Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
The majority of the projectiles used in the hypersonic penetration study are solid flat-nosed cylindrical projectiles with a diameter of less than 20 mm.This study aims to fill the gap in the experimental and analytic...The majority of the projectiles used in the hypersonic penetration study are solid flat-nosed cylindrical projectiles with a diameter of less than 20 mm.This study aims to fill the gap in the experimental and analytical study of the evolution of the nose shape of larger hollow projectiles under hypersonic penetration.In the hypersonic penetration test,eight ogive-nose AerMet100 steel projectiles with a diameter of 40 mm were launched to hit concrete targets with impact velocities that ranged from 1351 to 1877 m/s.Severe erosion of the projectiles was observed during high-speed penetration of heterogeneous targets,and apparent localized mushrooming occurred in the front nose of recovered projectiles.By examining the damage to projectiles,a linear relationship was found between the relative length reduction rate and the initial kinetic energy of projectiles in different penetration tests.Furthermore,microscopic analysis revealed the forming mechanism of the localized mushrooming phenomenon for eroding penetration,i.e.,material spall erosion abrasion mechanism,material flow and redistribution abrasion mechanism and localized radial upsetting deformation mechanism.Finally,a model of highspeed penetration that included erosion was established on the basis of a model of the evolution of the projectile nose that considers radial upsetting;the model was validated by test data from the literature and the present study.Depending upon the impact velocity,v0,the projectile nose may behave as undistorted,radially distorted or hemispherical.Due to the effects of abrasion of the projectile and enhancement of radial upsetting on the duration and amplitude of the secondary rising segment in the pulse shape of projectile deceleration,the predicted DOP had an upper limit.展开更多
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resol...We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resolution transmission electron microscopy(HRTEM),and electron backscatter diffraction(EBSD).The findings reveal that annealing processing has a significant impact on diminishing residual stresses.As the annealing temperature rose from 950 to 1150℃,the majority of the residual stresses were relieved from 60.1 MPa down to 10.9 MPa.Moreover,the stress relaxation mechanism transitioned from being mainly controlled by dislocation slip to a combination of dislocation slip and grain boundary migration.Meanwhile,the annealing treatment promotes the decomposition of the Laves,accompanied by the precipitation ofμ-(Mo_(6)Co_(7))starting at 950℃ and reaching a maximum value at 1050℃.The tensile strength and plasticity of the annealing alloy at 1150℃ reached the maximum(1394 MPa,56.1%)which was 131%,200%fold than those of the as-cast alloy(1060 MPa,26.6%),but the oxidation process in the alloy was accelerated at 1150℃.The enhancement in durability and flexibility is primarily due to the dissolution of the brittle phase,along with the shape and dispersal of theγ′phase.展开更多
High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion te...High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.展开更多
Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB ...Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB structures,a series of triaxial stepwise-increasing-amplitude cyclic loading experiments was conducted with cylindrical RB specimens(rock on outside,backfill on inside)with different volume fractions of rock(VF=0.48,0.61,0.73,and 0.84),confining pressures(0,6,9,and 12 MPa),and cyclic loading rates(200,300,400,and 500 N/s).The damage evolution and meso-crack formation during the cyclic tests were analyzed with results from stress-strain hysteresis loops,acoustic emission events,and post-failure X-ray 3D fracture morphology.The results showed significant differences between cyclic and monotonic loadings of RB specimens,particularly with regard to the generation of shear microcracks,the development of stress memory and strain hardening,and the contact forces and associated friction that develops along the rock-backfill interface.One important finding is that as a function of the number of cycles,the elastic strain increases linearly and the dissipated energy increases exponentially.Also,compared with monotonic loading,the cyclic strain hardening characteristics are more sensitive to rising confining pressures during the initial compaction stage.Another finding is that compared with monotonic loading,more shear microcracks are generated during every reloading stage,but these microcracks tend to be dispersed and lessen the likelihood of large shear fracture formation.The transition from elastic to plastic behavior varies depending on the parameters of each test(confinement,volume fraction,and cyclic rate),and an interesting finding was that the transformation to plastic behavior is significantly lower under the conditions of 0.73 rock volume fraction,400 N/s cyclic loading rate,and 9 MPa confinement.All the findings have important practical implications on the ability of backfill to support underground excavations.展开更多
