Combining the phase-field method and the moving boundary method,a three-dimensional phase-field simulation was conducted for the growth and grain evolution of Ti films deposited by physical vapor deposition under diff...Combining the phase-field method and the moving boundary method,a three-dimensional phase-field simulation was conducted for the growth and grain evolution of Ti films deposited by physical vapor deposition under different deposition rates and grain orientations.The evolution of grain morphology and grain orientation was also taken into consideration.Simulation results show that at lower deposition rates,the surface of the formed Ti film exhibits a distinct oriented texture structure.The surface roughness of the Ti film is positively correlated with the grain misorientation.Moreover,the surface roughness obtained from the simulation is in good agreement with the experiment results.展开更多
While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an an...While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an analysis framework(expression variance decomposition,EVaDe)for comparative single-cell expression data based on phenotypic evolution theory.After decomposing the gene expression variance into separate components,we use two strategies to identify genes exhibiting large between-taxon expression divergence and small within-cell-type expression noise in certain cell types,attributing this pattern to putative adaptive evolution.In a dataset of primate prefrontal cortex,we find that such humanspecific key genes enrich with neurodevelopment-related functions,while most other genes exhibit neutral evolution patterns.Specific neuron types are found to harbor more of these key genes than other cell types,thus likely to have experienced more extensive adaptation.Reassuringly,at the molecular sequence level,the key genes are significantly associated with the rapidly evolving conserved non-coding elements.An additional case analysis comparing the naked mole-rat(NMR)with the mouse suggests that innateimmunity-related genes and cell types have undergone putative expression adaptation in NMR.Overall,the EVaDe framework may effectively probe adaptive evolution mode in single-cell expression data.展开更多
Gibbons are small,arboreal apes that play a critical role in tropical biodiversity and ecosystem ecology.However,nearly all species of gibbons are threatened by habitat loss,illegal trade,hunting,and other human activ...Gibbons are small,arboreal apes that play a critical role in tropical biodiversity and ecosystem ecology.However,nearly all species of gibbons are threatened by habitat loss,illegal trade,hunting,and other human activities.Long-term poor understanding of their genetics and evolution undermines effective conservation efforts.In this study,we analyse comparative population genomic data of four Nomascus species.Our results reveal strong genetic differentiation and gene flow among Nomascus species.Additionally,we identify genomic features that are potentially related to natural selection linked to vocalization,fructose metabolism,motor balance,and body size,consistent with the unique phenotype and adaptability of gibbons.Inbreeding,coupled with population declines due to climate change and historical human activities,leads to reduced genetic diversity and the accumulation of deleterious variations that likely affect cardiovascular disease and the reproductive potential of gibbons and further reduce their fitness,highlighting the urgent need for effective conservation strategies.展开更多
To realize the practical application of anion exchange membrane water electrolysis(AEMWE),it is essential to develop highly active,durable,and cost-effective electrocatalyst for oxygen evolution reaction(OER).Herein,w...To realize the practical application of anion exchange membrane water electrolysis(AEMWE),it is essential to develop highly active,durable,and cost-effective electrocatalyst for oxygen evolution reaction(OER).Herein,we report a hollow-structured Ni_(x)Co_(1−x)O/Ni_(3)S_(2)/Co_(9)S_(8)heterostructure synthesized via sequential template-assisted growth,thermal oxidation,and controlled sulfidation process.The abundant bimetallic heterointerfaces not only provide additional active sites but also promote electronic modulation via charge redistribution.Additionally,the porous and hollow architecture enhances active surface area and mass transfer ability,thereby increasing the number of accessible active sites for alkaline OER.As a result,the prepared electrocatalyst achieves low overpotential of 310 mV at 10 mA cm^(−2)and small Tafel slope of 55.94 mV dec^(−1),demonstrating the exceptional electrocatalytic performance for alkaline OER.When integrated as the anode in an AEMWE cell,it delivers outstanding performance with only 1.657 V at 1.0 A cm^(−2)and reaches high current density of 5.0 A cm^(−2)at 1.989 V,surpassing those of commercial RuO_(2).The cell also shows excellent long-term durability over 100 h with minimal degradation.This study highlights the strong potential of rationally engineered oxide/sulfide heterostructures for next-generation alkaline water electrolysis.展开更多
To reveal the influence of coupled effects of dry-wet cycling and precompression stress(CEDWCPS)on the damage evolution of limestone with horizontal fissure(LHF),a series of degradation and uniaxial compression tests ...To reveal the influence of coupled effects of dry-wet cycling and precompression stress(CEDWCPS)on the damage evolution of limestone with horizontal fissure(LHF),a series of degradation and uniaxial compression tests were conducted,and a corresponding piecewise damage constitutive model(PDCM)was established.We found that both dry-wet cycling and precompression stress deteriorate the physical properties,alter the microscopic characteristics,and reduce the mechanical properties of the LHF.These degradations are particularly pronounced under the CEDWCPS,although the magnitude of these changes gradually diminishes with the progression of dry-wet cycling.Meanwhile,they also reduce the deformation degree,prolong the micropore compaction stage,shorten the unstable crack propagation stage,lower the frequency and intensity of AE events,decrease the high-amplitude and high-frequency AE signals,enlarge crack scales,and shorten the crack initiation time.Among the changes of these indicators,the dry-wet cycling plays a dominant role.The crack types of LHF under the CEDWCPS(LHFCEDWCPS)are predominantly tensile cracks,supplemented by shear cracks.The failure mode can be defined as tensileshear composite failure.Finally,the established PDCM effectively captures the nonlinear deformation of micropore and the linear deformation of the matrix in LHFCEDWCPS,with all corresponding R^(2) consistently exceeding 0.97.展开更多
Understanding the evolution and mechanisms of livestock industry agglomeration provides valuable policy insights for reconciling growing meat demand with constrained resource endowments. This study analyzes the spatia...Understanding the evolution and mechanisms of livestock industry agglomeration provides valuable policy insights for reconciling growing meat demand with constrained resource endowments. This study analyzes the spatial agglomeration of livestock industry at the county level across China from 2000 to 2022 using the localization quotient and Moran's I. An interpretable machine learning approach is employed to test hypotheses concerning the driving mechanisms underlying the spatial distribution of livestock industry. The results show that the agglomeration of China's livestock industry is intensifying, with the agro-pastoral transitional zone(APTZ) emerging as a prominent agglomeration area and distinct agglomeration patterns observed within the zone as well as in its eastern and western regions. Proximity to markets has become an increasingly important determinant of livestock industry agglomeration in China. This market-driven shift has heightened the demand for agricultural feed, prompting the livestock industry to relax its dependence on local natural resource endowments and gradually relocate eastward. Regionally, the agglomeration within the APTZ is shaped by the joint effects of natural and social factors. Natural factors dominate agglomeration dynamics in the western regions of the zone, whereas social factors are more influential in its eastern regions.展开更多
