What system should a multinational state adopt to resolve ethnic minority problems and ensure the rights of minorities? This is a major problem that has to be settled. There are roughly three options: confederacy, aut...What system should a multinational state adopt to resolve ethnic minority problems and ensure the rights of minorities? This is a major problem that has to be settled. There are roughly three options: confederacy, autonomy and power sharing. The former Soviet Union adopted the form of confederacy. That was determined by the fact that during the October Revolution, many ethnic groups were in a state of entire separation and isolation. In his speech in 1989, Chinese leader Deng Xiaoping said: We owe the stable and united situation in the areas inhabited by ethnic minorities to Chairman展开更多
Taking the Paleozoic of the Sichuan and Tarim basins in China as example,the controlling effects of the Earth system evolution and multi-spherical interactions on the formation and enrichment of marine ultra-deep petr...Taking the Paleozoic of the Sichuan and Tarim basins in China as example,the controlling effects of the Earth system evolution and multi-spherical interactions on the formation and enrichment of marine ultra-deep petroleum in China have been elaborated.By discussing the development of“source-reservoir-seal”controlled by the breakup and assembly of supercontinents and regional tectonic movements,and the mechanisms of petroleum generation and accumulation controlled by temperature-pressure system and fault conduit system,Both the South China and Tarim blocks passed through the intertropical convergence zone(ITCZ)of the low-latitude Hadley Cell twice during their drifts,and formed hydrocarbon source rocks with high quality.It is proposed that deep tectonic activities and surface climate evolution jointly controlled the types and stratigraphic positions of ultra-deep hydrocarbon source rocks,reservoirs,and seals in the Sichuan and Tarim basins,forming multiple petroleum systems in the Ediacaran-Cambrian,Cambrian-Ordovician,Cambrian-Permian and Permian-Triassic strata.The matching degree of source-reservoir-seal,the type of organic matter in source rocks,the deep thermal regime of basin,and the burial-uplift process across tectonic periods collectively control the entire process from the generation to the accumulation of oil and gas.Three types of oil and gas enrichment models are formed,including near-source accumulation in platform marginal zones,distant-source accumulation in high-energy beaches through faults,and three-dimensional accumulation in strike-slip fault zones,which ultimately result in the multi-layered natural gas enrichment in ultra-deep layers of the Sichuan Basin and co-enrichment of oil and gas in the ultra-deep layers of the Tarim Basin.展开更多
The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the micro...The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was investigated.Furthermore,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric method.The findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and interconnect.This provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron coke.Accelerating the heating rate in non-isothermal gasification can enhance the reactivity of iron coke.The metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon atoms.The kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore structure.Moreover,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.展开更多
The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional ...The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.展开更多
The influence of thermal damage on macroscopic and microscopic characteristics of different rocks has received much attention in the field of rock engineering.When the rocks are subjected to thermal treatment,the chan...The influence of thermal damage on macroscopic and microscopic characteristics of different rocks has received much attention in the field of rock engineering.When the rocks are subjected to thermal treatment,the change of macroscopic characteristics and evolution of micro-structure would be induced,ultimately resulting in different degrees of thermal damage in rocks.To better understand the thermal damage mechanism of different rocks and its effect on the rock performance,this study reviews a large number of test results of rock specimens experiencing heating and cooling treatment in the laboratory.Firstly,the variations of macroscopic behaviors,including physical parameters,mechanical parameters,thermal conductivity and permeability,are examined.The variations of mechanical parameters with thermal treatment variables(i.e.temperature or the number of thermal cycles)are divided into four types.Secondly,several measuring methods for microstructure,such as polarizing microscopy,fluorescent method,scanning electron microscopy(SEM),X-ray computerized tomography(CT),acoustic emission(AE)and ultrasonic technique,are introduced.Furthermore,the effect of thermal damage on the mechanical parameters of rocks in response to different thermal treatments,involving temperature magnitude,cooling method and thermal cycle,are discussed.Finally,the limitations and prospects for the research of rock thermal damage are proposed.展开更多
Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-gr...Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.展开更多
The continental Asia is mainly composed of three major tectonic regimes,the Tethys,Paleo Asian Ocean,and West Pacific.It underwent multi-stage plate convergences,ocean-continent transformations,and subductions,collisi...The continental Asia is mainly composed of three major tectonic regimes,the Tethys,Paleo Asian Ocean,and West Pacific.It underwent multi-stage plate convergences,ocean-continent transformations,and subductions,collisions and/or collages,and post collisional(orogenic)extensions in Phanerozoic.Tectonic evolution of the Asia brings up a unique fault system and tectonic geomorphological features in the China's Mainland.Also,it provides a geodynamic background for the formation and evolution of metallogeneses and mineral systems,resulting in nonuniform distribution of tectono-metallogenic systems and metallogenic belts.The spatiotemporal distribution of mineral deposits in China and adjacent areas exhibits periodic variation under controlling of the full life Wilson cycle and tectonic evolution,forming the plate convergence-related mineral system in East Asia.Porphyry Cu deposits are mainly related to compressional systems in Paleozoic and early Mesozoic,and more closely related to post-collision extensional settings in late Mesozoic and Cenozoic.Orogenic Au deposits mainly formed in post-orogeny extensional setting.Alkaline rock related rare earth element deposits formed mainly at margins of the North China and Yangtze cratons.Granite-pegmatite Li and other rare metal deposits formed mainly in early Mesozoic,related to Indosinian post-orogeny extension.Tectono-metallogenic systems provide important basis for the prospecting of mineral resources.展开更多
