a record rate of 11,527 mmol h − 1 g cat − 1 . Here, we show the feasibility and versatility of metal single-site catalyst design using various commercial carbon and cobalt phthalocyanine as starting materials and the high…