The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate...The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate evolution mechanism(AEM),lattice oxygen mechanism(LOM),and oxide path mechanism(OPM).Compared to AEM,limited by scaling relationships,and LOM,constrained by stability issues,the OPM offers a promising alternative by enabling direct O-O bond formation via dual active sites,thus bypassing^(*)OOH intermediates and lattice O involvement and achieving a balance between activity and durability.However,activating the OPM process requires precise control over the spatial and electronic structure of active sites,making the design of OPM-based catalysts challenging.While previous reviews have focused on homo/heteronuclear diatomic perspectives of OPM-based catalysts,it is urgent to systematically summarize design strategies to provide a rational reference for their development.Herein,a review of design strategies for OPM-based OER catalysts across three scales is comprehensively presented,including in-situ engineering,doping-enabled sites reconstruction,and introducing new sites for nanoparticles,direct synthesis or post-treatments for molecular catalysts,and doping or template strategies for atom pairs or arrays.The unique advantage of atom arrays is also highlighted,and their future research directions and possible strategies are discussed.This review provides a systematic summary and forward-looking perspectives for rationally designing high-performance OPM-based OER catalysts.展开更多
The shale gas development in China faces challenges such as complex reservoir conditions and high development costs.Based on the pore pressure and geostress coupling theory,this paper studies the geostress evolution l...The shale gas development in China faces challenges such as complex reservoir conditions and high development costs.Based on the pore pressure and geostress coupling theory,this paper studies the geostress evolution laws and fracture network characteristics of shale gas infill wells.A mechanism model of CN platform logging data and geomechanical parameters is established to simulate the influence of parent well’s production on the geostress in the infill well area.It is suggested that with the increase of production time,normal fault stress state and horizontal stress deflection will occur.The smaller the parent well spacing and the longer the production time,the earlier the normal fault stress state appears and the larger the range.Based on the model,the fracture network morphology and construction parameters of infill wells are optimized.parentparentparentparent The results indicate that:1:A well spacing of 500 m achieves a Pareto optimum between“full reserve coverage”and“stress barrier”;2:A parent well recovery degree of 30%corresponds to the critical point of stress reversal,where the lateral deflection rate of the infill fracture is less than 8%and the SRV loss is minimized;3:6-cluster intensive completion with twice the liquid intensity increases the fracture complexity index by 1.7 times,enhances well group EUR by 15.4%,and reduces single-well cost by 22%.This research fills the theoretical gap in the collaborative optimization of“multi-parameter,multi-objective and multi-constraint”and provide parameter optimization basis for shale gas infill well development in China and help to improve the development efficiency and economic benefits.展开更多
We report for the first time the combination of directed evolution focused on enhancing and reversing the stereoselectivity of an enzyme with Cu(I)-mediated click chemistry(CuAAC),providing an asymmetric click approac...We report for the first time the combination of directed evolution focused on enhancing and reversing the stereoselectivity of an enzyme with Cu(I)-mediated click chemistry(CuAAC),providing an asymmetric click approach for versatile chiral triazoles products.In this study,the halohydrin dehalogenase HheG was used as the enzyme which was evolved to induce a stereoselective ring-opening reaction of cyclic epoxides in the presence of NaN3 with the formation of chiral azido products.Two mutants of opposite stereopreference were generated,which convert cyclohexene oxide as well as cycloheptene oxide to(1S,2S)-2-azidocyclohexanol,(1R,2R)-2-azidocyclohexanol,(1S,2S)-2-azidocycloheptanol and(1R,2R)-2-azidocycloheptanol with essentially high stereoselectivity.The chiral products were then subjected to CuAAC in reactions with structurally different alkynes.Since HheG was found to be compatible with Cu(I),the process was also performed successfully in a unique 2-step one-pot process leading to various chiral triazoles.In order to understand the enhancement and reversal of the evolved enantioselectivity,QM and MD computations were performed.This approach harnesses the modifiability and high stereoselectivity of the evolved biocatalysts in combination with click chemistry.It holds great potential for diverse fields,particularly in the area of pharmaceuticals.展开更多
The advancement of effective and stable non-precious metal-based catalysts for oxygen evolution reactions(OER)with a lowcost and simple technique is essential for the practical application of rechargeable zinc–air ba...The advancement of effective and stable non-precious metal-based catalysts for oxygen evolution reactions(OER)with a lowcost and simple technique is essential for the practical application of rechargeable zinc–air battery(ZAB).However,facilitating the deep reconstruction of electrocatalysts to form active species remains a significant challenge.Here,a simple two-step method composed of impregnation and carbonization process is proposed to synthesize N,S co-doped microcrystalline cellulose-derived carbon-supported nickel sulfide(Ni_(3)S_(2))nanoparticles.The in situ Raman reveals that Fe substitution promotes the reconstruction of Ni_(3)S_(2),accompanied by the cleavage of the Ni–S bond,leading to the deep reconstruction into(Ni,Fe)OOH(DR-(Ni,Fe)OOH)during the OER.Moreover,density functional theory calculations reveal that Fe substitution induces a downshift in the energy band structure,which lowers the energy barriers and thereby improves the kinetics of the OER.The generated DR-(Ni,Fe)OOH delivers a relatively low overpotential of 260 m V and superior durability for 50 h under OER condition.The ZAB incorporating DR-(Ni,Fe)OOH+Pt/C as the air cathode demonstrates superior efficiency and durability,achieving a peak power density of 188.3 m W cm^(-2),a specific capacity of 811.1 m Ah g^(-1),and long-term stability exceeding 200 h.展开更多