Background The role of human lineage mutations(HLMs)in human evolution through post-transcriptional modification is unclear.Aims To investigate the contribution of HLMs to human evolution through post-transcriptional ...Background The role of human lineage mutations(HLMs)in human evolution through post-transcriptional modification is unclear.Aims To investigate the contribution of HLMs to human evolution through post-transcriptional modification.Methods We applied a deep learning model Seqweaver to predict how HLMs impact RNA-binding protein affinity.Results We found that only 0.27%of HLMs had significant impacts on RNA-binding proteins at the threshold of the top 1%of human common variations.These HLMs enriched in a set of conserved genes highly expressed in adult excitatory neurons and prenatal Purkinje neurons,and were involved in synapse organisation and the GTPase pathway.These genes also carried excess damaging coding mutations that caused neurodevelopmental disorders,ataxia and schizophrenia.Among these genes,NTRK2 and ITPR1 had the most aggregated evidence of functional importance,suggesting their essential roles in cognition and bipedalism.Conclusions Our findings suggest that a small subset of human-specific mutations have contributed to human speciation through impacts on post-transcriptional modification of critical brain-related genes.展开更多
The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on...The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.展开更多
With economic development and urbanization in China,the rural settlements have experienced great change.To explore the evolution process of rural settlements in terms of land,population and industry can reveal the dev...With economic development and urbanization in China,the rural settlements have experienced great change.To explore the evolution process of rural settlements in terms of land,population and industry can reveal the development law of rural spatial distribution,population structure and industrial economy in different stages and regions.Studying the development status and evolution characteristics of villages in the upper Tuojiang River basin in Southwest China in the past 20 years are of significant value.The upper Tuojiang River basin includes the main types of terrain found in the Southwest region:mountainous,plains,and hills,exhibiting a certain typicality of geographical characteristics.This study took towns and townships at the town-level scale as the basic unit of research,and constructed an evaluation system for village evolution based on'land,population,and industry'.It employed Criteria Importance Through Inter-Criteria Correlation(CRITIC)analysis to examine the characteristics of village evolution in the area from 2000 to 2020,and used geographic detector analysis to identify the leading factors affecting village evolution.The results show that:(1)From 2000 to 2010,villages in the upper Tuojiang River basin experienced significant changes,and the pace of these transformations slowed from 2010 to 2020.(2)From a comprehensive perspective,from 2000 to 2020,villages in hilly areas show a decline,while villages in plain areas near the city center show a positive urbanization development.(3)Road accessibility and distance from the city center are the main factors that explain the spatial differentiation of village evolution degree in the study area.This study elucidates the spatiotemporal evolution characteristics of villages in the upper Tuojiang River basin and identifies the primary factors contributing to their changes,which will provide a reference for investigating the development of rural areas in different terrains of Southwest China.展开更多
Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibili...Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.展开更多
Developing highly stable and efficient catalysts for oxygen evolution reaction(OER)is extremely important to sustainable energy conversion and storage,but improved efficiency is largely hindered by sluggish reaction k...Developing highly stable and efficient catalysts for oxygen evolution reaction(OER)is extremely important to sustainable energy conversion and storage,but improved efficiency is largely hindered by sluggish reaction kinetics.Dense and bimetal ruthenates have emerged as one of the promising substitutes to replace single-metal ruthenium or iridium oxides,but the fundamental understanding the role of A-site cations is still blurring.Herein,a family of lanthanides(Ln=all the lanthanides except Pm)are applied to synthesize pyrochlore lanthanide ruthenates(Ln_(2)Ru_(2)O_(7)),and only Ln_(2)Ru_(2)O_(7)(Ln=Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,or Lu)with pure phase can be obtained by the ambient-pressure calcination.Compared with the perovskite ruthenates(SrRuO_(3))and rutile RuO_(2),the[RuO_(6)]units in these Ln_(2)Ru_(2)O_(7) present the largely distorted configurations and different energy level splitting to prevent the excessive Ru oxidation and dissolution,which leads the primary improvement in the electrocatalytic OER performance.In the similar crystalline field split states,the charge transfer between[RuO6]units and Ln^(3+)cations also affect catalytic activities,even in the Ln_(2)Ru_(2)O_(7) surface reconstruction during the OER process.Consequently,Tb_(2)Ru_(2)O_(7) showed the highest OER performance among all the prepared Ln_(2)Ru_(2)O_(7) with similar morphologies and crystallization.This systematic work gives fundamental cognition to rational design of high-performance OER electrocatalysts in proper water electrolysis technologies.展开更多
