Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
In the harsh service environment of high temperature and intense neutron irradiation in water-cooled nuclear reactors,the austenitic stainless steel weld overlay cladding on the inner surface of the reactor pressure v...In the harsh service environment of high temperature and intense neutron irradiation in water-cooled nuclear reactors,the austenitic stainless steel weld overlay cladding on the inner surface of the reactor pressure vessel suffers from thermal aging and irradiation damage simultaneously,which can induce microstructural evolution and hardening of the material.Since it is quite difficult to achieve this simul-taneous process out of the pile,two kinds of combined experiments,i.e.,post-irradiation thermal aging and post-aging irradiation were performed on 308 L stainless steel weld metals in this work.The interactive effect of thermal aging and proton irradiation on microstructural evolution and hardening ofδ-ferrite in 308 L weld metal was investigated by combining atom probe tomography,transmission elec-tron microscopy and nanoindentation tests.The results revealed that thermal aging could eliminate the dislocation loops induced by irradiation and affect the phase transition process by accelerating spinodal decomposition and G-phase precipitation,thus enhancing hardening of irradiatedδ-ferrite.For the effect of irradiation on the microstructure and hardening of thermally agedδ-ferrite,however,intensive collision cascades can intensify G-phase precipitation and dislocation loop formation but decrease spinodal decomposition,leading to a limited effect on hardening of thermally agedδ-ferrite.Furthermore,the interaction of thermal aging and irradiation can promote G-phase precipitation.Meanwhile,the interaction can causeδ-ferrite hardening,which is mainly influenced by spinodal decomposition,followed by G-phase and dislocation loops,where spinodal decomposition and G-phase cause hardening by inducing strain fields.展开更多
The efficiency of electrochemical water splitting is extremely hampered by the sluggish oxygen evolution reaction(OER)occurred at the anode.Therefore,developing high-performance OER electrocatalysts is crucial for rea...The efficiency of electrochemical water splitting is extremely hampered by the sluggish oxygen evolution reaction(OER)occurred at the anode.Therefore,developing high-performance OER electrocatalysts is crucial for realizing the industrialized application of water splitting.Herein,a high-efficiency electrocatalyst of ruthenium-decorated nickel-iron hydroxide(10 Ru-NiFe LDH)supported on Ni foam is successfully synthesized for OER.Modifying NiFe LDH with ruthenium can optimize the electronic density to form high valences of metal sites,which is beneficial to promote its OER performance.Consequently,the 10 Ru-NiFe LDH only needs a low overpotential of 222 mV to achieve a current density of50 mA,cm^(-2),which exhibits fast OER kinetics with a small Tafel slope of 58 mV.dec^(-1).Moreover,this electrocatalyst shows high stability over 20 h at a high current density of 100 mA·cm^(-2)without obvious decay.The decent OER performances can be ascribed to the increased active sites and the synergistic electronic interactions among Ni,Fe and Ru.This work provides an effective approach for designing desirable electrocatalysts for OER.展开更多
The B-box(BBX)family of proteins consists of zinc-finger transcription factors with one or two highly conserved B-box motifs at their N-termini.BBX proteins play crucial roles in various aspects of plant growth and de...The B-box(BBX)family of proteins consists of zinc-finger transcription factors with one or two highly conserved B-box motifs at their N-termini.BBX proteins play crucial roles in various aspects of plant growth and development,including seedling photomorphogenesis,shade avoidance,flowering time,and biotic and abiotic stress responses.Previous studies have identified many different BBXs from several plant species,although the BBX family members in maize are largely unknown.Genome-wide identification and comprehensive analysis of maize BBX(ZmBBX)expression and interaction networks would therefore provide valuable information for understanding their functions.In this study,36 maize BBXs in three major clades were identified.The ZmBBXs within a given clade were found to share similar domains,motifs,and genomic structures.Gene duplication analyses revealed that the expansion of BBX proteins in maize has mainly occurred by segmental duplication.The expression levels of ZmBBXs were analyzed in various organs and tissues,and under different abiotic stress conditions.Protein–protein interaction networks of ZmBBXs were established using bioinformatic tools and verified by bimolecular fluorescence complementation(BiFC)assays.Our findings can facilitate a greater understanding of the complexity of the ZmBBX family and provide novel clues for unravelling ZmBBX protein functions.展开更多
As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attra...As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attracted much attention from researchers due to its operational simplicity,the high purity of the hydrogen generated,and its potential for achieving zero carbon emissions throughout the process.Numerous studies has been manipulated on platinum(Pt)-based catalysts,which exhibit superior performance in hydrogen evolution reactions.Within this category,Pt nanoclusters stand out due to their unique attributes,such as quantum size effects and unique coordination environments.These features enable them to outperform both Pt metal atoms and nanoparticles in hydrogen evolution reactions regarding activity and stability.Here,we primarily delve into the reaction mechanisms underlying Pt nanocluster-based hydrogen catalysts,with particular emphasis on the interactions between the metal catalysts and their associated support materials.We provide an exhaustive summary of the strategies employed in the synthesis,the structural analyses conducted,and the performance metrics observed for Pt nanocluster catalysts when paired with various supporting materials.In closing,we explore the future potential and challenges facing Pt nanocluster-based catalysts in the context of industrial water electrolysis,along with emerging avenues for their design and optimization.展开更多