To clarify the thermal evolution characteristics of organic matter in the ZizhongWeiyuan area in Sichuan Basin,solid bitumen reflectance of the Lower Cambrian Qiongzhusi Formation(QFm)shale was measured by Raman Spect...To clarify the thermal evolution characteristics of organic matter in the ZizhongWeiyuan area in Sichuan Basin,solid bitumen reflectance of the Lower Cambrian Qiongzhusi Formation(QFm)shale was measured by Raman Spectroscopy(RS)method.Constrained by vitrinite reflectance(Ro)data,burial and thermal evolution histories of QFm shale were reconstructed through basin numerical simulation technology.The evolution model of and critical period of organic matter was determined,and its dominant drivers were analyzed.The results show that the asphalt Raman vitrinite reflectance(_(Rmc)Ro)ranges from 3.21%to 4.15%.Thermal maturity within the trough follows a southern part>central part>northern part trend.Thermal maturity is moderate within the paleo-uplift,whereas organic matter outside the paleo-uplift has undergone graphitization.Two types of thermal evolution imprints were established:a continuous heating type and a stop heating type of Silurian–Permian.Sedimentary burial,paleogeomorphology,tectonic movement and Emeishan mantle plume are the dominant drivers of multi-stage thermal imprints of the QFm shale.The three factors are coupled with each other.The Late Caledonian and Late Indosinian are the key periods of organic matter thermal evolution.The Leshan-Longnüsi paleo-uplift weakens the thermal effect of the Permian Emeishan mantle plume.The current thermal evolution pattern of the QFm is mainly determined by the continuous subsidence of the Triassic–Cretaceous.Stop heating model of Silurian–Permian locks the maturity of organic matter in the gold window,thus controlling the enrichment of QFm shale gas.It provides new insights for shale gas migration,enrichment and effective exploration and development of shale gas in the Lower Paleozoic QFm.展开更多
Prediction of permeability changes in surrounding rock induced by engineering disturbances is crucial for mitigating tunnel water inrush accidents.This study investigates the progressive failure characteristics and pe...Prediction of permeability changes in surrounding rock induced by engineering disturbances is crucial for mitigating tunnel water inrush accidents.This study investigates the progressive failure characteristics and permeability evolution of hard and soft rocks subjected to triaxial compression.A series of laboratory tests were conducted at confining pressures ranging from 4 to 20 MPa.Experimental results demonstrate that rock permeability variation with strain shows three distinct stages:an initial decrease,a stage of rapid mutation,and a postpeak increase.The concept of critical permeability barrier strength is introduced,representing the stress level at which continuous fracture formation enables significant seepage.Furthermore,two generalized permeability–stress models are developed for soft and hard rocks.The predicted permeability values obtained from these models align well with the experimental data.These findings offer valuable insights into the hydro-mechanical coupling behavior of rocks,providing a foundation for safe construction practices in underground engineering.展开更多
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
Regulating the microenvironment of the support enables precise control of electronic metal-support interactions(EMSI),boosting better catalytic activity of the metal species.However,the fundamental relationship betwee...Regulating the microenvironment of the support enables precise control of electronic metal-support interactions(EMSI),boosting better catalytic activity of the metal species.However,the fundamental relationship between support defect-induced EMSI modulation and the resulting catalytic performance enhancement still needs further elucidation.Herein,a nonequilibrium high-temperature shock(HTS)method,which combines rapid high-temperature heating at 1273 K for 30 s with liquid nitrogen quenching,was adopted to load uniform Pt nanoparticles onto the nitrogen vacancy-rich TiN support(Pt@TiNVN).The catalyst demonstrates a high mass activity of 15.99 A mgPt^(-1)at an overpotential of 100 mV for the hydrogen evolution reaction(HER)in acidic solution and exhibits long-term stability for 60 h at 200 mA cm^(-2).Detailed spectroscopic characterizations and theoretical calculations reveal that the generated nitrogen vacancies can effectively modulate the charge transfer between Pt nanoparticles and the TiN-VN support,leading to a downshifted d-band center of metallic Pt and optimized Pt-H bond strength.This nonequilibrium HTS approach offers new and valuable insights into designing advanced electrocatalysts by harnessing substrate defects to modulate the electronic states of loaded noble metals.展开更多
Water electrolysis is pivotal for converting renewable energy into clean hydrogen fuel,addressing global energy demand sustainably.However,the development of highly efficient and cost-effective catalysts for the oxyge...Water electrolysis is pivotal for converting renewable energy into clean hydrogen fuel,addressing global energy demand sustainably.However,the development of highly efficient and cost-effective catalysts for the oxygen evolution reaction(OER)remains a significant challenge,particularly at the industrial scale.This report explores a newly discovered pathway,the oxide path mechanism(OPM) for OER-mechanism involving the oxide formation and evolution during the reaction,emphasizing its potential to overcome existing limitations.OPM enables direct O-O coupling without oxygen vacancies,offering superior stability.We detail both classical and innovative in-situ characterization techniques that are central to unraveling the OER mechanism.The advanced in-situ electrochemical techniques,such as inductively coupled plasma mass spectroscopy,X-ray photoelectron spectroscopy,and Mössbauer spectroscopy,coupled with in-situ structural analyses,provide crucial insights into the catalyst surface,the electrode-electrolyte interface and the kinetics of OER.This review provides a systematic analysis integrating classical electrochemical methods with advanced in-situ/operando techniques,specifically focusing on understanding OPM.While numerous studies have examined individual characterization methods,this study systematically integrates traditional electrochemical approaches with in-situ and operando techniques,offering critical insights into their complementary roles in elucidating reaction pathways.The integration of these methodologies provides unprecedented understanding of catalyst behavior under operational conditions,guiding the rational design of next-generation OER catalysts.Furthermore,we discuss essential standardized test toolkits and protocols,such as those for rotating disk electrode and membrane electrode assembly,which are vital for ensuring reproducibility and scalability in OER catalyst research.展开更多
Transition metal phosphides exhibit excellent efficiency in the oxygen evolution reaction under alkaline conditions,and they have garnered widespread recognition.Currently,most studies have focused on the evolution an...Transition metal phosphides exhibit excellent efficiency in the oxygen evolution reaction under alkaline conditions,and they have garnered widespread recognition.Currently,most studies have focused on the evolution and role of metal cations in the oxygen evolution reaction process,while attention to phosphorus elements is relatively scarce.Actually,phosphides possess unique properties that distinguish them from other metal compounds,and the role of phosphorus in them cannot be ignored.This study used nickel phosphide(Ni_(2)P)as a model catalyst to reveal the reconstruction and dynamic behavior of anions under alkaline conditions through cyclic voltammetry.The results indicate that as the cycle progresses,surface phosphides are converted into active oxyhydroxides.It is worth noting that the presence of the P element accelerates the rapid completion of the reconstruction process but also exhibits triple synergistic functions.First,the internal phosphorus nuclei of the active layer act as conductive scaffolds,effectively enhancing the efficiency of electron conduction.Second,the oxygen-containing anions formed in situ on metal hydroxides optimize the adsorption of reaction intermediates.Finally,the phosphorus atoms dissolved in the electrolyte suppress nickel loss,improve stability,and increase the electrochemical activity specific surface area,exposing more active sites.This study elucidates the oxygen evolution reaction mechanism of phosphides from a novel perspective,enhancing comprehension of surface reconstruction phenomena and the characteristics of active sites,guiding the rational design of phosphide pre-catalysts.展开更多