Black shales are important products of material cycling and energy exchange among the lithosphere,atmosphere,hydrosphere,and biosphere.They are widely distributed throughout geological history and provide essential en...Black shales are important products of material cycling and energy exchange among the lithosphere,atmosphere,hydrosphere,and biosphere.They are widely distributed throughout geological history and provide essential energy and mineral resources for the development of human society.They also record the evolution process of the earth and improve the understanding of the earth.This review focuses on the diagenesis and formation mechanisms of black shales sedimentation,composition,evolution,and reconstruction,which have had a significant impact on the formation and enrichment of shale oil and gas.In terms of sedimentary environment,black shales can be classified into three types:Marine,terrestrial,and marine-terrestrial transitional facies.The formation processes include mechanisms such as eolian input,hypopycnal flow,gravity-driven and offshore bottom currents.From a geological perspective,the formation of black shales is often closely related to global or regional major geological events.The enrichment of organic matter is generally the result of the interaction and coupling of several factors such as primary productivity,water redox condition,and sedimentation rate.In terms of evolution,black shales have undergone diagenetic evolution of inorganic minerals,thermal evolution of organic matter and hydrocarbon generation,interactions between organic matter and inorganic minerals,and pore evolution.In terms of reconstruction,the effects of fold deformation,uplift and erosion,and fracturing have changed the stress state of black shale reservoirs,thereby having a significant impact on the pore structure.Fluid activity promotes the formation of veins,and have changed the material composition,stress structure,and reservoir properties of black shales.Regarding resource effects,the deposition of black shales is fundamental for shale oil and gas resources,the evolution of black shales promotes the shale oil and gas formation and storage,and the reconstruction of black shales would have caused the heterogeneous distribution of oil and gas in shales.Exploring the formation mechanisms and interactions of black shales at different scales is a key to in-depth research on shale formation and evolution,as well as the key to revealing the mechanism controlling shale oil and gas accumulation.The present records can reveal how these processes worked in geological history,and improve our understanding of the coupling mechanisms among regional geological events,black shales evolution,and shale oil and gas formation and enrichment.展开更多
Wampee(Clausena lansium)is an important evergreen fruit tree native to southern China that has a long history of use for medicinal purposes.Here,a chromosome-level genome of C.lansium was constructed with a genome siz...Wampee(Clausena lansium)is an important evergreen fruit tree native to southern China that has a long history of use for medicinal purposes.Here,a chromosome-level genome of C.lansium was constructed with a genome size of 282.9 Mb and scaffold N50 of 30.75 Mb.The assembled genome contains 48.70%repetitive elements and 24,381 protein-coding genes.Comparative genomic analysis showed that C.lansium diverged from Aurantioideae 15.91-24.95 million years ago.Additionally,some expansive and specific gene families related to methyltransferase activity and S-adenosylmethionine-dependent methyltransferase activity were also identified.Further analysis indicated that N-methyltransferase(NMT)is mainly involved in alkaloid biosynthesis and O-methyltransferase(OMT)participates in the regulation of coumarin accumulation in wampee.This suggested that wampee's richness in alkaloids and coumarins might be due to the gene expansions of NMT and OMT.The tandem repeat event was one of the major reasons for the NMT expansion.Hence,the reference genome of C.lansium will facilitate the identification of some useful medicinal compounds from wampee resources and reveal their biosynthetic pathways.展开更多
Accurate measurement of the evolution of rock joint void geometry is essential for comprehending the distribution characteristics of asperities responsible for shear and seepage behaviors.However,existing techniques o...Accurate measurement of the evolution of rock joint void geometry is essential for comprehending the distribution characteristics of asperities responsible for shear and seepage behaviors.However,existing techniques often require specialized equipment and skilled operators,posing practical challenges.In this study,a cost-effective photogrammetric approach is proposed.Particularly,local coordinate systems are established to facilitate the alignment and precise quantification of the relative position between two halves of a rock joint.Push/pull tests are conducted on rock joints with varying roughness levels to induce different contact states.A high-precision laser scanner serves as a benchmark for evaluating the photogrammetry method.Despite certain deviations exist,the measured evolution of void geometry is generally consistent with the qualitative findings of previous studies.The photogrammetric measurements yield comparable accuracy to laser scanning,with maximum errors of 13.2%for aperture and 14.4%for void volume.Most joint matching coefficient(JMC)measurement errors are below 20%.Larger measurement errors occur primarily in highly mismatched rock joints with JMC values below 0.2,but even in cases where measurement errors exceed 80%,the maximum JMC error is only 0.0434.Thus,the proposed photogrammetric approach holds promise for widespread application in void geometry measurements in rock joints.展开更多
The Upper Cretaceous Qingshankou Formation black shales,deposited in the late Turonian(LTB shales),are the main source rocks of the Songliao Basin.The origins of organic matter enrichment of the shales is a contentiou...The Upper Cretaceous Qingshankou Formation black shales,deposited in the late Turonian(LTB shales),are the main source rocks of the Songliao Basin.The origins of organic matter enrichment of the shales is a contentious subject fuelling many ongoing debates.This study investigates the genesis of the organic matter-rich shale by using molecular geochemistry.The LTB shales can be divided into three sections.The SectionⅠshales were deposited in saline,stratified and anoxic water conditions,which are related to seawater incursion events.At least three episodic and periodic seawater incursion events were recognized during SectionⅠshale deposition.The SectionⅡshales deposited in brackish to fresh and deep lake-level conditions with high primary productivity,which are related to lake-level transgression.The SectionⅢshales were deposited under fresh and slightly oxidized water conditions,which are related to lake-level regression.Two organic matter enrichment models for the LTB shales are identified,that is,the seawater incursion model and the maximum lake-level transgression sedimentation model,which act on different shale sections,both playing significant roles in the enrichment of organic matter.展开更多