Ingredient optimization plays a pivotal role in the copper industry,for which it is closely related to the concentrate utilization rate,stability of furnace conditions,and the quality of copper production.To acquire a...Ingredient optimization plays a pivotal role in the copper industry,for which it is closely related to the concentrate utilization rate,stability of furnace conditions,and the quality of copper production.To acquire a practical ingredient plan,which should exhibit long duration time with sufficient utilization and feeding stability for real applications,an ingredient plan optimization model is proposed in this study to effectively guarantee continuous production and stable furnace conditions.To address the complex challenges posed by this integer programming model,including multiple coupling feeding stages,intricate constraints,and significant non-linearity,a multi-stage differential-multifactorial evolution algorithm is developed.In the proposed algorithm,the differential evolutionary(DE)algorithm is improved in three aspects to efficiently tackle challenges when optimizing the proposed model.First,unlike traditional time-consuming serial approaches,the multifactorial evolutionary algorithm is utilized to optimize multiple complex models contained in the population of evolutionary algorithm caused by the feeding stability in a parallel manner.Second,a repair algorithm is employed to adjust infeasible ingredient lists in a timely manner.In addition,a local search strategy taking feedback from the current optima and considering the different positions of global optimum is developed to avoiding premature convergence of the differential evolutionary algorithm.Finally,the simulation experiments considering different planning horizons using real data from the copper industry in China are conducted,which demonstrates the superiority of the proposed method on feeding duration and stability compared with other commonly deployed approaches.It is practically helpful for reducing material cost as well as increasing production profit for the copper industry.展开更多
With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transfo...With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.展开更多
Developing highly active oxygen evolution reaction(OER)electrocatalysts with robust durability is essential in producing high-purity hydrogen through water electrolysis.Layered double hydroxide(LDH)based catalysts hav...Developing highly active oxygen evolution reaction(OER)electrocatalysts with robust durability is essential in producing high-purity hydrogen through water electrolysis.Layered double hydroxide(LDH)based catalysts have demonstrated efficient catalytic performance toward the relatively sluggish OER.By considering the promotion effect of phosphate(Pi)on proton transfer,herein,a facile phosphate acid(PA)surface-neutralization strategy is developed to in-situ construct NiCo-LDH/NiCoPi hetero-sheets toward OER catalysis.OER activity of NiCoLDH is significantly boosted due to the proton promotion effect and the electronic modulation effect of NiCoPi.As a result,the facilely prepared NiCo-LDH/NiCoPi catalyst displays superior OER catalytic activity with a low overpotential of 300 mV to deliver 100 mA cm^(-2)OER and a Tafel slope of 73 mV dec^(-1).Furthermore,no visible activity decay is detected after a 200-h continuous OER operation.The present work,therefore,provides a promising strategy to exploit robust OER electrocatalysts for commercial water electrolysers.展开更多
During the mining process of impact-prone coal seams,drilling pressure relief can reduce the impact propensity of the coal seam,but it also reduces the integrity and strength of the coal mass at the side of the roadwa...During the mining process of impact-prone coal seams,drilling pressure relief can reduce the impact propensity of the coal seam,but it also reduces the integrity and strength of the coal mass at the side of the roadway.Therefore,studying the mechanical properties and energy evolution rules of coal samples containing holes and filled structures has certain practical significance for achieving coordinated control of coal mine rockburst disasters and the stability of roadway surrounding rocks.To achieve this aim,seven types of burst-prone coal samples were prepared and subject to uniaxial compression experiments with the aid of a TAW-3000 electro-hydraulic servo testing machine.Besides,the stress–strain curves,acoustic emission signals,DIC strain fields and other data were collected during the experiments.Furthermore,the failure modes and energy evolutions of samples with varying drilled hole sizes and filling materials were analyzed.The results show that the indexes related to burst propensity of the drilled coal samples decline to some extent compared with those of the intact one,and the decline is positively corelated to the diameter of the drilled hole.After hole filling,the strain concentration degree around the drilled hole is lowered to a certain degree,and polyurethane filling has a more remarkable effect than cement filling.Meanwhile,hole filling can enhance the strength and deformation resistance of coal.Hole drilling can accelerate the release of accumulated elastic strain energy,turning the acoustic emission events from low-frequency and high-energy ones to high-frequency and low-energy ones,whereas hole filling can reduce the intensity of energy release.The experimental results and theoretical derivation demonstrate that hole filling promotes coal deformability and strength mainly by weakening stress concentration surrounding the drilled holes.Moreover,the fillings can achieve a better filling effect if their elastic modulus and Poisson’s ratio are closer to those of the coal body.展开更多
Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4...Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.展开更多
This article employs a combined approach of biology and economics to reveal that biological evolution has an economic nature, evolving towards improved energy efficiency. The orthodox Darwinian theory of evolution des...This article employs a combined approach of biology and economics to reveal that biological evolution has an economic nature, evolving towards improved energy efficiency. The orthodox Darwinian theory of evolution describes evolution as the random variation of organisms and their survival through natural selection. In fact, the natural environment itself is a constantly changing context, and the strategy to adapt to this change is to enhance behavioral capabilities, thereby expanding the range and dimensions of behavior. Therefore, the improvement of behavioral capabilities is an important aspect of evolution. The enhancement of behavioral capabilities expands the range of adaptation to the natural environment and increases the space for behavioral choices. Within this space of behavioral choices, some options are more effective and superior to others;thus, the ability to select is necessary to make the improved behavioral capabilities more beneficial to the organism itself. The birth and development of the brain serve the purpose of selection. By using the brain to make selections, at least the “better” behavior will be chosen between two alternatives. Once the better behavior yields better results, and the organism can associate these results with the corresponding behavior, it will persist in this behavior. The persistent repetition of a behavior over generations will form a habit. Habits passed down through generations constitute a new environment, causing the organism’s genes to activate or deactivate certain functions, ultimately leading to genetic changes that are beneficial to that habit. Since the brain’s selection represents the organism’s self-selection, it differs from random variation;it is also a rational selection, choosing behaviors that either obtain more energy or reduce energy consumption. Thus, this evolution possesses an economic nature.展开更多
Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology.In this study,the CuFe_(2)O_(4)@C/Cd_(0.9)Zn_(0.1)S(CFO@C/CZS)S-scheme photocatalyst with...Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology.In this study,the CuFe_(2)O_(4)@C/Cd_(0.9)Zn_(0.1)S(CFO@C/CZS)S-scheme photocatalyst with photothermal effect was synthesized by ultrasonic self-assembly combined with calcination.The dark CFO@C absorbed visible light and partly converted into heat to promote the hydrogen evolution reaction.The presence of heterojunctions inhibited the photogenerated electron-hole recombination.The graphite-carbon layer provided a stable channel for electron transfer,and the presence of magnetic CFO made recycle easier.Under the action of photothermal assistance and heterojunction,the hydrogen evolution rate of the optimal CFO@C/CZS was 80.79 mmol g^(-1) h^(-1),which was 2.55 times and 260.61 times of that of pure CZS and CFO@C,respectively.Notably,the composite samples also exhibit excellent stability and a wide range of environmental adaptability.Through experimental tests and first-principles simulation calculation methods,the plausible mechanism of photoactivity enhancement was proposed.This work provided a feasible strategy of photothermal assistance for the development of heterojunction photocatalysts with distinctive hydrogen evolution.展开更多
Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy...Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.展开更多
Industrial wastes such as steel slag and coal gangue etc.were chosen as raw materials for preparing ceramic via the conventional solid-state reaction method.With steel slag and coal gangue mixed in various mass ratios...Industrial wastes such as steel slag and coal gangue etc.were chosen as raw materials for preparing ceramic via the conventional solid-state reaction method.With steel slag and coal gangue mixed in various mass ratios,from 100%steel slag to 100%coal gangue at 10%intervals,microstructure and possible phase evolution of the coal gangue-steel slag ceramics were investigated using X-ray powder diffraction,scanning electron microscopy,mercury intrusion porosimetry and Archimedes boiling method.The experimental results suggest that the phase compositions of the as-prepared ceramics could be altered with the increased amount of coal gangue in the ceramics.The anorthite-diopside eutectic can be formed in the ceramics with the mass ratios of steel slag to coal gangue arranged from 8:2 to 2:8,which was responsible for the melting of the steel slag-coal gangue ceramics at relatively high temperature.Further investigations on the microstructure suggested that the addition of the proper amount of steel slag in ceramic compositions was conducive to the pore formation and further contributed to an increment in porosity.展开更多
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金the National Natural Science Foundation of China(Grant No.12102050)the Open Fund of State Key Laboratory of Explosion Science and Technology(Grant No.SKLEST-ZZ-21-18).