Efficient alkaline hydrogen evolution reaction(HER)catalysts are critical for anion exchange membrane water electrolysis(AEMWE).However,the intrinsic scaling relationship between water dissociation and OH desorption f...Efficient alkaline hydrogen evolution reaction(HER)catalysts are critical for anion exchange membrane water electrolysis(AEMWE).However,the intrinsic scaling relationship between water dissociation and OH desorption fundamentally impedes designing catalysts requiring concurrent superior water dissociation and facile OH desorption.Here,we engineer a superhydrophilic Ru/Cr_(2)O_(3) heterostructured electrocatalyst through in situ confinement of Ru nanoparticles(5-10 nm)within a Cr_(2)O_(3) matrix.Acting as a Lewis acid,the Cr_(2)O_(3) component provides alternative sites for water dissociation,accelerating the Volmer step kinetics and downshifting the Ru d-band center via interfacial charge transfer,while simultaneously adsorbing OH-to form a surface-bound Lewis base that repels excess OH-from Ru sites,thereby suppressing hydroxyl over-adsorption.Concurrently,the superhydrophilic surface architecture promotes efficient hydrogen bubble release,thereby reducing mass transport resistance.As a result,the Ru/Cr_(2)O_(3) heterostructured electrocatalyst exhibits an ultralow overpotential of 36.7 mV at 10 mA cm^(-2) and a Tafel slope of 33.2 mV dec^(-1).Integrated into an AEMWE device,the electrode delivers500 mA cm^(-2) for 2000 h in 1.0 M KOH,underscoring its industrial viability(hydrogen production energy consumption per cubic meter(EW):3.94 kW h m^(-3);electricity-to-hydrogen energy conversion efficiency(η_(ETH)):89%@80℃).展开更多
Current quantitative characterization methods for the mechanical response and damage evolution of coal seams at different burial depths under mining-induced stress remains insufficient.To address this,this study estab...Current quantitative characterization methods for the mechanical response and damage evolution of coal seams at different burial depths under mining-induced stress remains insufficient.To address this,this study establishes a quantitative characterization model for the evolution of mechanical properties in gas-bearing coal masses at varying burial depths.It innovatively introduces a dual damage quantification technique and develops a coupled damage evolution model that comprehensively considers energy evolution,effective mining-induced stress,permeability,and a damage sensitivity coefficient,followed by extensive analysis.Key findings include:coal damage exhibits heterogeneous evolutionary characteristics under mining-induced stress;based on the theory of irreversible deformation,the proposed damage characterization equation can effectively determine the critical damage threshold of coal;the three-parameter EXP function model is more suitable for characterizing the time-dependent damage process of coal under mining-induced stress;a new characterization method for the coal brittleness evaluation index is proposed,revealing an 800 m burial depth boundary for the coal brittleness index;at the microscopic level,achieving quantitative characterization of the correlation between peak stress and the average reduction in functional groups during mining-induced failure of coal at different burial depths.Finally,the mapping relationship between laboratory experimental parameters and field monitoring indicators for early warning of coal mine dynamic disasters is established.展开更多
Root-inspired anchorage systems in the field of bio-inspired geotechnics are renowned for enhancing the pullout capacity of traditional geotechnical anchorage systems by simulating the morphology and architecture of p...Root-inspired anchorage systems in the field of bio-inspired geotechnics are renowned for enhancing the pullout capacity of traditional geotechnical anchorage systems by simulating the morphology and architecture of plant root systems.However,limited studies have explored their practical applications,particularly in improving slope stability.To fill this gap,this study investigates the reinforcement effect of root-inspired anchors on slope stabilization using transparent soil modeling and 3D-printed anchors,and examines the impact of anchor branching patterns(i.e.branching numbers,branching angle,and branching nodes)on slope bearing capacity,shear band evolution,and temporal and spatial variation of slope deformation.The results show that peak slope bearing capacity increases with branching numbers and branching angles,correlating with the envelope area of the curved shear band.Upper anchors result in step-like deflections in the shear band near the trailing edge,while lower anchors convert the upward concave shear band into an upward convex one,thus increasing the slope bearing capacity.Slope deformation is minimized with intermediate branching parameters,such as a branching number of 4 and a branching angle of 45°.The anchor reinforcement mechanisms,i.e.anchor rod shear resistance,interface friction,anchor pullout capacity,and plate tightening effects,are comprehensively discussed,and the installation effects resulting from compromise slope modeling are identified as the contributors.These findings shed light on the failure process of root-inspired anchors reinforced slopes and provide a preliminary reference for potential applications,especially for the tradeoff between anchor branching,slope deformation,and slope stability.展开更多
During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective r...During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective reconstruction regulation strategies.In this study,we first explored the reconstruction mechanism of CoS_(2)during OER from the perspective of electronic structure and identified two possible pathways:the OH-assisted mechanism and the O-assisted mechanism.Further verification showed that these mechanisms are universally applicable to other TMSs(e.g.,FeS_(2)).Based on the reconstruction mechanism,we investigated the basic reasons for the influence of various regulation strategies,such as vacancy modification and facet engineering,on the reconstruction ability.This verified that the method of analyzing the change in the reconstruction ability of catalysts based on the reconstruction mechanism has a high degree of applicability.Importantly,we proposed a core regulation strategy:the coordination symmetry regulation strategy.Specifically,by breaking the symmetry of the surface coordination environment of TMSs(such as introducing heteroatom doping or strain),the reconstruction process will be facilitated.Our findings provide a comprehensive mechanistic explanation for the reconstruction of TMS catalysts and offer a new idea for the rational design of OER catalysts with controllable reconstruction capacity.展开更多
基金National MCF Energy R&D Program of China(2018YFE0306100)Natural Science Foundation of Hunan Province for Distinguished Young Scholars(2021JJ10062)+1 种基金National Natural Science Foundation of China(52101028)China Postdoctoral Science Foundation(2021M703628)。
文摘Combining the phase-field method and the moving boundary method,a three-dimensional phase-field simulation was conducted for the growth and grain evolution of Ti films deposited by physical vapor deposition under different deposition rates and grain orientations.The evolution of grain morphology and grain orientation was also taken into consideration.Simulation results show that at lower deposition rates,the surface of the formed Ti film exhibits a distinct oriented texture structure.The surface roughness of the Ti film is positively correlated with the grain misorientation.Moreover,the surface roughness obtained from the simulation is in good agreement with the experiment results.