Gypsum caprocks'sealing ability is affected by temperature-pressure coupling.Due to the limitations of experimental conditions,there is still a lack of triaxial stress-strain experiments that simultaneously consid...Gypsum caprocks'sealing ability is affected by temperature-pressure coupling.Due to the limitations of experimental conditions,there is still a lack of triaxial stress-strain experiments that simultaneously consider changes in temperature and pressure conditions,which limits the accuracy of the comprehensive evaluation of the brittle plastic evolution and sealing ability of gypsum rocks using temperature pressure coupling.Triaxial stress-strain tests were utilized to investigate the differences in the evolution of the confinement capacity of gypsum rocks under coupled temperaturepressure action and isothermal-variable pressure action on the basis of sample feasibility analysis.According to research,the gypsum rock's peak and residual strengths decrease under simultaneous increases in temperature and pressure over isothermal pressurization experimental conditions,and it becomes more ductile.This reduces the amount of time it takes for the rock to transition from brittle to plastic.When temperature is taken into account,both the brittle–plastic transformation's depth limit and the lithological transformation of gypsum rocks become shallower,and the evolution of gypsum rocks under variable temperature and pressure conditions is more complicated than that under isothermal pressurization.The sealing ability under the temperature-pressure coupling is more in line with the actual geological context when the application results of the Well#ZS5 are compared.This provides a theoretical basis for precisely determining the process of hydrocarbon accumulation and explains why the early hydrocarbon were not well preserved.展开更多
The oxygen evolution reaction(OER)is a crucial step in metal-air batteries and water splitting technologies,playing a significant role in the efficiency and achievable heights of these two technologies.However,the OER...The oxygen evolution reaction(OER)is a crucial step in metal-air batteries and water splitting technologies,playing a significant role in the efficiency and achievable heights of these two technologies.However,the OER is a four-step,four-electron reaction,and its slow kinetics result in high overpotentials,posing a challenge.To address this issue,numerous strategies involving modified catalysts have been proposed and proven to be highly efficient.In these strategies,the introduction of strain has been widely reported because it is generally believed to effectively regulate the electronic structure of metal sites and alter the adsorption energy of catalyst surfaces with reaction intermediates.However,strain has many other effects that are not well known,making it an important yet unexplored area.Based on this,this review provides a detailed introduction to the various roles of strain in OER.To better explain these roles,the review also presents the definition of strain and elucidates the potential mechanisms of strain in OER based on the d-band center theory and adsorption volcano plot.Additionally,the review showcases various ways of introducing strain in OER through examples reported in the latest literature,aiming to provide a comprehensive perspective for the development of strain engineering.Finally,the review analyzes the appropriate proportion of strain introduction,compares compressive and tensile strain,and examines the impact of strain on stability.And the review offers prospects for future research directions in this emerging field.展开更多
Based on the petrology,isotope geochemistry and fluid inclusions analysis,we established the evolutionary mode of the diagenetic fluid of dawsonite-bearing sandstone in the Jiyang Depression.Dawsonite-bearing sandston...Based on the petrology,isotope geochemistry and fluid inclusions analysis,we established the evolutionary mode of the diagenetic fluid of dawsonite-bearing sandstone in the Jiyang Depression.Dawsonite-bearing sandstone is characterized by double injection of CO_(2)and oil-gas in the Jiyang Depression that have experienced a relatively complex diagenetic fluid evolution process.The diagenetic sequence of secondary minerals involves secondary enlargement of quartz,kaolinite,first-stage calcite,dawsonite,second-stage calcite,ferrocalcite,dolomite and ankerite.Hydrocarbon charging in the dawsonite-bearing sandstone occurred at around 2.6–0 Myr.The CO_(2)charging event occurred during Dongying tectonism,forming the Pingfangwang CO_(2)gas reservoir,which provided an abundant carbon source for dawsonite precipitation.Carbon and oxygen isotopic compositions of dawsonite demonstrate that CO_(2)forming the dawsonite was of an inorganic origin derived from the mantle,and that water mediating the proc-ess during dawsonite precipitation was sequestered brine with a fluid temperature of 82℃.The evolutionary sequence of the diagenetic fluid in the dawsonite-bearing sandstone was:alkaline syngenetic fluids,weak alkaline fluids during organic acid forma-tion,acidic fluids in the early stage of CO_(2)injection,alkaline fluids in the late stage of CO_(2)injection,and weak alkaline fluids during oil and gas charging.The mode indicates an increase in-HCO_(3)because of the CO_(2)injection,and the loss of Ca^(2+)and Mg^(2+)due to the precipitation of carbonate minerals.Therefore,the evolutionary mode of diagenetic fluids is in good agreement with high HCO_(3)^(-),low Ca^(2+)and low Mg^(2+)composition of the present formation water in the dawsonite-bearing sandstone.展开更多
This study investigates the effects of Fe on the oxygen-evolution reaction(OER)in the presence of Au.Two distinct areas of OER were identified:the first associated with Fe sites at low overpotential(~330 mV),and the s...This study investigates the effects of Fe on the oxygen-evolution reaction(OER)in the presence of Au.Two distinct areas of OER were identified:the first associated with Fe sites at low overpotential(~330 mV),and the second with Au sites at high overpotential(~870 mV).Various factors such as surface Fe concentration,electrochemical method,scan rate,potential range,concentration,method of adding K_(2)Fe O_(4),nature of Fe,and temperature were varied to observe diverse behaviors during OER for Fe O_(x)H_(y)/Au.Trace amounts of Fe ions had a significant impact on OER,reaching a saturation point where the activity did not increase further.Strong electronic interaction between Fe and Au ions was indicated by X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)analyses.In situ visible spectroscopy confirmed the formation of Fe O_(4)^(2-)during OER.In situ Mossbauer and surfaceenhanced Raman spectroscopy(SERS)analyses suggest the involvement of Fe-based species as intermediates during the rate-determining step of OER.A lattice OER mechanism based on Fe O_(x)H_(y)was proposed for operation at low overpotentials.Density functional theory(DFT)calculations revealed that Fe oxide,Fe-oxide clusters,and Fe doping on the Au foil exhibited different activities and stabilities during OER.The study provides insights into the interplay between Fe and Au in OER,advancing the understanding of OER mechanisms and offering implications for the design of efficient electrocatalytic systems.展开更多