文摘The majority of the projectiles used in the hypersonic penetration study are solid flat-nosed cylindrical projectiles with a diameter of less than 20 mm.This study aims to fill the gap in the experimental and analytical study of the evolution of the nose shape of larger hollow projectiles under hypersonic penetration.In the hypersonic penetration test,eight ogive-nose AerMet100 steel projectiles with a diameter of 40 mm were launched to hit concrete targets with impact velocities that ranged from 1351 to 1877 m/s.Severe erosion of the projectiles was observed during high-speed penetration of heterogeneous targets,and apparent localized mushrooming occurred in the front nose of recovered projectiles.By examining the damage to projectiles,a linear relationship was found between the relative length reduction rate and the initial kinetic energy of projectiles in different penetration tests.Furthermore,microscopic analysis revealed the forming mechanism of the localized mushrooming phenomenon for eroding penetration,i.e.,material spall erosion abrasion mechanism,material flow and redistribution abrasion mechanism and localized radial upsetting deformation mechanism.Finally,a model of highspeed penetration that included erosion was established on the basis of a model of the evolution of the projectile nose that considers radial upsetting;the model was validated by test data from the literature and the present study.Depending upon the impact velocity,v0,the projectile nose may behave as undistorted,radially distorted or hemispherical.Due to the effects of abrasion of the projectile and enhancement of radial upsetting on the duration and amplitude of the secondary rising segment in the pulse shape of projectile deceleration,the predicted DOP had an upper limit.
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
基金This work was financially supported by the National Science and Technology Major Project of China(No.J2019-VI-0006-0120)the National Key R&D Program of China(No.2021YFB3700402)the National Natural Science Foundation of China(Nos.52074092 and 52274330).
文摘We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resolution transmission electron microscopy(HRTEM),and electron backscatter diffraction(EBSD).The findings reveal that annealing processing has a significant impact on diminishing residual stresses.As the annealing temperature rose from 950 to 1150℃,the majority of the residual stresses were relieved from 60.1 MPa down to 10.9 MPa.Moreover,the stress relaxation mechanism transitioned from being mainly controlled by dislocation slip to a combination of dislocation slip and grain boundary migration.Meanwhile,the annealing treatment promotes the decomposition of the Laves,accompanied by the precipitation ofμ-(Mo_(6)Co_(7))starting at 950℃ and reaching a maximum value at 1050℃.The tensile strength and plasticity of the annealing alloy at 1150℃ reached the maximum(1394 MPa,56.1%)which was 131%,200%fold than those of the as-cast alloy(1060 MPa,26.6%),but the oxidation process in the alloy was accelerated at 1150℃.The enhancement in durability and flexibility is primarily due to the dissolution of the brittle phase,along with the shape and dispersal of theγ′phase.
基金the staff at Beamline (BL08U1-A and BL11B)of the Shanghai Synchrotron Radiation Facility (SSRF)the support from the National Key Research&Development Program of China (2022YFB3803700)+2 种基金the National Natural Science Foundation of China (52171186)the support through the Overseas Outstanding Youth Fund and Shanghai Pujiang Talent Project (21PJ1408500)the financial support from the Center of Hydrogen Science,Shanghai Jiao Tong University。
文摘High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.
基金We acknowledge the funding support from the National Natural Science Foundation of China Youth Fund(Grant No.52004019)the National Natural Science Foundation of China(Grant No.41825018)China Postdoctoral Science Foundation(Grant No.2023M733481).
文摘Rock-encased-backfill(RB)structures are common in underground mining,for example in the cut-andfill and stoping methods.To understand the effects of cyclic excavation and blasting activities on the damage of these RB structures,a series of triaxial stepwise-increasing-amplitude cyclic loading experiments was conducted with cylindrical RB specimens(rock on outside,backfill on inside)with different volume fractions of rock(VF=0.48,0.61,0.73,and 0.84),confining pressures(0,6,9,and 12 MPa),and cyclic loading rates(200,300,400,and 500 N/s).The damage evolution and meso-crack formation during the cyclic tests were analyzed with results from stress-strain hysteresis loops,acoustic emission events,and post-failure X-ray 3D fracture morphology.The results showed significant differences between cyclic and monotonic loadings of RB specimens,particularly with regard to the generation of shear microcracks,the development of stress memory and strain hardening,and the contact forces and associated friction that develops along the rock-backfill interface.One important finding is that as a function of the number of cycles,the elastic strain increases linearly and the dissipated energy increases exponentially.Also,compared with monotonic loading,the cyclic strain hardening characteristics are more sensitive to rising confining pressures during the initial compaction stage.Another finding is that compared with monotonic loading,more shear microcracks are generated during every reloading stage,but these microcracks tend to be dispersed and lessen the likelihood of large shear fracture formation.The transition from elastic to plastic behavior varies depending on the parameters of each test(confinement,volume fraction,and cyclic rate),and an interesting finding was that the transformation to plastic behavior is significantly lower under the conditions of 0.73 rock volume fraction,400 N/s cyclic loading rate,and 9 MPa confinement.All the findings have important practical implications on the ability of backfill to support underground excavations.