文摘While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an analysis framework(expression variance decomposition,EVaDe)for comparative single-cell expression data based on phenotypic evolution theory.After decomposing the gene expression variance into separate components,we use two strategies to identify genes exhibiting large between-taxon expression divergence and small within-cell-type expression noise in certain cell types,attributing this pattern to putative adaptive evolution.In a dataset of primate prefrontal cortex,we find that such humanspecific key genes enrich with neurodevelopment-related functions,while most other genes exhibit neutral evolution patterns.Specific neuron types are found to harbor more of these key genes than other cell types,thus likely to have experienced more extensive adaptation.Reassuringly,at the molecular sequence level,the key genes are significantly associated with the rapidly evolving conserved non-coding elements.An additional case analysis comparing the naked mole-rat(NMR)with the mouse suggests that innateimmunity-related genes and cell types have undergone putative expression adaptation in NMR.Overall,the EVaDe framework may effectively probe adaptive evolution mode in single-cell expression data.
基金supported by Science and Technology Program from the Forestry Administration of Guangdong Province(2024KJQT0012)the Guangdong Provincial Key R&D Program(2022B1111040001)+2 种基金the National Forestry Administration rare and endangered species field rescue and breeding project(Gui lin hu yu O10)the National Natural Science Foundation of China(32200337)a fellowship from the China Postdoctoral Science Foundation(2022M712003).
文摘Gibbons are small,arboreal apes that play a critical role in tropical biodiversity and ecosystem ecology.However,nearly all species of gibbons are threatened by habitat loss,illegal trade,hunting,and other human activities.Long-term poor understanding of their genetics and evolution undermines effective conservation efforts.In this study,we analyse comparative population genomic data of four Nomascus species.Our results reveal strong genetic differentiation and gene flow among Nomascus species.Additionally,we identify genomic features that are potentially related to natural selection linked to vocalization,fructose metabolism,motor balance,and body size,consistent with the unique phenotype and adaptability of gibbons.Inbreeding,coupled with population declines due to climate change and historical human activities,leads to reduced genetic diversity and the accumulation of deleterious variations that likely affect cardiovascular disease and the reproductive potential of gibbons and further reduce their fitness,highlighting the urgent need for effective conservation strategies.
基金supported by the Korea Institute for Advancement of Technology (KIAT)the Ministry of Trade,Industry&Energy (MOTIE) of the Republic of Korea (No. P0022130)by the Institute of Information&Communications Technology Planning&Evaluation(IITP)-Innovative Human Resource Development for Local Intellectualization program grant funded by the Korea government (MSIT)(IITP-2025-RS-2023-00259678)
文摘To realize the practical application of anion exchange membrane water electrolysis(AEMWE),it is essential to develop highly active,durable,and cost-effective electrocatalyst for oxygen evolution reaction(OER).Herein,we report a hollow-structured Ni_(x)Co_(1−x)O/Ni_(3)S_(2)/Co_(9)S_(8)heterostructure synthesized via sequential template-assisted growth,thermal oxidation,and controlled sulfidation process.The abundant bimetallic heterointerfaces not only provide additional active sites but also promote electronic modulation via charge redistribution.Additionally,the porous and hollow architecture enhances active surface area and mass transfer ability,thereby increasing the number of accessible active sites for alkaline OER.As a result,the prepared electrocatalyst achieves low overpotential of 310 mV at 10 mA cm^(−2)and small Tafel slope of 55.94 mV dec^(−1),demonstrating the exceptional electrocatalytic performance for alkaline OER.When integrated as the anode in an AEMWE cell,it delivers outstanding performance with only 1.657 V at 1.0 A cm^(−2)and reaches high current density of 5.0 A cm^(−2)at 1.989 V,surpassing those of commercial RuO_(2).The cell also shows excellent long-term durability over 100 h with minimal degradation.This study highlights the strong potential of rationally engineered oxide/sulfide heterostructures for next-generation alkaline water electrolysis.
基金supported by the Yunnan Province Science and Technology Plan Project(No.202403AA080001-4)the Key Research and Development Project of Guangxi,China(No.guikeAB24010144)the National Key Research and Development Project of China(Nos.2021YFB3901402 and 2018YFC1504802)。
文摘To reveal the influence of coupled effects of dry-wet cycling and precompression stress(CEDWCPS)on the damage evolution of limestone with horizontal fissure(LHF),a series of degradation and uniaxial compression tests were conducted,and a corresponding piecewise damage constitutive model(PDCM)was established.We found that both dry-wet cycling and precompression stress deteriorate the physical properties,alter the microscopic characteristics,and reduce the mechanical properties of the LHF.These degradations are particularly pronounced under the CEDWCPS,although the magnitude of these changes gradually diminishes with the progression of dry-wet cycling.Meanwhile,they also reduce the deformation degree,prolong the micropore compaction stage,shorten the unstable crack propagation stage,lower the frequency and intensity of AE events,decrease the high-amplitude and high-frequency AE signals,enlarge crack scales,and shorten the crack initiation time.Among the changes of these indicators,the dry-wet cycling plays a dominant role.The crack types of LHF under the CEDWCPS(LHFCEDWCPS)are predominantly tensile cracks,supplemented by shear cracks.The failure mode can be defined as tensileshear composite failure.Finally,the established PDCM effectively captures the nonlinear deformation of micropore and the linear deformation of the matrix in LHFCEDWCPS,with all corresponding R^(2) consistently exceeding 0.97.
基金National Natural Science Foundation of China,No.42277488Strategic Priority Research Program of the Chinese Academy of Sciences,No.XDA26010301。
文摘Understanding the evolution and mechanisms of livestock industry agglomeration provides valuable policy insights for reconciling growing meat demand with constrained resource endowments. This study analyzes the spatial agglomeration of livestock industry at the county level across China from 2000 to 2022 using the localization quotient and Moran's I. An interpretable machine learning approach is employed to test hypotheses concerning the driving mechanisms underlying the spatial distribution of livestock industry. The results show that the agglomeration of China's livestock industry is intensifying, with the agro-pastoral transitional zone(APTZ) emerging as a prominent agglomeration area and distinct agglomeration patterns observed within the zone as well as in its eastern and western regions. Proximity to markets has become an increasingly important determinant of livestock industry agglomeration in China. This market-driven shift has heightened the demand for agricultural feed, prompting the livestock industry to relax its dependence on local natural resource endowments and gradually relocate eastward. Regionally, the agglomeration within the APTZ is shaped by the joint effects of natural and social factors. Natural factors dominate agglomeration dynamics in the western regions of the zone, whereas social factors are more influential in its eastern regions.