The Beishan orogen,located in the central segment of the Tianshan–Solonker suture within the southern Central Asian Orogenic Belt(CAOB),is crucial for understanding the accretionary processes and continental growth i...The Beishan orogen,located in the central segment of the Tianshan–Solonker suture within the southern Central Asian Orogenic Belt(CAOB),is crucial for understanding the accretionary processes and continental growth in Central Asia.This orogen developed through the episodic amalgamation and accretion of continental margin arcs,island arcs,ophiolites,and accretionary wedges,undergoing a complex process of accretion and evolution.Since the Phanerozoic,the Beishan orogen has experienced multiple phases of magmatic and collision events.The intricate distribution of magmatic arc rocks has obscured the complete basement traces,and the spatial superposition of multiple magmatic arc phases has complicated the study of its evolutionary history.展开更多
Urban-suburban-rural(U-S-R)zones exhibit distinctive transitional characteristics in interaction between human and nature.U-S-R transition zones(U-S-RTZ)are also highlighting the function diversity and landscape heter...Urban-suburban-rural(U-S-R)zones exhibit distinctive transitional characteristics in interaction between human and nature.U-S-R transition zones(U-S-RTZ)are also highlighting the function diversity and landscape heterogeneity across territorial spaces.As a super megacity in western China,Chengdu’s rapid urbanization has driven the evolution of U-S-R spaces,resulting in a sequential structure.To promote the high-quality spatial development of urban-rural region in a structured and efficient manner,it is essential to con-duct a scientific examination of the multidimensional interconnection within the U-S-RTZ framework.By proposing a novel identifica-tion method of U-S-RTZ and taking Chengdu,China as a case study,grounded in a blender of natural and humanistic factors,this study quantitatively delineated and explored the spatial evolutions of U-S-RTZ and stated the optimization orientation and sustainable devel-opment strategies of the production-living-ecological spaces along the U-S-R gradients.The results show that:1)it is suitable for the quantitative analysis of U-S-RTZ by established three-dimensional identification system in this study.2)In 1990-2020,the urban-sub-urban transition zones(U-STZ)in Chengdu have continuously undergone a substantial increase,and the scale of the suburban-rural transition zones(S-RTZ)has continued to expand slightly,while the space of rural-ecological transition zones(R-ETZ)has noticeably compressed.3)The landuse dynamics within U-S-RTZ has gradually increased in 1990-2020.The main direction of landuse transition was from farmland to construction land or woodlands,with the expansion of construction land being the most significant.4)R-ETZ primarily focus on ecological functions,and there is a trade-off relationship between the production-ecological function within the S-RTZ,and in the U-STZ,production-living composite functions are prioritized.This study emphasizes the importance of elastic planning and precise governance within the U-S-RTZ in a rapid urbanization region,particularly highlighting the role of suburbs as landscape corridors and service hubs in urban-rural integration.It elucidates to the practical implications for achieving high-quality development of integrated U-S-R territorial spaces.展开更多
Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catal...Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER.Herein,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied potentials.Guided by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly.Our work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.展开更多
The experimental results of the reactions between an alkaline basaltic melt and mantle orthopyroxenes under high-temperature and high-pressure conditions of 1300–1400℃ and 2.0–3.0 GPa using a six-anvil apparatus ar...The experimental results of the reactions between an alkaline basaltic melt and mantle orthopyroxenes under high-temperature and high-pressure conditions of 1300–1400℃ and 2.0–3.0 GPa using a six-anvil apparatus are reported in this paper.The reactions are proposed to simulate the interactions between melts from the asthenospheric mantle and the lithospheric mantle.The starting melt in the experiments was made from the alkaline basalt occurring in Fuxin,Liaoning Province,and the orthopyroxenes were separated from the mantle xenoliths in Damaping,Hebei Province.The results show that clinopyroxenes were formed in all the reactions between the alkaline basaltic melt and orthopyroxenes under the studied P–T conditions.The formation of clinopyroxene in the reaction zone is mainly controlled by dissolution–crystallization,and the chemical compositions of the reacted melt are primarily infl uenced by the diff usion eff ect.Temperature is the most important parameter controlling the reactions between the melt and orthopyroxenes,which has a direct impact on the melting of orthopyroxenes and the diff usion of chemical components in the melt.Temperature also directly controls the chemical compositions of the newly formed clinopyroxenes in the reaction zone and the reacted melt.The formation of clinopyroxenes from the reactions between the alkaline basaltic melt and orthopyroxenes can result in an increase of CaO and Al_(2)O_(3) contents in the rocks containing this mineral.Therefore,the reactions between the alkaline basaltic melt from the asthenospheric mantle and orthopyroxenes from the lithospheric mantle can lead to the evolution of lithospheric mantle in the North China Craton from refractory to fertile with relatively high CaO and Al 2 O 3 contents.In addition,the reacted melts in some runs were transformed from the starting alkaline basaltic into tholeiitic after reactions,indicating that tholeiitic magma could be generated from alkaline basaltic one via reactions between the latter and orthopyroxene.展开更多
Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely use...Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER.展开更多
文摘What system should a multinational state adopt to resolve ethnic minority problems and ensure the rights of minorities? This is a major problem that has to be settled. There are roughly three options: confederacy, autonomy and power sharing. The former Soviet Union adopted the form of confederacy. That was determined by the fact that during the October Revolution, many ethnic groups were in a state of entire separation and isolation. In his speech in 1989, Chinese leader Deng Xiaoping said: We owe the stable and united situation in the areas inhabited by ethnic minorities to Chairman