基金supported by grants from the 2030 Science and Technology Innovation Key Program of Ministry of Science and Technology of China(No.2022ZD020910001)the Natural Science Foundation of Shanghai(No.21ZR1428600)the Medical-Engineering Cross Foundation of Shanghai Jiao Tong University(No.YG2022ZD026,21Z510902252,23X010302269).
文摘Background The role of human lineage mutations(HLMs)in human evolution through post-transcriptional modification is unclear.Aims To investigate the contribution of HLMs to human evolution through post-transcriptional modification.Methods We applied a deep learning model Seqweaver to predict how HLMs impact RNA-binding protein affinity.Results We found that only 0.27%of HLMs had significant impacts on RNA-binding proteins at the threshold of the top 1%of human common variations.These HLMs enriched in a set of conserved genes highly expressed in adult excitatory neurons and prenatal Purkinje neurons,and were involved in synapse organisation and the GTPase pathway.These genes also carried excess damaging coding mutations that caused neurodevelopmental disorders,ataxia and schizophrenia.Among these genes,NTRK2 and ITPR1 had the most aggregated evidence of functional importance,suggesting their essential roles in cognition and bipedalism.Conclusions Our findings suggest that a small subset of human-specific mutations have contributed to human speciation through impacts on post-transcriptional modification of critical brain-related genes.
文摘The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.
基金The authors thank the project of Remote Sensing Data and Related Parameters Processing in Southwest China(Project No.612106241)the project of Urban Remote Sensing Data Processing and Multi-Source Integration in Central China(Project No.111/611508101).
文摘With economic development and urbanization in China,the rural settlements have experienced great change.To explore the evolution process of rural settlements in terms of land,population and industry can reveal the development law of rural spatial distribution,population structure and industrial economy in different stages and regions.Studying the development status and evolution characteristics of villages in the upper Tuojiang River basin in Southwest China in the past 20 years are of significant value.The upper Tuojiang River basin includes the main types of terrain found in the Southwest region:mountainous,plains,and hills,exhibiting a certain typicality of geographical characteristics.This study took towns and townships at the town-level scale as the basic unit of research,and constructed an evaluation system for village evolution based on'land,population,and industry'.It employed Criteria Importance Through Inter-Criteria Correlation(CRITIC)analysis to examine the characteristics of village evolution in the area from 2000 to 2020,and used geographic detector analysis to identify the leading factors affecting village evolution.The results show that:(1)From 2000 to 2010,villages in the upper Tuojiang River basin experienced significant changes,and the pace of these transformations slowed from 2010 to 2020.(2)From a comprehensive perspective,from 2000 to 2020,villages in hilly areas show a decline,while villages in plain areas near the city center show a positive urbanization development.(3)Road accessibility and distance from the city center are the main factors that explain the spatial differentiation of village evolution degree in the study area.This study elucidates the spatiotemporal evolution characteristics of villages in the upper Tuojiang River basin and identifies the primary factors contributing to their changes,which will provide a reference for investigating the development of rural areas in different terrains of Southwest China.
基金financially supported by the Agricultural Science and Technology Innovation Program(CAASASTIP-2021-RIP-02)。
文摘Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.
基金This work was supported by the National Key R&D Program of China[2022YFE0110400]the National Natural Science Foundation of China[52122207,52173245,U20A20337,52130206,and 52221006]the Fundamental Research Funds for the Central Universities[CLYY2022].
文摘Developing highly stable and efficient catalysts for oxygen evolution reaction(OER)is extremely important to sustainable energy conversion and storage,but improved efficiency is largely hindered by sluggish reaction kinetics.Dense and bimetal ruthenates have emerged as one of the promising substitutes to replace single-metal ruthenium or iridium oxides,but the fundamental understanding the role of A-site cations is still blurring.Herein,a family of lanthanides(Ln=all the lanthanides except Pm)are applied to synthesize pyrochlore lanthanide ruthenates(Ln_(2)Ru_(2)O_(7)),and only Ln_(2)Ru_(2)O_(7)(Ln=Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,or Lu)with pure phase can be obtained by the ambient-pressure calcination.Compared with the perovskite ruthenates(SrRuO_(3))and rutile RuO_(2),the[RuO_(6)]units in these Ln_(2)Ru_(2)O_(7) present the largely distorted configurations and different energy level splitting to prevent the excessive Ru oxidation and dissolution,which leads the primary improvement in the electrocatalytic OER performance.In the similar crystalline field split states,the charge transfer between[RuO6]units and Ln^(3+)cations also affect catalytic activities,even in the Ln_(2)Ru_(2)O_(7) surface reconstruction during the OER process.Consequently,Tb_(2)Ru_(2)O_(7) showed the highest OER performance among all the prepared Ln_(2)Ru_(2)O_(7) with similar morphologies and crystallization.This systematic work gives fundamental cognition to rational design of high-performance OER electrocatalysts in proper water electrolysis technologies.