High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging sca...High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.展开更多
Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote t...Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote the generation of hydrogen from mild methods.In this work,Co–Mo phosphide nanosheets with the adjustable ratio of Co and Mo were fabricated on carbon cloth by a facile hydrothermal-annealing method.Owing to the unique nanostructures,abundant active surfaces and small resistance were achieved.Excellent electrocatalytic performances are obtained,such as the small overpotential of^67.3 mV to realize a current density of 10 mA cm^(-2) and a Tafel slope of 69.9 mV dec^(-1).Rapid recovery of the current response under multistep chronoamperometry is realized and excellent stability retained after the CV test for 2000 cycles.The change of electronic states of different elements was carefully studied which suggested the optimal electrochemical performance can be realized by tuning phosphorous and metal interactions.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
It is urgent and important to explore the dynamic evolution in comprehensive transportation green efficiency(CTGE)in the context of green development.We constructed a social development index that reflects the social ...It is urgent and important to explore the dynamic evolution in comprehensive transportation green efficiency(CTGE)in the context of green development.We constructed a social development index that reflects the social benefits of transportation services,and incorporated it into the comprehensive transportation efficiency evaluation framework as an expected output.Based on the panel data of 30 regions in China from 2003-2018,the CTGE in China was measured using the slacks-based measure-data envelopment analysis(SBM-DEA)model.Further,the dynamic evolution trends of CTGE were determined using the spatial Markov model and exploratory spatio-temporal data analysis(ESTDA)technique from a spatio-temporal perspective.The results showed that the CTGE shows a U-shaped change trend but with an overall low level and significant regional differences.The state transition of CTGE has a strong spatial dependence,and there exists the phenomenon of“club convergence”.Neighbourhood background has a significant impact on the CTGE transition types,and the spatial spillover effect is pronounced.The CTGE has an obvious positive correlation and spatial agglomeration characteristics.The geometric characteristics of the LISA time path show that the evolution process of local spatial structure and local spatial dependence of China’s CTGE is stable,but the integration of spatial evolution is weak.The spatio-temporal transition results of LISA indicate that the CTGE has obvious transfer inertness and has certain path-dependence and spatial locking characteristics,which will become the major difficulty in improving the CTGE.展开更多
Owing to the exorbitant overpotential and serious carrier recombination of graphitic carbon nitride(gC_(3)N_(4)),noble metal(NM)is usually served as the H_(2)evolution co-catalyst.Although the NM(such as Pt)nanopartic...Owing to the exorbitant overpotential and serious carrier recombination of graphitic carbon nitride(gC_(3)N_(4)),noble metal(NM)is usually served as the H_(2)evolution co-catalyst.Although the NM(such as Pt)nanoparticles can reduce the H_(2)evolution overpotential,the weak van der Waals interaction between Pt and g-C_(3)N_(4)makes against the charge transfer.Herein,the solvothermal method is developed to achieve semi-chemical interaction between Pt and g-C_(3)N_(4)nanotube(Pt-CNNT)for fast charge transfer.Moreover,the generated in-plane homojunction of CNNT can accelerate charge separation and restrain recombination.Meanwhile,the metallic Pt is an excellent H_(2)evolution co-catalyst.Photo/electrochemical tests verify that the semi-chemical interaction can improve photogenerated charge separation and transferability of CNNT.As a result,the photocatalytic H_(2)evolution turnover frequency(TOF)of Pt-CNNT under visible light irradiation reaches up to 918 h^(-1),which is one of the highest in the g-C_(3)N_(4)-based photocatalysts.This work provides a new idea to improve the charge transfer for efficient photocatalytic H_(2)evolution.展开更多
This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionar...This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionary processes.By representing agents and their defined environments with probabilistic interactions,ABM allows the assessment of the effects of individual behavior at the micro level on the greater social phenomena at the macro level.The review looks into the applications of ABM in portraying some of the key components of emotions and cognition-empathy,cooperation,decision making,and emotional transmission-and analyzes the problems including scalability,empirical validation,and description of sensitive emotional states.The most important conclusion is that merging ABM with information neurobiological data and artificial intelligence(AI)techniques would allow for deepening the interactions within the system and enhancing its responsiveness to stimuli.This review highlights approaches that aim to exploit the ABM methodology more fully and integrates methods from biology,neuroscience,and engineering.This integration could contribute to our understanding of the human behavior evolution and adaptation within systems relevant to policymaking,healthcare,and education.展开更多
Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from ...Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low efficiencies.In this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption spectra.The VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good stability.Under optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure g-C3N4.The role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs effectively.It is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.展开更多