基金Supported by National Key Research and Development Program of China(2017YFC0603101)National Natural Science Foundation of China(42225303,42372162,42102146)+1 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(XDA14010101)Basic and Forward-Looking Major Technology Project of China National Petroleum Corporation(2023ZZ0203)。
文摘Taking the Paleozoic of the Sichuan and Tarim basins in China as example,the controlling effects of the Earth system evolution and multi-spherical interactions on the formation and enrichment of marine ultra-deep petroleum in China have been elaborated.By discussing the development of“source-reservoir-seal”controlled by the breakup and assembly of supercontinents and regional tectonic movements,and the mechanisms of petroleum generation and accumulation controlled by temperature-pressure system and fault conduit system,Both the South China and Tarim blocks passed through the intertropical convergence zone(ITCZ)of the low-latitude Hadley Cell twice during their drifts,and formed hydrocarbon source rocks with high quality.It is proposed that deep tectonic activities and surface climate evolution jointly controlled the types and stratigraphic positions of ultra-deep hydrocarbon source rocks,reservoirs,and seals in the Sichuan and Tarim basins,forming multiple petroleum systems in the Ediacaran-Cambrian,Cambrian-Ordovician,Cambrian-Permian and Permian-Triassic strata.The matching degree of source-reservoir-seal,the type of organic matter in source rocks,the deep thermal regime of basin,and the burial-uplift process across tectonic periods collectively control the entire process from the generation to the accumulation of oil and gas.Three types of oil and gas enrichment models are formed,including near-source accumulation in platform marginal zones,distant-source accumulation in high-energy beaches through faults,and three-dimensional accumulation in strike-slip fault zones,which ultimately result in the multi-layered natural gas enrichment in ultra-deep layers of the Sichuan Basin and co-enrichment of oil and gas in the ultra-deep layers of the Tarim Basin.
基金financially supported by the National Science Foundation of China(Nos.51974212 and 52274316)the China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202116)+1 种基金the Science and Technology Major Project of Wuhan(No.2023020302020572)the Foundation of Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education(No.FMRUlab23-04)。
文摘The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was investigated.Furthermore,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric method.The findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and interconnect.This provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron coke.Accelerating the heating rate in non-isothermal gasification can enhance the reactivity of iron coke.The metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon atoms.The kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore structure.Moreover,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.
基金financial support from the National Natural Science Foundation of China (52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing (STRZ202203)the financial support provided by the China Scholarship Council (CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship,Australia。
文摘The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.
基金supported by the National Key Research and Development Plan(Grant No.2022YFC2905700)Natural Science Foundation of Anhui Province(Grant No.2208085ME120)Key Research and Development Plan of Anhui Province(Grant No.2022m07020001).
文摘The influence of thermal damage on macroscopic and microscopic characteristics of different rocks has received much attention in the field of rock engineering.When the rocks are subjected to thermal treatment,the change of macroscopic characteristics and evolution of micro-structure would be induced,ultimately resulting in different degrees of thermal damage in rocks.To better understand the thermal damage mechanism of different rocks and its effect on the rock performance,this study reviews a large number of test results of rock specimens experiencing heating and cooling treatment in the laboratory.Firstly,the variations of macroscopic behaviors,including physical parameters,mechanical parameters,thermal conductivity and permeability,are examined.The variations of mechanical parameters with thermal treatment variables(i.e.temperature or the number of thermal cycles)are divided into four types.Secondly,several measuring methods for microstructure,such as polarizing microscopy,fluorescent method,scanning electron microscopy(SEM),X-ray computerized tomography(CT),acoustic emission(AE)and ultrasonic technique,are introduced.Furthermore,the effect of thermal damage on the mechanical parameters of rocks in response to different thermal treatments,involving temperature magnitude,cooling method and thermal cycle,are discussed.Finally,the limitations and prospects for the research of rock thermal damage are proposed.
基金supported by the National Natural Science Foundation of China(Grant Nos.22075159,22002066)Shandong Taishan Scholars Project(Grant Nos.ts20190932,tsqn202103058)+1 种基金Open Fund of Hubei Key Laboratory of Processing and Application of Catalytic Materials(Grant No.202203404)Postdoctoral Applied Research Project in Qingdao,and the Youth Innovation Team Project of Shandong Provincial Education Department(Grant No.2019KJC023).
文摘Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.
基金funded by the Deep Geological Survey Project of the China Geological Survey(Grant Nos.DD20230229,DD20230008,DD20160083 and DD20190011)the DREAM―Deep Resource Exploration and Advanced Mining of the National Key Research and Development Program of China(Grant No.2018YFC0603701)。
文摘The continental Asia is mainly composed of three major tectonic regimes,the Tethys,Paleo Asian Ocean,and West Pacific.It underwent multi-stage plate convergences,ocean-continent transformations,and subductions,collisions and/or collages,and post collisional(orogenic)extensions in Phanerozoic.Tectonic evolution of the Asia brings up a unique fault system and tectonic geomorphological features in the China's Mainland.Also,it provides a geodynamic background for the formation and evolution of metallogeneses and mineral systems,resulting in nonuniform distribution of tectono-metallogenic systems and metallogenic belts.The spatiotemporal distribution of mineral deposits in China and adjacent areas exhibits periodic variation under controlling of the full life Wilson cycle and tectonic evolution,forming the plate convergence-related mineral system in East Asia.Porphyry Cu deposits are mainly related to compressional systems in Paleozoic and early Mesozoic,and more closely related to post-collision extensional settings in late Mesozoic and Cenozoic.Orogenic Au deposits mainly formed in post-orogeny extensional setting.Alkaline rock related rare earth element deposits formed mainly at margins of the North China and Yangtze cratons.Granite-pegmatite Li and other rare metal deposits formed mainly in early Mesozoic,related to Indosinian post-orogeny extension.Tectono-metallogenic systems provide important basis for the prospecting of mineral resources.