基金supported by the National Natural Science Foundation(61833003,62125302,U1908218).
文摘Ingredient optimization plays a pivotal role in the copper industry,for which it is closely related to the concentrate utilization rate,stability of furnace conditions,and the quality of copper production.To acquire a practical ingredient plan,which should exhibit long duration time with sufficient utilization and feeding stability for real applications,an ingredient plan optimization model is proposed in this study to effectively guarantee continuous production and stable furnace conditions.To address the complex challenges posed by this integer programming model,including multiple coupling feeding stages,intricate constraints,and significant non-linearity,a multi-stage differential-multifactorial evolution algorithm is developed.In the proposed algorithm,the differential evolutionary(DE)algorithm is improved in three aspects to efficiently tackle challenges when optimizing the proposed model.First,unlike traditional time-consuming serial approaches,the multifactorial evolutionary algorithm is utilized to optimize multiple complex models contained in the population of evolutionary algorithm caused by the feeding stability in a parallel manner.Second,a repair algorithm is employed to adjust infeasible ingredient lists in a timely manner.In addition,a local search strategy taking feedback from the current optima and considering the different positions of global optimum is developed to avoiding premature convergence of the differential evolutionary algorithm.Finally,the simulation experiments considering different planning horizons using real data from the copper industry in China are conducted,which demonstrates the superiority of the proposed method on feeding duration and stability compared with other commonly deployed approaches.It is practically helpful for reducing material cost as well as increasing production profit for the copper industry.
基金supported by the National Natural Science Foundation of China(Grant No.42061035)the Guizhou Provincial Program on Commercialization of Scientific and Technological Achievements([2022]010).
文摘With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.
基金financial support from the National Natural Science Foundation of China(21875224 and22179121)Knowledge Innovation Program of Wuhan-Basic Research(2022010801010202)Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202201)。
文摘Developing highly active oxygen evolution reaction(OER)electrocatalysts with robust durability is essential in producing high-purity hydrogen through water electrolysis.Layered double hydroxide(LDH)based catalysts have demonstrated efficient catalytic performance toward the relatively sluggish OER.By considering the promotion effect of phosphate(Pi)on proton transfer,herein,a facile phosphate acid(PA)surface-neutralization strategy is developed to in-situ construct NiCo-LDH/NiCoPi hetero-sheets toward OER catalysis.OER activity of NiCoLDH is significantly boosted due to the proton promotion effect and the electronic modulation effect of NiCoPi.As a result,the facilely prepared NiCo-LDH/NiCoPi catalyst displays superior OER catalytic activity with a low overpotential of 300 mV to deliver 100 mA cm^(-2)OER and a Tafel slope of 73 mV dec^(-1).Furthermore,no visible activity decay is detected after a 200-h continuous OER operation.The present work,therefore,provides a promising strategy to exploit robust OER electrocatalysts for commercial water electrolysers.
基金National Natural Science Foundation of China(Grant Nos.52174080 and 51974160)Science Foundation of Tiandi Technology Co.,Ltd.(2022-2-TD-ZD016).
文摘During the mining process of impact-prone coal seams,drilling pressure relief can reduce the impact propensity of the coal seam,but it also reduces the integrity and strength of the coal mass at the side of the roadway.Therefore,studying the mechanical properties and energy evolution rules of coal samples containing holes and filled structures has certain practical significance for achieving coordinated control of coal mine rockburst disasters and the stability of roadway surrounding rocks.To achieve this aim,seven types of burst-prone coal samples were prepared and subject to uniaxial compression experiments with the aid of a TAW-3000 electro-hydraulic servo testing machine.Besides,the stress–strain curves,acoustic emission signals,DIC strain fields and other data were collected during the experiments.Furthermore,the failure modes and energy evolutions of samples with varying drilled hole sizes and filling materials were analyzed.The results show that the indexes related to burst propensity of the drilled coal samples decline to some extent compared with those of the intact one,and the decline is positively corelated to the diameter of the drilled hole.After hole filling,the strain concentration degree around the drilled hole is lowered to a certain degree,and polyurethane filling has a more remarkable effect than cement filling.Meanwhile,hole filling can enhance the strength and deformation resistance of coal.Hole drilling can accelerate the release of accumulated elastic strain energy,turning the acoustic emission events from low-frequency and high-energy ones to high-frequency and low-energy ones,whereas hole filling can reduce the intensity of energy release.The experimental results and theoretical derivation demonstrate that hole filling promotes coal deformability and strength mainly by weakening stress concentration surrounding the drilled holes.Moreover,the fillings can achieve a better filling effect if their elastic modulus and Poisson’s ratio are closer to those of the coal body.
基金the financial support from the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFB4002000,2022YFA1203400)the National Natural Science Foundation of China(22102172,22072145,22372155,22005294,21925205,21721003)。
文摘Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.
文摘This article employs a combined approach of biology and economics to reveal that biological evolution has an economic nature, evolving towards improved energy efficiency. The orthodox Darwinian theory of evolution describes evolution as the random variation of organisms and their survival through natural selection. In fact, the natural environment itself is a constantly changing context, and the strategy to adapt to this change is to enhance behavioral capabilities, thereby expanding the range and dimensions of behavior. Therefore, the improvement of behavioral capabilities is an important aspect of evolution. The enhancement of behavioral capabilities expands the range of adaptation to the natural environment and increases the space for behavioral choices. Within this space of behavioral choices, some options are more effective and superior to others;thus, the ability to select is necessary to make the improved behavioral capabilities more beneficial to the organism itself. The birth and development of the brain serve the purpose of selection. By using the brain to make selections, at least the “better” behavior will be chosen between two alternatives. Once the better behavior yields better results, and the organism can associate these results with the corresponding behavior, it will persist in this behavior. The persistent repetition of a behavior over generations will form a habit. Habits passed down through generations constitute a new environment, causing the organism’s genes to activate or deactivate certain functions, ultimately leading to genetic changes that are beneficial to that habit. Since the brain’s selection represents the organism’s self-selection, it differs from random variation;it is also a rational selection, choosing behaviors that either obtain more energy or reduce energy consumption. Thus, this evolution possesses an economic nature.
基金supported by the Shandong Provincial Natural Science Foundation(ZR2022ME179,ZR2021QE086)the Shandong Provincial Key Research and Development Program(Public Welfare Science and Technology Research)(2019GGX103010)+2 种基金the Science and Technology Planning Project of Higher School in Shandong Province(J18KA243)the Liaocheng Key Research and Development Program(Policy guidance category)(2022YDSF90)the Liaocheng University High-level Talents&PhD Research Startup Foundation(318051619)。
文摘Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology.In this study,the CuFe_(2)O_(4)@C/Cd_(0.9)Zn_(0.1)S(CFO@C/CZS)S-scheme photocatalyst with photothermal effect was synthesized by ultrasonic self-assembly combined with calcination.The dark CFO@C absorbed visible light and partly converted into heat to promote the hydrogen evolution reaction.The presence of heterojunctions inhibited the photogenerated electron-hole recombination.The graphite-carbon layer provided a stable channel for electron transfer,and the presence of magnetic CFO made recycle easier.Under the action of photothermal assistance and heterojunction,the hydrogen evolution rate of the optimal CFO@C/CZS was 80.79 mmol g^(-1) h^(-1),which was 2.55 times and 260.61 times of that of pure CZS and CFO@C,respectively.Notably,the composite samples also exhibit excellent stability and a wide range of environmental adaptability.Through experimental tests and first-principles simulation calculation methods,the plausible mechanism of photoactivity enhancement was proposed.This work provided a feasible strategy of photothermal assistance for the development of heterojunction photocatalysts with distinctive hydrogen evolution.
基金supported by the National Natural Sci-ence Foundation of China(22272081),Jiangsu Provincial Specially Appointed Professors Foundation.
文摘Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.
基金Funded by the Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province(No.BE2022028-4)。
文摘Industrial wastes such as steel slag and coal gangue etc.were chosen as raw materials for preparing ceramic via the conventional solid-state reaction method.With steel slag and coal gangue mixed in various mass ratios,from 100%steel slag to 100%coal gangue at 10%intervals,microstructure and possible phase evolution of the coal gangue-steel slag ceramics were investigated using X-ray powder diffraction,scanning electron microscopy,mercury intrusion porosimetry and Archimedes boiling method.The experimental results suggest that the phase compositions of the as-prepared ceramics could be altered with the increased amount of coal gangue in the ceramics.The anorthite-diopside eutectic can be formed in the ceramics with the mass ratios of steel slag to coal gangue arranged from 8:2 to 2:8,which was responsible for the melting of the steel slag-coal gangue ceramics at relatively high temperature.Further investigations on the microstructure suggested that the addition of the proper amount of steel slag in ceramic compositions was conducive to the pore formation and further contributed to an increment in porosity.