High-order accurate schemes are employed to numerically simulate the interaction of a supersonic jet and a co-directional supersonic inflow. A double backward-facing step model is proposed to investigate the interacti...High-order accurate schemes are employed to numerically simulate the interaction of a supersonic jet and a co-directional supersonic inflow. A double backward-facing step model is proposed to investigate the interaction between the jet shear layer and the supersonic inflow shear layer. It is found that due to the interaction of the shear layer, a secondary jet is injected into the recirculation zone at the intersection of the two shear layers. The secondary jet produced by the interaction of the two shear layers has a periodicity because of shear layers interaction. The distinction in the shape of double backward-facing steps will induce changes in the period of the secondary jet. The analysis and discussion of the periodicity of the secondary jet are mainly focused in this letter.展开更多
In this part, the temporal evolution and interaction across the equator of 30-50 day oscillation in the atmosphere are investigated further. The annual variation of 30-50 day oscillation is quite obvious in the mid-hi...In this part, the temporal evolution and interaction across the equator of 30-50 day oscillation in the atmosphere are investigated further. The annual variation of 30-50 day oscillation is quite obvious in the mid-high latitudes. In the tropical atmosphere, the obvious interannual variation is an important property for temporal evolution of 30-50 day oscillation. The low-frequency wavetrain across the equator over the central Pacific and central Atlantic area, the movement of the long-lived low-frequency system across the equator and the meridional wind component across the equator will obviously show the interaction of 30-50 day oscillation in the atmosphere across the equator.展开更多
We study one-and two-soliton solutions for the Cahn–Allen(CA) equation and the Brethorton equation. The CA equation has broad spectrum of applications especially in anti-phase boundary motion and it is used in phase-...We study one-and two-soliton solutions for the Cahn–Allen(CA) equation and the Brethorton equation. The CA equation has broad spectrum of applications especially in anti-phase boundary motion and it is used in phase-field models.While the Brethorton equation is a model for dispersive wave systems, it is used to find the resonant nonlinear interaction among three linear modes. We use the Hirota bilinear method to obtain one-and two-soliton solutions to the CA equation and the Brethorton equation.展开更多
Gneiss\|distilled water interaction at room temperature was investigated with batch\|reactors to study water\|rock reaction and geochemical evolution of the aqueous phase with time. The ion concentrations in water wer...Gneiss\|distilled water interaction at room temperature was investigated with batch\|reactors to study water\|rock reaction and geochemical evolution of the aqueous phase with time. The ion concentrations in water were controlled not only by the dissolution of primary minerals, but also by the precipitation of secondary minerals. The decreasing fraction sizes of gneiss could favor dissolution and precipitation simultaneously. Ca\+\{2+\} and K\++ were the major cations, and HCO\+-\-3 was the major anion in water. All the ions except Ca\+\{2+\} increased in concentration with time. The Ca\+\{2+\} release from the rock to the aqueous phase was initially much faster than the release of K\++, Na\++ and Mg\+\{2+\}. But after about 5-24 hours, the Ca\+\{2+\} concentrations in water decreased very slowly with time and became relatively stable. During the experiment, the water varied from the Ca\|(K)\|HCO\-3\|type water to the K\|Ca\|HCO\-3\|type water, and then to the K\|(Ca,Na)\|HCO\-3\|type water. The water\|gneiss interaction was dominated by the dissolution of K\|feldspar in the solution. The remaining secondary minerals were mainly kaolinite, illite and K(Mg)\|mica.展开更多
Softening of soft red-bed rocks subjected to rainfall-evaporation cycles is commonly characterized by rapid disintegration and is often accompanied by cracking,resulting in degradation of the mechanical properties of ...Softening of soft red-bed rocks subjected to rainfall-evaporation cycles is commonly characterized by rapid disintegration and is often accompanied by cracking,resulting in degradation of the mechanical properties of the rock,which can lead to slope instability or rockfalls.The microstructural changes in soft red-bed rocks after immersion were imaged,and two-dimensional(2D)images of cracks under water absorption-evaporation conditions were obtained.The dynamics,fractal characteristics,and geometry of the cracks were analyzed using digital image processing and analysis based on morphological algorithms.The results indicate that the faceeface particle bonds become pointeface bonds with numerous micropores with sizes of 1-5 mm.The evolution of cracks generated after water absorption can be divided into four stages:edge crack initiation,crack propagation,crack coalescence forming the main crack,and subcrack segmentation.The evolution of the dynamic characteristics of cracks during water absorption and drying cycles can be effectively described by the crack intensity factor,crack density,and average width.The fractal dimension increases to a stable value with increasing soaking time,whereas drying increases the crack complexity,resulting in fractal dimensions ranging from 1.106 to 1.126.The geometry results indicate that the crack directions are mainly at angles of 30°-70°after soaking and primarily in the range of 50°-60°after 10 drying cycles.The transition of the crack intersection angle from a bimodal to a unimodal distribution suggests that water absorption and drying processes tend to form Y-shaped and T-shaped cracks,respectively.Finally,the evolution of the watererock interface induced by particle dissolution,ion exchange,expansion force,and liquid surface tensionwas used to explain the mechanism of crack evolution related to water entry and evaporation.These results provide a theoretical basis for evaluating the cracking behavior of soft red-bed rocks.展开更多