基金supported by the projects of the China Geological Survey(DD20230043,DD20240048)the project of the National Natural Science Foundation of China(42102123)。
文摘Black shales are important products of material cycling and energy exchange among the lithosphere,atmosphere,hydrosphere,and biosphere.They are widely distributed throughout geological history and provide essential energy and mineral resources for the development of human society.They also record the evolution process of the earth and improve the understanding of the earth.This review focuses on the diagenesis and formation mechanisms of black shales sedimentation,composition,evolution,and reconstruction,which have had a significant impact on the formation and enrichment of shale oil and gas.In terms of sedimentary environment,black shales can be classified into three types:Marine,terrestrial,and marine-terrestrial transitional facies.The formation processes include mechanisms such as eolian input,hypopycnal flow,gravity-driven and offshore bottom currents.From a geological perspective,the formation of black shales is often closely related to global or regional major geological events.The enrichment of organic matter is generally the result of the interaction and coupling of several factors such as primary productivity,water redox condition,and sedimentation rate.In terms of evolution,black shales have undergone diagenetic evolution of inorganic minerals,thermal evolution of organic matter and hydrocarbon generation,interactions between organic matter and inorganic minerals,and pore evolution.In terms of reconstruction,the effects of fold deformation,uplift and erosion,and fracturing have changed the stress state of black shale reservoirs,thereby having a significant impact on the pore structure.Fluid activity promotes the formation of veins,and have changed the material composition,stress structure,and reservoir properties of black shales.Regarding resource effects,the deposition of black shales is fundamental for shale oil and gas resources,the evolution of black shales promotes the shale oil and gas formation and storage,and the reconstruction of black shales would have caused the heterogeneous distribution of oil and gas in shales.Exploring the formation mechanisms and interactions of black shales at different scales is a key to in-depth research on shale formation and evolution,as well as the key to revealing the mechanism controlling shale oil and gas accumulation.The present records can reveal how these processes worked in geological history,and improve our understanding of the coupling mechanisms among regional geological events,black shales evolution,and shale oil and gas formation and enrichment.
基金supported by the Central Public-interest Scientific Institution Basal Research Fund for the Chinese Academy of Tropical Agricultural Sciences(1630062019010 and 1630062020010)the Fund of Protection of Species Resources for the Ministry of Agriculture and Rural Affairs of China(125A0605)。
文摘Wampee(Clausena lansium)is an important evergreen fruit tree native to southern China that has a long history of use for medicinal purposes.Here,a chromosome-level genome of C.lansium was constructed with a genome size of 282.9 Mb and scaffold N50 of 30.75 Mb.The assembled genome contains 48.70%repetitive elements and 24,381 protein-coding genes.Comparative genomic analysis showed that C.lansium diverged from Aurantioideae 15.91-24.95 million years ago.Additionally,some expansive and specific gene families related to methyltransferase activity and S-adenosylmethionine-dependent methyltransferase activity were also identified.Further analysis indicated that N-methyltransferase(NMT)is mainly involved in alkaloid biosynthesis and O-methyltransferase(OMT)participates in the regulation of coumarin accumulation in wampee.This suggested that wampee's richness in alkaloids and coumarins might be due to the gene expansions of NMT and OMT.The tandem repeat event was one of the major reasons for the NMT expansion.Hence,the reference genome of C.lansium will facilitate the identification of some useful medicinal compounds from wampee resources and reveal their biosynthetic pathways.
基金supported by the National Natural Science Foundation of China (Nos.42207175 and 42177117)the Ningbo Natural Science Foundation (No.2022J115)。
文摘Accurate measurement of the evolution of rock joint void geometry is essential for comprehending the distribution characteristics of asperities responsible for shear and seepage behaviors.However,existing techniques often require specialized equipment and skilled operators,posing practical challenges.In this study,a cost-effective photogrammetric approach is proposed.Particularly,local coordinate systems are established to facilitate the alignment and precise quantification of the relative position between two halves of a rock joint.Push/pull tests are conducted on rock joints with varying roughness levels to induce different contact states.A high-precision laser scanner serves as a benchmark for evaluating the photogrammetry method.Despite certain deviations exist,the measured evolution of void geometry is generally consistent with the qualitative findings of previous studies.The photogrammetric measurements yield comparable accuracy to laser scanning,with maximum errors of 13.2%for aperture and 14.4%for void volume.Most joint matching coefficient(JMC)measurement errors are below 20%.Larger measurement errors occur primarily in highly mismatched rock joints with JMC values below 0.2,but even in cases where measurement errors exceed 80%,the maximum JMC error is only 0.0434.Thus,the proposed photogrammetric approach holds promise for widespread application in void geometry measurements in rock joints.
基金funded by a grant from the National Natural Science Foundation of China(Grant Nos.U2244207,42102200)the China Geological Survey Foundation(Grant Nos.DD20230257,DD20242404)。
文摘The Upper Cretaceous Qingshankou Formation black shales,deposited in the late Turonian(LTB shales),are the main source rocks of the Songliao Basin.The origins of organic matter enrichment of the shales is a contentious subject fuelling many ongoing debates.This study investigates the genesis of the organic matter-rich shale by using molecular geochemistry.The LTB shales can be divided into three sections.The SectionⅠshales were deposited in saline,stratified and anoxic water conditions,which are related to seawater incursion events.At least three episodic and periodic seawater incursion events were recognized during SectionⅠshale deposition.The SectionⅡshales deposited in brackish to fresh and deep lake-level conditions with high primary productivity,which are related to lake-level transgression.The SectionⅢshales were deposited under fresh and slightly oxidized water conditions,which are related to lake-level regression.Two organic matter enrichment models for the LTB shales are identified,that is,the seawater incursion model and the maximum lake-level transgression sedimentation model,which act on different shale sections,both playing significant roles in the enrichment of organic matter.