基金funding from the National Natural Science Foundation of China(22378289)the Key Central Government Guides Local Funds for Science and Technology Development(YDZJSX2022A021)the special fund for Science and Technology Innovation Teams of Shanxi Province(202304051001026)。
文摘The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate evolution mechanism(AEM),lattice oxygen mechanism(LOM),and oxide path mechanism(OPM).Compared to AEM,limited by scaling relationships,and LOM,constrained by stability issues,the OPM offers a promising alternative by enabling direct O-O bond formation via dual active sites,thus bypassing^(*)OOH intermediates and lattice O involvement and achieving a balance between activity and durability.However,activating the OPM process requires precise control over the spatial and electronic structure of active sites,making the design of OPM-based catalysts challenging.While previous reviews have focused on homo/heteronuclear diatomic perspectives of OPM-based catalysts,it is urgent to systematically summarize design strategies to provide a rational reference for their development.Herein,a review of design strategies for OPM-based OER catalysts across three scales is comprehensively presented,including in-situ engineering,doping-enabled sites reconstruction,and introducing new sites for nanoparticles,direct synthesis or post-treatments for molecular catalysts,and doping or template strategies for atom pairs or arrays.The unique advantage of atom arrays is also highlighted,and their future research directions and possible strategies are discussed.This review provides a systematic summary and forward-looking perspectives for rationally designing high-performance OPM-based OER catalysts.
文摘The shale gas development in China faces challenges such as complex reservoir conditions and high development costs.Based on the pore pressure and geostress coupling theory,this paper studies the geostress evolution laws and fracture network characteristics of shale gas infill wells.A mechanism model of CN platform logging data and geomechanical parameters is established to simulate the influence of parent well’s production on the geostress in the infill well area.It is suggested that with the increase of production time,normal fault stress state and horizontal stress deflection will occur.The smaller the parent well spacing and the longer the production time,the earlier the normal fault stress state appears and the larger the range.Based on the model,the fracture network morphology and construction parameters of infill wells are optimized.parentparentparentparent The results indicate that:1:A well spacing of 500 m achieves a Pareto optimum between“full reserve coverage”and“stress barrier”;2:A parent well recovery degree of 30%corresponds to the critical point of stress reversal,where the lateral deflection rate of the infill fracture is less than 8%and the SRV loss is minimized;3:6-cluster intensive completion with twice the liquid intensity increases the fracture complexity index by 1.7 times,enhances well group EUR by 15.4%,and reduces single-well cost by 22%.This research fills the theoretical gap in the collaborative optimization of“multi-parameter,multi-objective and multi-constraint”and provide parameter optimization basis for shale gas infill well development in China and help to improve the development efficiency and economic benefits.
基金support from the National Key Research and Development Program of China(No.2023YFA0914100/2023YFA0914102)the National Natural Science Foundation of China(Nos.22077029 and 22034002)+2 种基金the Science Fund for Distinguished Young Scholars of Hunan Province(No.2021JJ10034)support from the National Natural Science Foundation of China(No.22276049)M.M.acknowledge the support from the National Natural Science Foundation of China(No.22276050).
文摘We report for the first time the combination of directed evolution focused on enhancing and reversing the stereoselectivity of an enzyme with Cu(I)-mediated click chemistry(CuAAC),providing an asymmetric click approach for versatile chiral triazoles products.In this study,the halohydrin dehalogenase HheG was used as the enzyme which was evolved to induce a stereoselective ring-opening reaction of cyclic epoxides in the presence of NaN3 with the formation of chiral azido products.Two mutants of opposite stereopreference were generated,which convert cyclohexene oxide as well as cycloheptene oxide to(1S,2S)-2-azidocyclohexanol,(1R,2R)-2-azidocyclohexanol,(1S,2S)-2-azidocycloheptanol and(1R,2R)-2-azidocycloheptanol with essentially high stereoselectivity.The chiral products were then subjected to CuAAC in reactions with structurally different alkynes.Since HheG was found to be compatible with Cu(I),the process was also performed successfully in a unique 2-step one-pot process leading to various chiral triazoles.In order to understand the enhancement and reversal of the evolved enantioselectivity,QM and MD computations were performed.This approach harnesses the modifiability and high stereoselectivity of the evolved biocatalysts in combination with click chemistry.It holds great potential for diverse fields,particularly in the area of pharmaceuticals.
基金financially supported by the National Natural Science Foundation of China(32301514)the Young Elite Scientist Sponsorship Program by CAST(YESS20220240)。
文摘The advancement of effective and stable non-precious metal-based catalysts for oxygen evolution reactions(OER)with a lowcost and simple technique is essential for the practical application of rechargeable zinc–air battery(ZAB).However,facilitating the deep reconstruction of electrocatalysts to form active species remains a significant challenge.Here,a simple two-step method composed of impregnation and carbonization process is proposed to synthesize N,S co-doped microcrystalline cellulose-derived carbon-supported nickel sulfide(Ni_(3)S_(2))nanoparticles.The in situ Raman reveals that Fe substitution promotes the reconstruction of Ni_(3)S_(2),accompanied by the cleavage of the Ni–S bond,leading to the deep reconstruction into(Ni,Fe)OOH(DR-(Ni,Fe)OOH)during the OER.Moreover,density functional theory calculations reveal that Fe substitution induces a downshift in the energy band structure,which lowers the energy barriers and thereby improves the kinetics of the OER.The generated DR-(Ni,Fe)OOH delivers a relatively low overpotential of 260 m V and superior durability for 50 h under OER condition.The ZAB incorporating DR-(Ni,Fe)OOH+Pt/C as the air cathode demonstrates superior efficiency and durability,achieving a peak power density of 188.3 m W cm^(-2),a specific capacity of 811.1 m Ah g^(-1),and long-term stability exceeding 200 h.
基金funded by the Innovative Research Group Project of the National Natural Science Foundation of China(Nos.U24A20592 and 42272137)Guizhou Province Science and Technology Innovation Talent Team,Construction of the Science and Technology Innovation Talent Team for the Evaluation and Development of Unconventional Natural Gas Resources in Complex Structural Areas(No.Qian Ke He Platform Talent-CXTD[2023]013)。
文摘To clarify the thermal evolution characteristics of organic matter in the ZizhongWeiyuan area in Sichuan Basin,solid bitumen reflectance of the Lower Cambrian Qiongzhusi Formation(QFm)shale was measured by Raman Spectroscopy(RS)method.Constrained by vitrinite reflectance(Ro)data,burial and thermal evolution histories of QFm shale were reconstructed through basin numerical simulation technology.The evolution model of and critical period of organic matter was determined,and its dominant drivers were analyzed.The results show that the asphalt Raman vitrinite reflectance(_(Rmc)Ro)ranges from 3.21%to 4.15%.Thermal maturity within the trough follows a southern part>central part>northern part trend.Thermal maturity is moderate within the paleo-uplift,whereas organic matter outside the paleo-uplift has undergone graphitization.Two types of thermal evolution imprints were established:a continuous heating type and a stop heating type of Silurian–Permian.Sedimentary burial,paleogeomorphology,tectonic movement and Emeishan mantle plume are the dominant drivers of multi-stage thermal imprints of the QFm shale.The three factors are coupled with each other.The Late Caledonian and Late Indosinian are the key periods of organic matter thermal evolution.The Leshan-Longnüsi paleo-uplift weakens the thermal effect of the Permian Emeishan mantle plume.The current thermal evolution pattern of the QFm is mainly determined by the continuous subsidence of the Triassic–Cretaceous.Stop heating model of Silurian–Permian locks the maturity of organic matter in the gold window,thus controlling the enrichment of QFm shale gas.It provides new insights for shale gas migration,enrichment and effective exploration and development of shale gas in the Lower Paleozoic QFm.
基金National Natural Science Foundation of China,Grant/Award Numbers:52274082,42307244,42230704Jiangxi Provincial Natural Science Foundation,Grant/Award Number:2024BAB26047+3 种基金Innovative Experts,Long-term Program of Jiangxi Province,Grant/Award Number:jxsq2018106049Opening Foundation of Anhui Province Key Laboratory of Building Structure and Underground Engineering,Grant/Award Number:KLBSUE‐2022‐04Program of Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology,Grant/Award Number:JXUSTQJBJ2020003Fundamental Research Funds for the Central Universities,Grant/Award Number:2023QN1024。
文摘Prediction of permeability changes in surrounding rock induced by engineering disturbances is crucial for mitigating tunnel water inrush accidents.This study investigates the progressive failure characteristics and permeability evolution of hard and soft rocks subjected to triaxial compression.A series of laboratory tests were conducted at confining pressures ranging from 4 to 20 MPa.Experimental results demonstrate that rock permeability variation with strain shows three distinct stages:an initial decrease,a stage of rapid mutation,and a postpeak increase.The concept of critical permeability barrier strength is introduced,representing the stress level at which continuous fracture formation enables significant seepage.Furthermore,two generalized permeability–stress models are developed for soft and hard rocks.The predicted permeability values obtained from these models align well with the experimental data.These findings offer valuable insights into the hydro-mechanical coupling behavior of rocks,providing a foundation for safe construction practices in underground engineering.
基金supported by the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
基金supported by the National Natural Science Foundation of China(Nos.22209088,22472082,and 22075159)Taishan Scholar Program(Nos.tsqn202103058 and tsqn202306173)Qingdao New Energy Shandong Laboratory Open Project(QNESLOP202302)。
文摘Regulating the microenvironment of the support enables precise control of electronic metal-support interactions(EMSI),boosting better catalytic activity of the metal species.However,the fundamental relationship between support defect-induced EMSI modulation and the resulting catalytic performance enhancement still needs further elucidation.Herein,a nonequilibrium high-temperature shock(HTS)method,which combines rapid high-temperature heating at 1273 K for 30 s with liquid nitrogen quenching,was adopted to load uniform Pt nanoparticles onto the nitrogen vacancy-rich TiN support(Pt@TiNVN).The catalyst demonstrates a high mass activity of 15.99 A mgPt^(-1)at an overpotential of 100 mV for the hydrogen evolution reaction(HER)in acidic solution and exhibits long-term stability for 60 h at 200 mA cm^(-2).Detailed spectroscopic characterizations and theoretical calculations reveal that the generated nitrogen vacancies can effectively modulate the charge transfer between Pt nanoparticles and the TiN-VN support,leading to a downshifted d-band center of metallic Pt and optimized Pt-H bond strength.This nonequilibrium HTS approach offers new and valuable insights into designing advanced electrocatalysts by harnessing substrate defects to modulate the electronic states of loaded noble metals.
基金funded by the EU H2020 Marie Skłodowska-Curie Fellowship (1439425)the National Natural Science Foundation of China (No. 52171199 and 22479011)
文摘Water electrolysis is pivotal for converting renewable energy into clean hydrogen fuel,addressing global energy demand sustainably.However,the development of highly efficient and cost-effective catalysts for the oxygen evolution reaction(OER)remains a significant challenge,particularly at the industrial scale.This report explores a newly discovered pathway,the oxide path mechanism(OPM) for OER-mechanism involving the oxide formation and evolution during the reaction,emphasizing its potential to overcome existing limitations.OPM enables direct O-O coupling without oxygen vacancies,offering superior stability.We detail both classical and innovative in-situ characterization techniques that are central to unraveling the OER mechanism.The advanced in-situ electrochemical techniques,such as inductively coupled plasma mass spectroscopy,X-ray photoelectron spectroscopy,and Mössbauer spectroscopy,coupled with in-situ structural analyses,provide crucial insights into the catalyst surface,the electrode-electrolyte interface and the kinetics of OER.This review provides a systematic analysis integrating classical electrochemical methods with advanced in-situ/operando techniques,specifically focusing on understanding OPM.While numerous studies have examined individual characterization methods,this study systematically integrates traditional electrochemical approaches with in-situ and operando techniques,offering critical insights into their complementary roles in elucidating reaction pathways.The integration of these methodologies provides unprecedented understanding of catalyst behavior under operational conditions,guiding the rational design of next-generation OER catalysts.Furthermore,we discuss essential standardized test toolkits and protocols,such as those for rotating disk electrode and membrane electrode assembly,which are vital for ensuring reproducibility and scalability in OER catalyst research.
基金support of the National Natural Science Foundation of China(22275035).
文摘Transition metal phosphides exhibit excellent efficiency in the oxygen evolution reaction under alkaline conditions,and they have garnered widespread recognition.Currently,most studies have focused on the evolution and role of metal cations in the oxygen evolution reaction process,while attention to phosphorus elements is relatively scarce.Actually,phosphides possess unique properties that distinguish them from other metal compounds,and the role of phosphorus in them cannot be ignored.This study used nickel phosphide(Ni_(2)P)as a model catalyst to reveal the reconstruction and dynamic behavior of anions under alkaline conditions through cyclic voltammetry.The results indicate that as the cycle progresses,surface phosphides are converted into active oxyhydroxides.It is worth noting that the presence of the P element accelerates the rapid completion of the reconstruction process but also exhibits triple synergistic functions.First,the internal phosphorus nuclei of the active layer act as conductive scaffolds,effectively enhancing the efficiency of electron conduction.Second,the oxygen-containing anions formed in situ on metal hydroxides optimize the adsorption of reaction intermediates.Finally,the phosphorus atoms dissolved in the electrolyte suppress nickel loss,improve stability,and increase the electrochemical activity specific surface area,exposing more active sites.This study elucidates the oxygen evolution reaction mechanism of phosphides from a novel perspective,enhancing comprehension of surface reconstruction phenomena and the characteristics of active sites,guiding the rational design of phosphide pre-catalysts.
基金supported by the National Natural Science Foundation of China(22479113,52101268)the Fundamental Research Funds for the Central Universities(buctrc202323)。
文摘Efficient alkaline hydrogen evolution reaction(HER)catalysts are critical for anion exchange membrane water electrolysis(AEMWE).However,the intrinsic scaling relationship between water dissociation and OH desorption fundamentally impedes designing catalysts requiring concurrent superior water dissociation and facile OH desorption.Here,we engineer a superhydrophilic Ru/Cr_(2)O_(3) heterostructured electrocatalyst through in situ confinement of Ru nanoparticles(5-10 nm)within a Cr_(2)O_(3) matrix.Acting as a Lewis acid,the Cr_(2)O_(3) component provides alternative sites for water dissociation,accelerating the Volmer step kinetics and downshifting the Ru d-band center via interfacial charge transfer,while simultaneously adsorbing OH-to form a surface-bound Lewis base that repels excess OH-from Ru sites,thereby suppressing hydroxyl over-adsorption.Concurrently,the superhydrophilic surface architecture promotes efficient hydrogen bubble release,thereby reducing mass transport resistance.As a result,the Ru/Cr_(2)O_(3) heterostructured electrocatalyst exhibits an ultralow overpotential of 36.7 mV at 10 mA cm^(-2) and a Tafel slope of 33.2 mV dec^(-1).Integrated into an AEMWE device,the electrode delivers500 mA cm^(-2) for 2000 h in 1.0 M KOH,underscoring its industrial viability(hydrogen production energy consumption per cubic meter(EW):3.94 kW h m^(-3);electricity-to-hydrogen energy conversion efficiency(η_(ETH)):89%@80℃).
文摘Current quantitative characterization methods for the mechanical response and damage evolution of coal seams at different burial depths under mining-induced stress remains insufficient.To address this,this study establishes a quantitative characterization model for the evolution of mechanical properties in gas-bearing coal masses at varying burial depths.It innovatively introduces a dual damage quantification technique and develops a coupled damage evolution model that comprehensively considers energy evolution,effective mining-induced stress,permeability,and a damage sensitivity coefficient,followed by extensive analysis.Key findings include:coal damage exhibits heterogeneous evolutionary characteristics under mining-induced stress;based on the theory of irreversible deformation,the proposed damage characterization equation can effectively determine the critical damage threshold of coal;the three-parameter EXP function model is more suitable for characterizing the time-dependent damage process of coal under mining-induced stress;a new characterization method for the coal brittleness evaluation index is proposed,revealing an 800 m burial depth boundary for the coal brittleness index;at the microscopic level,achieving quantitative characterization of the correlation between peak stress and the average reduction in functional groups during mining-induced failure of coal at different burial depths.Finally,the mapping relationship between laboratory experimental parameters and field monitoring indicators for early warning of coal mine dynamic disasters is established.
基金supported by the High-end Foreign Expert Introduction Program(Grant No.G2022165004L)the Sichuan Transportation Science and Technology Project(Grant No.2018-ZL-01)China Railway 20th Bureau Science and Technology Project(Grant No.YF1900SD07B).
文摘Root-inspired anchorage systems in the field of bio-inspired geotechnics are renowned for enhancing the pullout capacity of traditional geotechnical anchorage systems by simulating the morphology and architecture of plant root systems.However,limited studies have explored their practical applications,particularly in improving slope stability.To fill this gap,this study investigates the reinforcement effect of root-inspired anchors on slope stabilization using transparent soil modeling and 3D-printed anchors,and examines the impact of anchor branching patterns(i.e.branching numbers,branching angle,and branching nodes)on slope bearing capacity,shear band evolution,and temporal and spatial variation of slope deformation.The results show that peak slope bearing capacity increases with branching numbers and branching angles,correlating with the envelope area of the curved shear band.Upper anchors result in step-like deflections in the shear band near the trailing edge,while lower anchors convert the upward concave shear band into an upward convex one,thus increasing the slope bearing capacity.Slope deformation is minimized with intermediate branching parameters,such as a branching number of 4 and a branching angle of 45°.The anchor reinforcement mechanisms,i.e.anchor rod shear resistance,interface friction,anchor pullout capacity,and plate tightening effects,are comprehensively discussed,and the installation effects resulting from compromise slope modeling are identified as the contributors.These findings shed light on the failure process of root-inspired anchors reinforced slopes and provide a preliminary reference for potential applications,especially for the tradeoff between anchor branching,slope deformation,and slope stability.
基金supported by the National Key Research and Development program(2022YFA1504000)the National Natural Science Foundation of China(22302101)+4 种基金the Fundamental Research Funds for the Central Universities(63185015)the Shenzhen Science and Technology Program(JCYJ20210324121002007,JCYJ20230807151503007)the Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202402AO370001)the China Postdoctoral Science Foundation(2022M721699)the Guangdong Basic and Applied Basic Research Foundation(2024A1515010347).
文摘During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective reconstruction regulation strategies.In this study,we first explored the reconstruction mechanism of CoS_(2)during OER from the perspective of electronic structure and identified two possible pathways:the OH-assisted mechanism and the O-assisted mechanism.Further verification showed that these mechanisms are universally applicable to other TMSs(e.g.,FeS_(2)).Based on the reconstruction mechanism,we investigated the basic reasons for the influence of various regulation strategies,such as vacancy modification and facet engineering,on the reconstruction ability.This verified that the method of analyzing the change in the reconstruction ability of catalysts based on the reconstruction mechanism has a high degree of applicability.Importantly,we proposed a core regulation strategy:the coordination symmetry regulation strategy.Specifically,by breaking the symmetry of the surface coordination environment of TMSs(such as introducing heteroatom doping or strain),the reconstruction process will be facilitated.Our findings provide a comprehensive mechanistic explanation for the reconstruction of TMS catalysts and offer a new idea for the rational design of OER catalysts with controllable reconstruction capacity.