Marine organic-rich marl is not only a high-quality hydrocarbon source of conventional oil and gas,but also a new type and field of unconventional oil and gas exploration.An understanding of its pore structure evoluti...Marine organic-rich marl is not only a high-quality hydrocarbon source of conventional oil and gas,but also a new type and field of unconventional oil and gas exploration.An understanding of its pore structure evolution characteristics during a hydrocarbon generation process is theoretically significant and has application prospects for the exploration and development of this special type of natural gas reservoirs.This study conducted thermal simulation of hydrocarbon generation under near-geological conditions during a whole process for cylinder samples of low mature marine organic-rich marl in the Middle Devonian of Luquan,Yunnan Province,China.During this process,hydrocarbon products at different evolution stages were quantified and corresponding geochemical properties were analyzed.Simultaneously,field emission scanning electron microscopy(FE-SEM)and low-pressure gas adsorption(CO_(2),N_(2))tests were applied to the corresponding cylinder residue samples to reveal the mechanisms of different types of pore formation and evolution,and clarify the dynamic evolution processes of their pore systems.The results show that with an increase in temperature and pressure,the total oil yield peaks at an equivalent vitrinite reflectance(VR_(o))of 1.03%and is at the maximum retention stage of liquid hydrocarbons,which are 367.51 mg/g TOC and 211.67 mg/g TOC,respectively.The hydrocarbon gas yield increases continuously with an increase in maturity.The high retained oil rate at the peak of oil generation provides an abundant material basis for gas formation at high maturity and over-maturity stage.The lower limit of VR_(o)for organic matter(OM)pore mass development is about 1.6%,and bitumen pores,organic-clay complex pores together with intergranular pores,grain edge seams and dissolution pores constitute a complicated pore-seam-network system,which is the main reservoir space for unconventional carbonate gas.Pore formation and evolution are controlled synergistically by hydrocarbon generation,diagenesis and organic-inorganic interactions,and the pattern of pore structure evolution can be divided into four stages.A pore volume(PV)and a specific surface area(SSA)are at their highest values within the maturity range of 1.9%to 2.5%,which is conducive to exploring unconventional natural gas.展开更多
Highly evolved granite associated with pegmatite shells exhibits significant potential for rare metal mineralization;however,the mechanisms through which these pegmatite shells contribute to magmatic evolution and rar...Highly evolved granite associated with pegmatite shells exhibits significant potential for rare metal mineralization;however,the mechanisms through which these pegmatite shells contribute to magmatic evolution and rare metal enrichment remain poorly understood.The Late Jurassic Shihuiyao Nb-Ta-(Rb-Be-Li)deposit is one of the largest rare-metal deposits in the Southern Great Xing’an Range(SGXR),Northeast China.Exploratory trenches expose distinct layered zones from top to bottom:alternating microcline pegmatite and aplite layers(zone I),topaz lepidolite albite granite and lepidolite amazonite pegmatite(zone II),and muscovite albite granite(zoneⅢ).We conducted U-Pb dating of cassiterite,monazite,and Nb-Ta oxide,monazite Nd isotopes,and whole-rock and mineral geochemistry for the three zones.Multi-mineral U-Pb ages indicate that the three zones formed during the Late Jurassic-Early Cretaceous(147-142 Ma).Geochemical analyses of whole-rock,mica,and microcline suggest an evolutionary sequence from zone I to zoneⅢ,and finally to zone II.The Zr/Hf,Nb/Ta,Y/Ho,and K/Rb ratios combined with the rare earth element(REE)tetrad effects suggest higher degree of differentiation and fluid-melt interaction of the Shihuiyao leucogranite without a pegmatite shell compared to coeval barren granites from both Shihuiyao and the SGXR.A progressive increase in the degree of evolution is evident from the leucogranite without a pegmatite shell to the leucogranite with a discontinuous shell,and ultimately to the leucogranite with a continuous shell.The pegmatite shell acted as a geochemical barrier that facilitated the accumulation of Li and F in the underlying magma,which played a crucial role in lowering the solidus temperature of the granitic magma.This process prolonged the crystallization duration while reducing melt viscosity and density,thereby creating favorable conditions for magma differentiation and fluid-melt interaction.Rapid crystallization of the earlier water-and Be-rich melt led to the Be mineralization in the pegmatite shell.Moreover,the formation of this shell served as a barrier for Li mineralization in the underlying topaz lepidolite albite granite.This study enhances our understanding of the critical contribution of pegmatite shells to magmatic evolution and rare-metal mineralization.展开更多
Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution(HER)electrocatalysts.Herein,a unique Pt-O-Ni bridge has been construc...Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution(HER)electrocatalysts.Herein,a unique Pt-O-Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles(Pt_n)and nickel metaphosphate(NPO)substrate(Pt-NPO).Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_n.Furthermore,H*is produced from the H_(2)O dissociation on Ni site and then spillover toward Pt sites to bind into H_(2),which makes up for the insufficient H_(2)O dissociation ability of Pt in Volmer step.Pt-NPO exhibits long-term stability and only need the overpotentials of 22.3,33.0 and 30.5 mV to attain 10 mA cm^(-2)in alkaline,neutral and acidic media,respectively.The anion-exchange membrane(AEM)water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of500 mA cm^(-2)in 1 M KOH at 80℃,at the same time maintains good stability for 350 h.The regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.展开更多
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金supported by the National Natural Science Foundation of China(No.52071018).
文摘In the harsh service environment of high temperature and intense neutron irradiation in water-cooled nuclear reactors,the austenitic stainless steel weld overlay cladding on the inner surface of the reactor pressure vessel suffers from thermal aging and irradiation damage simultaneously,which can induce microstructural evolution and hardening of the material.Since it is quite difficult to achieve this simul-taneous process out of the pile,two kinds of combined experiments,i.e.,post-irradiation thermal aging and post-aging irradiation were performed on 308 L stainless steel weld metals in this work.The interactive effect of thermal aging and proton irradiation on microstructural evolution and hardening ofδ-ferrite in 308 L weld metal was investigated by combining atom probe tomography,transmission elec-tron microscopy and nanoindentation tests.The results revealed that thermal aging could eliminate the dislocation loops induced by irradiation and affect the phase transition process by accelerating spinodal decomposition and G-phase precipitation,thus enhancing hardening of irradiatedδ-ferrite.For the effect of irradiation on the microstructure and hardening of thermally agedδ-ferrite,however,intensive collision cascades can intensify G-phase precipitation and dislocation loop formation but decrease spinodal decomposition,leading to a limited effect on hardening of thermally agedδ-ferrite.Furthermore,the interaction of thermal aging and irradiation can promote G-phase precipitation.Meanwhile,the interaction can causeδ-ferrite hardening,which is mainly influenced by spinodal decomposition,followed by G-phase and dislocation loops,where spinodal decomposition and G-phase cause hardening by inducing strain fields.
基金financially supported by the National Natural Science Foundation of China (Nos.12074435, 51871250 and 52001335)the Science and Technology Innovation Program of Hunan Province (No.2021RC4001)the State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum Metal (No.SKL-SPM-202005)
文摘The efficiency of electrochemical water splitting is extremely hampered by the sluggish oxygen evolution reaction(OER)occurred at the anode.Therefore,developing high-performance OER electrocatalysts is crucial for realizing the industrialized application of water splitting.Herein,a high-efficiency electrocatalyst of ruthenium-decorated nickel-iron hydroxide(10 Ru-NiFe LDH)supported on Ni foam is successfully synthesized for OER.Modifying NiFe LDH with ruthenium can optimize the electronic density to form high valences of metal sites,which is beneficial to promote its OER performance.Consequently,the 10 Ru-NiFe LDH only needs a low overpotential of 222 mV to achieve a current density of50 mA,cm^(-2),which exhibits fast OER kinetics with a small Tafel slope of 58 mV.dec^(-1).Moreover,this electrocatalyst shows high stability over 20 h at a high current density of 100 mA·cm^(-2)without obvious decay.The decent OER performances can be ascribed to the increased active sites and the synergistic electronic interactions among Ni,Fe and Ru.This work provides an effective approach for designing desirable electrocatalysts for OER.
基金financially supported by grants from the Natural Science Foundation of Shandong Province,China(ZR2018LC005 and ZR2019BC107)the Agricultural Science and Technology Innovation Project of Shandong Academy of Agricultural Sciences,China(CXGC2022C02)。
文摘The B-box(BBX)family of proteins consists of zinc-finger transcription factors with one or two highly conserved B-box motifs at their N-termini.BBX proteins play crucial roles in various aspects of plant growth and development,including seedling photomorphogenesis,shade avoidance,flowering time,and biotic and abiotic stress responses.Previous studies have identified many different BBXs from several plant species,although the BBX family members in maize are largely unknown.Genome-wide identification and comprehensive analysis of maize BBX(ZmBBX)expression and interaction networks would therefore provide valuable information for understanding their functions.In this study,36 maize BBXs in three major clades were identified.The ZmBBXs within a given clade were found to share similar domains,motifs,and genomic structures.Gene duplication analyses revealed that the expansion of BBX proteins in maize has mainly occurred by segmental duplication.The expression levels of ZmBBXs were analyzed in various organs and tissues,and under different abiotic stress conditions.Protein–protein interaction networks of ZmBBXs were established using bioinformatic tools and verified by bimolecular fluorescence complementation(BiFC)assays.Our findings can facilitate a greater understanding of the complexity of the ZmBBX family and provide novel clues for unravelling ZmBBX protein functions.
基金the National Key Research and Development Program of China(No.2022YFB4102000)the National Natural Science Foundation of China(NSFC,Nos.22102018 and 52171201)+4 种基金the Huzhou Science and Technology Bureau(No.2022GZ45)the Hefei National Research Center for Physical Sciences at the Microscale(No.KF2021005)the China Postdoctoral Science Foundation-Funded Project(No.2022M710601)the Huzhou Science and Technology Bureau(No.2023GZ02)the Natural Science Foundation of Sichuan Province(No.24NSFSC5779)。
文摘As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attracted much attention from researchers due to its operational simplicity,the high purity of the hydrogen generated,and its potential for achieving zero carbon emissions throughout the process.Numerous studies has been manipulated on platinum(Pt)-based catalysts,which exhibit superior performance in hydrogen evolution reactions.Within this category,Pt nanoclusters stand out due to their unique attributes,such as quantum size effects and unique coordination environments.These features enable them to outperform both Pt metal atoms and nanoparticles in hydrogen evolution reactions regarding activity and stability.Here,we primarily delve into the reaction mechanisms underlying Pt nanocluster-based hydrogen catalysts,with particular emphasis on the interactions between the metal catalysts and their associated support materials.We provide an exhaustive summary of the strategies employed in the synthesis,the structural analyses conducted,and the performance metrics observed for Pt nanocluster catalysts when paired with various supporting materials.In closing,we explore the future potential and challenges facing Pt nanocluster-based catalysts in the context of industrial water electrolysis,along with emerging avenues for their design and optimization.
基金project was funded by National Natural Science Foundation of China(Nos.21901154,21671129)the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT17R71)。
文摘High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.
基金funded by the NSFC(51602193)Shanghai“Chen Guang”Project(16CG63)+2 种基金the Fundamental Research Funds for the Central Universities(WD1817002)the STFC Batteries Network(ST/R006873/1)funding from the EPSRC(EP/R023581/1,EP/P009050/1).
文摘Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote the generation of hydrogen from mild methods.In this work,Co–Mo phosphide nanosheets with the adjustable ratio of Co and Mo were fabricated on carbon cloth by a facile hydrothermal-annealing method.Owing to the unique nanostructures,abundant active surfaces and small resistance were achieved.Excellent electrocatalytic performances are obtained,such as the small overpotential of^67.3 mV to realize a current density of 10 mA cm^(-2) and a Tafel slope of 69.9 mV dec^(-1).Rapid recovery of the current response under multistep chronoamperometry is realized and excellent stability retained after the CV test for 2000 cycles.The change of electronic states of different elements was carefully studied which suggested the optimal electrochemical performance can be realized by tuning phosphorous and metal interactions.
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National Key Research and Development Program of China(2019YFB1600400)National Natural Science Foundation of China(72174035)+2 种基金National Natural Science Foundation of China(71774018)Liaoning Revitalization Talents Program(XLYC2008030)Liaoning Provincial Natural Science Foundation Shipping Joint Foundation Program(2020-HYLH-20)。
文摘It is urgent and important to explore the dynamic evolution in comprehensive transportation green efficiency(CTGE)in the context of green development.We constructed a social development index that reflects the social benefits of transportation services,and incorporated it into the comprehensive transportation efficiency evaluation framework as an expected output.Based on the panel data of 30 regions in China from 2003-2018,the CTGE in China was measured using the slacks-based measure-data envelopment analysis(SBM-DEA)model.Further,the dynamic evolution trends of CTGE were determined using the spatial Markov model and exploratory spatio-temporal data analysis(ESTDA)technique from a spatio-temporal perspective.The results showed that the CTGE shows a U-shaped change trend but with an overall low level and significant regional differences.The state transition of CTGE has a strong spatial dependence,and there exists the phenomenon of“club convergence”.Neighbourhood background has a significant impact on the CTGE transition types,and the spatial spillover effect is pronounced.The CTGE has an obvious positive correlation and spatial agglomeration characteristics.The geometric characteristics of the LISA time path show that the evolution process of local spatial structure and local spatial dependence of China’s CTGE is stable,but the integration of spatial evolution is weak.The spatio-temporal transition results of LISA indicate that the CTGE has obvious transfer inertness and has certain path-dependence and spatial locking characteristics,which will become the major difficulty in improving the CTGE.
基金the National Natural Science Foundation of China(Nos.51868050,51938007,51878325,51868052,52100186,52170082,and 52063024)the Natural Science Foundation of Jiangxi Province(Nos.20202BAB213011 and 20181BBG78034)the Scientific Research Foundation of Nanchang Hangkong University(No.EA201902377)。
文摘Owing to the exorbitant overpotential and serious carrier recombination of graphitic carbon nitride(gC_(3)N_(4)),noble metal(NM)is usually served as the H_(2)evolution co-catalyst.Although the NM(such as Pt)nanoparticles can reduce the H_(2)evolution overpotential,the weak van der Waals interaction between Pt and g-C_(3)N_(4)makes against the charge transfer.Herein,the solvothermal method is developed to achieve semi-chemical interaction between Pt and g-C_(3)N_(4)nanotube(Pt-CNNT)for fast charge transfer.Moreover,the generated in-plane homojunction of CNNT can accelerate charge separation and restrain recombination.Meanwhile,the metallic Pt is an excellent H_(2)evolution co-catalyst.Photo/electrochemical tests verify that the semi-chemical interaction can improve photogenerated charge separation and transferability of CNNT.As a result,the photocatalytic H_(2)evolution turnover frequency(TOF)of Pt-CNNT under visible light irradiation reaches up to 918 h^(-1),which is one of the highest in the g-C_(3)N_(4)-based photocatalysts.This work provides a new idea to improve the charge transfer for efficient photocatalytic H_(2)evolution.
文摘This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionary processes.By representing agents and their defined environments with probabilistic interactions,ABM allows the assessment of the effects of individual behavior at the micro level on the greater social phenomena at the macro level.The review looks into the applications of ABM in portraying some of the key components of emotions and cognition-empathy,cooperation,decision making,and emotional transmission-and analyzes the problems including scalability,empirical validation,and description of sensitive emotional states.The most important conclusion is that merging ABM with information neurobiological data and artificial intelligence(AI)techniques would allow for deepening the interactions within the system and enhancing its responsiveness to stimuli.This review highlights approaches that aim to exploit the ABM methodology more fully and integrates methods from biology,neuroscience,and engineering.This integration could contribute to our understanding of the human behavior evolution and adaptation within systems relevant to policymaking,healthcare,and education.
基金supported by the National Natural Science Foundation of China(51572253,21771171)Scientific Research Grant of Hefei National Synchrotron Radiation Laboratory(UN2017LHJJ)+1 种基金the Fundamental Research Funds for the Central Universitiescooperation between NSFC and Netherlands Organization for Scientific Research(51561135011)~~
文摘Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low efficiencies.In this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption spectra.The VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good stability.Under optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure g-C3N4.The role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs effectively.It is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.
基金supported by the National Key Research and Development Program of China(Grant 2016YFA0401201)the National Natural Science Foundation of China(Grants 11872066,11472281,11727901,and 11532014)。
文摘High-order accurate schemes are employed to numerically simulate the interaction of a supersonic jet and a co-directional supersonic inflow. A double backward-facing step model is proposed to investigate the interaction between the jet shear layer and the supersonic inflow shear layer. It is found that due to the interaction of the shear layer, a secondary jet is injected into the recirculation zone at the intersection of the two shear layers. The secondary jet produced by the interaction of the two shear layers has a periodicity because of shear layers interaction. The distinction in the shape of double backward-facing steps will induce changes in the period of the secondary jet. The analysis and discussion of the periodicity of the secondary jet are mainly focused in this letter.
基金This study was supported in part by National Natural Science Foundation of China
文摘In this part, the temporal evolution and interaction across the equator of 30-50 day oscillation in the atmosphere are investigated further. The annual variation of 30-50 day oscillation is quite obvious in the mid-high latitudes. In the tropical atmosphere, the obvious interannual variation is an important property for temporal evolution of 30-50 day oscillation. The low-frequency wavetrain across the equator over the central Pacific and central Atlantic area, the movement of the long-lived low-frequency system across the equator and the meridional wind component across the equator will obviously show the interaction of 30-50 day oscillation in the atmosphere across the equator.
文摘We study one-and two-soliton solutions for the Cahn–Allen(CA) equation and the Brethorton equation. The CA equation has broad spectrum of applications especially in anti-phase boundary motion and it is used in phase-field models.While the Brethorton equation is a model for dispersive wave systems, it is used to find the resonant nonlinear interaction among three linear modes. We use the Hirota bilinear method to obtain one-and two-soliton solutions to the CA equation and the Brethorton equation.
文摘Gneiss\|distilled water interaction at room temperature was investigated with batch\|reactors to study water\|rock reaction and geochemical evolution of the aqueous phase with time. The ion concentrations in water were controlled not only by the dissolution of primary minerals, but also by the precipitation of secondary minerals. The decreasing fraction sizes of gneiss could favor dissolution and precipitation simultaneously. Ca\+\{2+\} and K\++ were the major cations, and HCO\+-\-3 was the major anion in water. All the ions except Ca\+\{2+\} increased in concentration with time. The Ca\+\{2+\} release from the rock to the aqueous phase was initially much faster than the release of K\++, Na\++ and Mg\+\{2+\}. But after about 5-24 hours, the Ca\+\{2+\} concentrations in water decreased very slowly with time and became relatively stable. During the experiment, the water varied from the Ca\|(K)\|HCO\-3\|type water to the K\|Ca\|HCO\-3\|type water, and then to the K\|(Ca,Na)\|HCO\-3\|type water. The water\|gneiss interaction was dominated by the dissolution of K\|feldspar in the solution. The remaining secondary minerals were mainly kaolinite, illite and K(Mg)\|mica.
基金funded by the Sichuan Science and Technology Program(Grant Nos.2023YFS0364 and 2024YFHZ0154)the Xizang Science and Technology Program(Grant No.XZ202401ZY0097).
文摘Softening of soft red-bed rocks subjected to rainfall-evaporation cycles is commonly characterized by rapid disintegration and is often accompanied by cracking,resulting in degradation of the mechanical properties of the rock,which can lead to slope instability or rockfalls.The microstructural changes in soft red-bed rocks after immersion were imaged,and two-dimensional(2D)images of cracks under water absorption-evaporation conditions were obtained.The dynamics,fractal characteristics,and geometry of the cracks were analyzed using digital image processing and analysis based on morphological algorithms.The results indicate that the faceeface particle bonds become pointeface bonds with numerous micropores with sizes of 1-5 mm.The evolution of cracks generated after water absorption can be divided into four stages:edge crack initiation,crack propagation,crack coalescence forming the main crack,and subcrack segmentation.The evolution of the dynamic characteristics of cracks during water absorption and drying cycles can be effectively described by the crack intensity factor,crack density,and average width.The fractal dimension increases to a stable value with increasing soaking time,whereas drying increases the crack complexity,resulting in fractal dimensions ranging from 1.106 to 1.126.The geometry results indicate that the crack directions are mainly at angles of 30°-70°after soaking and primarily in the range of 50°-60°after 10 drying cycles.The transition of the crack intersection angle from a bimodal to a unimodal distribution suggests that water absorption and drying processes tend to form Y-shaped and T-shaped cracks,respectively.Finally,the evolution of the watererock interface induced by particle dissolution,ion exchange,expansion force,and liquid surface tensionwas used to explain the mechanism of crack evolution related to water entry and evaporation.These results provide a theoretical basis for evaluating the cracking behavior of soft red-bed rocks.
基金supported by the National Natural Science Foundation of China(Grant No.41930426)。
文摘Marine organic-rich marl is not only a high-quality hydrocarbon source of conventional oil and gas,but also a new type and field of unconventional oil and gas exploration.An understanding of its pore structure evolution characteristics during a hydrocarbon generation process is theoretically significant and has application prospects for the exploration and development of this special type of natural gas reservoirs.This study conducted thermal simulation of hydrocarbon generation under near-geological conditions during a whole process for cylinder samples of low mature marine organic-rich marl in the Middle Devonian of Luquan,Yunnan Province,China.During this process,hydrocarbon products at different evolution stages were quantified and corresponding geochemical properties were analyzed.Simultaneously,field emission scanning electron microscopy(FE-SEM)and low-pressure gas adsorption(CO_(2),N_(2))tests were applied to the corresponding cylinder residue samples to reveal the mechanisms of different types of pore formation and evolution,and clarify the dynamic evolution processes of their pore systems.The results show that with an increase in temperature and pressure,the total oil yield peaks at an equivalent vitrinite reflectance(VR_(o))of 1.03%and is at the maximum retention stage of liquid hydrocarbons,which are 367.51 mg/g TOC and 211.67 mg/g TOC,respectively.The hydrocarbon gas yield increases continuously with an increase in maturity.The high retained oil rate at the peak of oil generation provides an abundant material basis for gas formation at high maturity and over-maturity stage.The lower limit of VR_(o)for organic matter(OM)pore mass development is about 1.6%,and bitumen pores,organic-clay complex pores together with intergranular pores,grain edge seams and dissolution pores constitute a complicated pore-seam-network system,which is the main reservoir space for unconventional carbonate gas.Pore formation and evolution are controlled synergistically by hydrocarbon generation,diagenesis and organic-inorganic interactions,and the pattern of pore structure evolution can be divided into four stages.A pore volume(PV)and a specific surface area(SSA)are at their highest values within the maturity range of 1.9%to 2.5%,which is conducive to exploring unconventional natural gas.
基金supported by the Key Research Program of the Institute of Geology&Geophysics,CAS(IGGCAS-202205)the National Natural Science Foundation of China(Grant No.92062216 and 42102046)+1 种基金Doctoral Students'Scientific Research and Innovation Capability Enhancement Program of Jilin Province(JJKH20250074BS)Graduate Innovation Fund of Jilin University(2024CX231).
文摘Highly evolved granite associated with pegmatite shells exhibits significant potential for rare metal mineralization;however,the mechanisms through which these pegmatite shells contribute to magmatic evolution and rare metal enrichment remain poorly understood.The Late Jurassic Shihuiyao Nb-Ta-(Rb-Be-Li)deposit is one of the largest rare-metal deposits in the Southern Great Xing’an Range(SGXR),Northeast China.Exploratory trenches expose distinct layered zones from top to bottom:alternating microcline pegmatite and aplite layers(zone I),topaz lepidolite albite granite and lepidolite amazonite pegmatite(zone II),and muscovite albite granite(zoneⅢ).We conducted U-Pb dating of cassiterite,monazite,and Nb-Ta oxide,monazite Nd isotopes,and whole-rock and mineral geochemistry for the three zones.Multi-mineral U-Pb ages indicate that the three zones formed during the Late Jurassic-Early Cretaceous(147-142 Ma).Geochemical analyses of whole-rock,mica,and microcline suggest an evolutionary sequence from zone I to zoneⅢ,and finally to zone II.The Zr/Hf,Nb/Ta,Y/Ho,and K/Rb ratios combined with the rare earth element(REE)tetrad effects suggest higher degree of differentiation and fluid-melt interaction of the Shihuiyao leucogranite without a pegmatite shell compared to coeval barren granites from both Shihuiyao and the SGXR.A progressive increase in the degree of evolution is evident from the leucogranite without a pegmatite shell to the leucogranite with a discontinuous shell,and ultimately to the leucogranite with a continuous shell.The pegmatite shell acted as a geochemical barrier that facilitated the accumulation of Li and F in the underlying magma,which played a crucial role in lowering the solidus temperature of the granitic magma.This process prolonged the crystallization duration while reducing melt viscosity and density,thereby creating favorable conditions for magma differentiation and fluid-melt interaction.Rapid crystallization of the earlier water-and Be-rich melt led to the Be mineralization in the pegmatite shell.Moreover,the formation of this shell served as a barrier for Li mineralization in the underlying topaz lepidolite albite granite.This study enhances our understanding of the critical contribution of pegmatite shells to magmatic evolution and rare-metal mineralization.
基金supported by the National Natural Science Foundation of China(22202080,22034006 and 22393930)Jilin Talent Development Foundation(E41S2001)the National Key Research and Development Program of China(2022YFF0710000).
文摘Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution(HER)electrocatalysts.Herein,a unique Pt-O-Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles(Pt_n)and nickel metaphosphate(NPO)substrate(Pt-NPO).Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_n.Furthermore,H*is produced from the H_(2)O dissociation on Ni site and then spillover toward Pt sites to bind into H_(2),which makes up for the insufficient H_(2)O dissociation ability of Pt in Volmer step.Pt-NPO exhibits long-term stability and only need the overpotentials of 22.3,33.0 and 30.5 mV to attain 10 mA cm^(-2)in alkaline,neutral and acidic media,respectively.The anion-exchange membrane(AEM)water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of500 mA cm^(-2)in 1 M KOH at 80℃,at the same time maintains good stability for 350 h.The regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.