基金funded by the National Natural Science Foundation of China(Grant No.42172147)PetroChina Major Science and Technology Project(Grant No.ZD2019-183-002).
文摘Gypsum caprocks'sealing ability is affected by temperature-pressure coupling.Due to the limitations of experimental conditions,there is still a lack of triaxial stress-strain experiments that simultaneously consider changes in temperature and pressure conditions,which limits the accuracy of the comprehensive evaluation of the brittle plastic evolution and sealing ability of gypsum rocks using temperature pressure coupling.Triaxial stress-strain tests were utilized to investigate the differences in the evolution of the confinement capacity of gypsum rocks under coupled temperaturepressure action and isothermal-variable pressure action on the basis of sample feasibility analysis.According to research,the gypsum rock's peak and residual strengths decrease under simultaneous increases in temperature and pressure over isothermal pressurization experimental conditions,and it becomes more ductile.This reduces the amount of time it takes for the rock to transition from brittle to plastic.When temperature is taken into account,both the brittle–plastic transformation's depth limit and the lithological transformation of gypsum rocks become shallower,and the evolution of gypsum rocks under variable temperature and pressure conditions is more complicated than that under isothermal pressurization.The sealing ability under the temperature-pressure coupling is more in line with the actual geological context when the application results of the Well#ZS5 are compared.This provides a theoretical basis for precisely determining the process of hydrocarbon accumulation and explains why the early hydrocarbon were not well preserved.
基金financially supported by the National Natural Science Foundation of China(52071072)the Fundamental Research Funds for the Central Universities(2023GFZD03)+4 种基金the Natural Science Foundation-Steel,the Iron Foundation of Hebei Province(E2022501030)the Key Research and Development Plan of Qinhuangdao City(202302B013)the Liaoning Applied Basic Research Program(2023JH2/101300011)the Basic scientific research project of Liaoning Province Department of Education(LJKZZ20220024)the Shenyang Science and Technology Project(23-407-3-13)。
文摘The oxygen evolution reaction(OER)is a crucial step in metal-air batteries and water splitting technologies,playing a significant role in the efficiency and achievable heights of these two technologies.However,the OER is a four-step,four-electron reaction,and its slow kinetics result in high overpotentials,posing a challenge.To address this issue,numerous strategies involving modified catalysts have been proposed and proven to be highly efficient.In these strategies,the introduction of strain has been widely reported because it is generally believed to effectively regulate the electronic structure of metal sites and alter the adsorption energy of catalyst surfaces with reaction intermediates.However,strain has many other effects that are not well known,making it an important yet unexplored area.Based on this,this review provides a detailed introduction to the various roles of strain in OER.To better explain these roles,the review also presents the definition of strain and elucidates the potential mechanisms of strain in OER based on the d-band center theory and adsorption volcano plot.Additionally,the review showcases various ways of introducing strain in OER through examples reported in the latest literature,aiming to provide a comprehensive perspective for the development of strain engineering.Finally,the review analyzes the appropriate proportion of strain introduction,compares compressive and tensile strain,and examines the impact of strain on stability.And the review offers prospects for future research directions in this emerging field.
基金supported by the National Natural Science Foundation of China(Nos.42072130,41872152).
文摘Based on the petrology,isotope geochemistry and fluid inclusions analysis,we established the evolutionary mode of the diagenetic fluid of dawsonite-bearing sandstone in the Jiyang Depression.Dawsonite-bearing sandstone is characterized by double injection of CO_(2)and oil-gas in the Jiyang Depression that have experienced a relatively complex diagenetic fluid evolution process.The diagenetic sequence of secondary minerals involves secondary enlargement of quartz,kaolinite,first-stage calcite,dawsonite,second-stage calcite,ferrocalcite,dolomite and ankerite.Hydrocarbon charging in the dawsonite-bearing sandstone occurred at around 2.6–0 Myr.The CO_(2)charging event occurred during Dongying tectonism,forming the Pingfangwang CO_(2)gas reservoir,which provided an abundant carbon source for dawsonite precipitation.Carbon and oxygen isotopic compositions of dawsonite demonstrate that CO_(2)forming the dawsonite was of an inorganic origin derived from the mantle,and that water mediating the proc-ess during dawsonite precipitation was sequestered brine with a fluid temperature of 82℃.The evolutionary sequence of the diagenetic fluid in the dawsonite-bearing sandstone was:alkaline syngenetic fluids,weak alkaline fluids during organic acid forma-tion,acidic fluids in the early stage of CO_(2)injection,alkaline fluids in the late stage of CO_(2)injection,and weak alkaline fluids during oil and gas charging.The mode indicates an increase in-HCO_(3)because of the CO_(2)injection,and the loss of Ca^(2+)and Mg^(2+)due to the precipitation of carbonate minerals.Therefore,the evolutionary mode of diagenetic fluids is in good agreement with high HCO_(3)^(-),low Ca^(2+)and low Mg^(2+)composition of the present formation water in the dawsonite-bearing sandstone.
基金the National Elite Foundationthe Institute for Advanced Studies in Basic Sciences for their financial supportfinancially supported by the National Natural Science Foundation of China(22173026,22350410386,22375200,U22A202175,21961142006)。
文摘This study investigates the effects of Fe on the oxygen-evolution reaction(OER)in the presence of Au.Two distinct areas of OER were identified:the first associated with Fe sites at low overpotential(~330 mV),and the second with Au sites at high overpotential(~870 mV).Various factors such as surface Fe concentration,electrochemical method,scan rate,potential range,concentration,method of adding K_(2)Fe O_(4),nature of Fe,and temperature were varied to observe diverse behaviors during OER for Fe O_(x)H_(y)/Au.Trace amounts of Fe ions had a significant impact on OER,reaching a saturation point where the activity did not increase further.Strong electronic interaction between Fe and Au ions was indicated by X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)analyses.In situ visible spectroscopy confirmed the formation of Fe O_(4)^(2-)during OER.In situ Mossbauer and surfaceenhanced Raman spectroscopy(SERS)analyses suggest the involvement of Fe-based species as intermediates during the rate-determining step of OER.A lattice OER mechanism based on Fe O_(x)H_(y)was proposed for operation at low overpotentials.Density functional theory(DFT)calculations revealed that Fe oxide,Fe-oxide clusters,and Fe doping on the Au foil exhibited different activities and stabilities during OER.The study provides insights into the interplay between Fe and Au in OER,advancing the understanding of OER mechanisms and offering implications for the design of efficient electrocatalytic systems.
基金supported by the China Geological Survey(Grant No.DD20230254)。
文摘The Beishan orogen,located in the central segment of the Tianshan–Solonker suture within the southern Central Asian Orogenic Belt(CAOB),is crucial for understanding the accretionary processes and continental growth in Central Asia.This orogen developed through the episodic amalgamation and accretion of continental margin arcs,island arcs,ophiolites,and accretionary wedges,undergoing a complex process of accretion and evolution.Since the Phanerozoic,the Beishan orogen has experienced multiple phases of magmatic and collision events.The intricate distribution of magmatic arc rocks has obscured the complete basement traces,and the spatial superposition of multiple magmatic arc phases has complicated the study of its evolutionary history.
基金Under the auspices of National Natural Science Foundation of China(No.41930651)Sichuan Science and Technology Program(No.2023NSFSC1979)。
文摘Urban-suburban-rural(U-S-R)zones exhibit distinctive transitional characteristics in interaction between human and nature.U-S-R transition zones(U-S-RTZ)are also highlighting the function diversity and landscape heterogeneity across territorial spaces.As a super megacity in western China,Chengdu’s rapid urbanization has driven the evolution of U-S-R spaces,resulting in a sequential structure.To promote the high-quality spatial development of urban-rural region in a structured and efficient manner,it is essential to con-duct a scientific examination of the multidimensional interconnection within the U-S-RTZ framework.By proposing a novel identifica-tion method of U-S-RTZ and taking Chengdu,China as a case study,grounded in a blender of natural and humanistic factors,this study quantitatively delineated and explored the spatial evolutions of U-S-RTZ and stated the optimization orientation and sustainable devel-opment strategies of the production-living-ecological spaces along the U-S-R gradients.The results show that:1)it is suitable for the quantitative analysis of U-S-RTZ by established three-dimensional identification system in this study.2)In 1990-2020,the urban-sub-urban transition zones(U-STZ)in Chengdu have continuously undergone a substantial increase,and the scale of the suburban-rural transition zones(S-RTZ)has continued to expand slightly,while the space of rural-ecological transition zones(R-ETZ)has noticeably compressed.3)The landuse dynamics within U-S-RTZ has gradually increased in 1990-2020.The main direction of landuse transition was from farmland to construction land or woodlands,with the expansion of construction land being the most significant.4)R-ETZ primarily focus on ecological functions,and there is a trade-off relationship between the production-ecological function within the S-RTZ,and in the U-STZ,production-living composite functions are prioritized.This study emphasizes the importance of elastic planning and precise governance within the U-S-RTZ in a rapid urbanization region,particularly highlighting the role of suburbs as landscape corridors and service hubs in urban-rural integration.It elucidates to the practical implications for achieving high-quality development of integrated U-S-R territorial spaces.
基金the National Natural Science Foundation of China(U21A20286,22206054 and 21805069)Natural Science Foundation of Hubei(2021CFB094)the Fundamental Research Funds for the Central China Normal University(CCNU)for financial support。
文摘Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER.Herein,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied potentials.Guided by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly.Our work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.
基金supported by the National Natural Science Foundation of China(Nos.41472065 and 42073059).
文摘The experimental results of the reactions between an alkaline basaltic melt and mantle orthopyroxenes under high-temperature and high-pressure conditions of 1300–1400℃ and 2.0–3.0 GPa using a six-anvil apparatus are reported in this paper.The reactions are proposed to simulate the interactions between melts from the asthenospheric mantle and the lithospheric mantle.The starting melt in the experiments was made from the alkaline basalt occurring in Fuxin,Liaoning Province,and the orthopyroxenes were separated from the mantle xenoliths in Damaping,Hebei Province.The results show that clinopyroxenes were formed in all the reactions between the alkaline basaltic melt and orthopyroxenes under the studied P–T conditions.The formation of clinopyroxene in the reaction zone is mainly controlled by dissolution–crystallization,and the chemical compositions of the reacted melt are primarily infl uenced by the diff usion eff ect.Temperature is the most important parameter controlling the reactions between the melt and orthopyroxenes,which has a direct impact on the melting of orthopyroxenes and the diff usion of chemical components in the melt.Temperature also directly controls the chemical compositions of the newly formed clinopyroxenes in the reaction zone and the reacted melt.The formation of clinopyroxenes from the reactions between the alkaline basaltic melt and orthopyroxenes can result in an increase of CaO and Al_(2)O_(3) contents in the rocks containing this mineral.Therefore,the reactions between the alkaline basaltic melt from the asthenospheric mantle and orthopyroxenes from the lithospheric mantle can lead to the evolution of lithospheric mantle in the North China Craton from refractory to fertile with relatively high CaO and Al 2 O 3 contents.In addition,the reacted melts in some runs were transformed from the starting alkaline basaltic into tholeiitic after reactions,indicating that tholeiitic magma could be generated from alkaline basaltic one via reactions between the latter and orthopyroxene.
基金the immense support provided by the National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIT)(RS-2023–00210114)the National R&D Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(2021M3D1A2051636)。
文摘Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER.