The development of economical,highly efficient,and stable bifunctional electrocatalysts for both the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR)remains a critical focus in advancing rechargeab...The development of economical,highly efficient,and stable bifunctional electrocatalysts for both the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR)remains a critical focus in advancing rechargeable metal-air battery systems.Significant progress has been made in the design of high-performance bifunctional electrocatalysts,the development of novel oxygen electrode architectures,and the in-depth understanding of electrocatalytic mechanisms through combined experimental and computational studies.This work provides a comprehensive review of recent advancements in design strategies for oxygen catalysts,including homogeneous electrodes,asymmetric electrodes,and biomimetic electrodes,are thoroughly discussed and summarized.Then,the advanced catalyst modification strategies for ORR/OER are summarized,focusing on critical factors such as enhancement effect of metal/nonmental and synergistic enhancement effect in multiple catalyst.Subsequently,a representative performance evaluation is presented,based on the reported oxygen electrodes used in rechargeable metal-air battery applications.By focusing on these key areas,the review outlines the current challenges and future prospects for the development of bifunctional oxygen electrocatalysts,aiming to guide the design of high-performance bifunctional electrocatalysts and to elucidate the underlying mechanisms involved.展开更多
The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate...The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate evolution mechanism(AEM),lattice oxygen mechanism(LOM),and oxide path mechanism(OPM).Compared to AEM,limited by scaling relationships,and LOM,constrained by stability issues,the OPM offers a promising alternative by enabling direct O-O bond formation via dual active sites,thus bypassing^(*)OOH intermediates and lattice O involvement and achieving a balance between activity and durability.However,activating the OPM process requires precise control over the spatial and electronic structure of active sites,making the design of OPM-based catalysts challenging.While previous reviews have focused on homo/heteronuclear diatomic perspectives of OPM-based catalysts,it is urgent to systematically summarize design strategies to provide a rational reference for their development.Herein,a review of design strategies for OPM-based OER catalysts across three scales is comprehensively presented,including in-situ engineering,doping-enabled sites reconstruction,and introducing new sites for nanoparticles,direct synthesis or post-treatments for molecular catalysts,and doping or template strategies for atom pairs or arrays.The unique advantage of atom arrays is also highlighted,and their future research directions and possible strategies are discussed.This review provides a systematic summary and forward-looking perspectives for rationally designing high-performance OPM-based OER catalysts.展开更多
An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to reg...An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to regulate the p H of the solution and slow down the release of OH^-, effectively regulating the phase, nanostructure, interlayer spacing, surface area, thickness, and the performance of binary Ni –Co hydroxide. The ion-slow-release mechanism is conducive to the formation of α-phase with larger interlayer spacing and thinner flakes rather than β-phase. Attributed to the enlarged interlayer spacing, thinner nanosheets, and more exposed active sites, the resultant α-phase hydroxides(NCNS-5.2), displayed much lower over potential of 285 mV with respect to the dense-stacked β-phase hydroxides(362 mV) for OER at 10 mA/cm^2. It also exhibited high specific capacitance of 1474.2 F/g, when tested at 0.5 A/g within a voltage range of 0–0.45 Vvs. Hg/Hg O. This composite was also stable for water oxidation reaction and supercapacitor. The proof-of-concept of using controlled-release agent may provide suggestive insights for the material innovation and a variety of applications.展开更多
The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed...The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed a precursor-modified strategy for the synthesis of graphitic CN with highly efficient photocatalytic performance.The precursor dicyandiamide reformed by different acids undergoes a basic structural change and transforms into diverse new precursors.The thin porous amino-rich HNO_(3)-CN(5H-CN)was calcined by dicyandiamidine nitrate,formed by concentrated nitric acid modified dicyandiamide,and presented the best photocatalytic degradation rate of Rh B,more than 34 times that of bulk graphitic CN.Moreover,the photocatalytic hydrogen evolution rate of 5H-CN significantly improved.The TG-DSC-FTIR analyses indicated that the distinguishing thermal polymerization process of 5H-CN led to its thin porous amino-rich structure,and the theoretical calculations revealed that the negative conduction band potential of 5H-CN was attributed to its amino-rich structure.It is anticipated that the thin porous structure and the negative conduction band position of 5H-CN play important roles in the improvement of the photocatalytic performance.This study demonstrates that precursor modification is a promising project to induce a new thermal polycondensation process for the synthesis of CN with enhanced photocatalytic performance.展开更多
The issues of fossil energy shortage and environmental pollution caused by the excessive consumption of conventional fossil fuels necessitates the exploration of renewable and clean energy sources such as hydrogen,whi...The issues of fossil energy shortage and environmental pollution caused by the excessive consumption of conventional fossil fuels necessitates the exploration of renewable and clean energy sources such as hydrogen,which is viable alternative to traditional energy sources in view of its high energy density and nonpolluting nature.In this regard,photocatalytic technology powered by inexhaustible solar energy is an ideal hydrogen production method.The recently developed copper-and zinc-based multinary metal sulfide(MMS)semiconductor photocatalysts exhibit the advantages of suitable bandgap,wide light-harvesting range,and flexible elemental composition,thus possessing great potential for achieving considerable photocatalytic hydrogen evolution(PHE)performance.Despite great progress has been achieved,the current photocatalysts still cannot meet the commercial application demands,which highlights the mechanisms understanding and optimization strategies for efficient PHE.Herein,the basic mechanisms of PHE,and effective optimization strategies are firstly introduced.Afterwards,the research process and the performance of copper-and zinc-based MMS photocatalysts,are thoroughly reviewed.Finally,the unresolved issues,and challenges hindering the achievement of overall water splitting have been discussed.展开更多
Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous ...Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO_(2) surface coating is proposed.Yttrium doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond energy.LiYO_(2) nanocoating has the function of structural constraint and protection,that protecting the lattice oxygen exposed to the surface,thus avoiding irreversible oxidation.As an Li^(+) conductor,LiYO_(2) nano-coating can provide a fast Li^(+) transfer channel,which enables the sample to have excellent rate performance.The synergistic effect of Y doping and nano-LiYO_(2) coating integration suppresses the oxygen release from the surface,accelerates the diffusion of Li^(+)from electrolyte to electrode and decreases the interfacial side reactions,enabling the lithium ion batteries to obtain good electrochemical performance.The lithium-ion full cell employing the Y-1 sample(cathode)and commercial graphite(anode)exhibit an excellent specific energy density of 442.9 Wh kg^(-1) at a current density of 0.1C,with very stable safety performance,which can be used in a wide temperature range(60 to-15℃)stable operation.This result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.展开更多
When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution...When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution mechanisms that allow for unmanned clusters to maximize their overall task effective-ness under the condition of strategic diversity.This paper ana-lyzes these task requirements from three perspectives:the diver-sity of the decision space,information network construction,and the autonomous collaboration mechanism.Then,this paper pro-poses a method for solving the problem of strategy selection diversity under two network structures.Next,this paper presents a Moran-rule-based evolution dynamics model for unmanned cluster strategies and a vision-driven-mechanism-based evolu-tion dynamics model for unmanned cluster strategy in the con-text of strategy selection diversity according to various unmanned cluster application scenarios.Finally,this paper pro-vides a simulation analysis of the effects of relevant parameters such as the payoff factor and cluster size on cooperative evolu-tion in autonomous cluster collaboration for the two types of models.On this basis,this paper presents advice for effectively addressing diverse choices in unmanned cluster tasks,thereby providing decision support for practical applications of unmanned cluster tasks.展开更多
The development of atomically dispersed platinum-based catalysts with high performance and welldefined active site structures is crucial for the commercialization of water electrolysis for hydrogen production.Herein,w...The development of atomically dispersed platinum-based catalysts with high performance and welldefined active site structures is crucial for the commercialization of water electrolysis for hydrogen production.Herein,we propose a coordination dual-shell synergistic regulation mechanism of coal pitchderived carbon-supported single atom Pt-N_(x)O_(y)-S_(1)catalytic sites by a self-assembly-pyrolysis strategy for promoting hydrogen evolution reaction(HER).The Pt-N_(3)O1-S_(1)sites exhibited the highest HER performance,with an overpotential of 92 mV at a current density of 400 mA cm^(-2).At 50 mV,the turnover frequency was 34.04 s^(-1)and the mass activity was 22.83 A mg_(Pt)^(-l),which is 63.4 times that of the 20%Pt/C catalyst.Theoretical calculations revealed that the coordination dual-shell impacts the electronic structure of the Pt atoms and the adsorption strength towards reactants synergistically.The S atoms in the second coordination shell weakened the strength of Pt-N first shell,resulting the more surface valence electrons around Pt atoms,exhibiting the most suitable adsorption free energy and enhancing the adsorption of H^(+)on Pt-N_(3)O_(1)-S_(1)sites,thus enhancing the electrocatalytic HER process by promoting Volmer step.This work reveals that coordination dual-shell synergistic regulation is an effective strategy for enhancing the electrocatalytic reaction process.展开更多
Overall figures of rural settlement landscapes on Guanzhong Plain were summarized,material components of these landscapes were classified into living landscape facilities and production landscape facilities,and then i...Overall figures of rural settlement landscapes on Guanzhong Plain were summarized,material components of these landscapes were classified into living landscape facilities and production landscape facilities,and then introduced respectively.From the perspective of rural central landscapes,rural yard landscapes,rural cluster landscapes and rural road landscapes,evolution of rural landscape spatial forms on Guanzhong Plain was analyzed.Moreover,problems of present rural landscapes were proposed,necessity and urgency of controlling evolution of rural settlement landscapes were stressed,and a rural landscape control mode in view of regional characteristics of Guanzhong Plain was given.展开更多
In China, rural settlements are usually multifunctional complex of natural societies and they also play important productive function. This study explored the spatiotemporal evolution of the productive function of thr...In China, rural settlements are usually multifunctional complex of natural societies and they also play important productive function. This study explored the spatiotemporal evolution of the productive function of three rural settlements, i.e.,Hetaoyuan, Dawengshan, and Gaoqiao, in the Yimeng Mountain in Shandong province of eastern China.Residents lived in this three types of rural settlements were all involved in agricultural production(i.e., grain threshing, drying and storage), which had remained dominant in Hetaoyuan. Dawengshan became an industrial-oriented settlement, while Gaoqiao became a commercial-oriented settlement. This evolution was reflected in the livelihood strategy changes of rural households and the transition of rural settlements changes. The choice of livelihood strategy was affected by the livelihood assets and policies, which resulted in the spatiotemporal evolution of the productive function of rural settlements. This study can provide references for the implementation and adjustment of rural residential land consolidation policies and the improvement of production and the quality of rural life in future.展开更多
Repeated games describe situations where players interact with each other in a dynamic pattern and make decisions ac- cording to outcomes of previous stage games. Very recently, Press and Dyson have revealed a new cla...Repeated games describe situations where players interact with each other in a dynamic pattern and make decisions ac- cording to outcomes of previous stage games. Very recently, Press and Dyson have revealed a new class of zero-determinant (ZD) strategies for the repeated games, which can enforce a fixed linear relationship between expected payoffs of two play- ers, indicating that a smart player can control her unwitting co-player's payoff in a unilateral way [Proc. Acad. Natl. Sci. USA 109, 10409 (2012)]. The theory of ZD strategies provides a novel viewpoint to depict interactions among players, and fundamentally changes the research paradigm of game theory. In this brief survey, we first introduce the mathematical framework of ZD strategies, and review the properties and constrains of two specifications of ZD strategies, called pinning strategies and extortion strategies. Then we review some representative research progresses, including robustness analysis, cooperative ZD strategy analysis, and evolutionary stability analysis. Finally, we discuss some significant extensions to ZD strategies, including the multi-player ZD strategies, and ZD strategies under noise. Challenges in related research fields are also listed.展开更多
Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via el...Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.展开更多
Starch,as a typical polysaccharide with natural spherical morphology,is not only a preferred precursor for preparing carbon materials but also a model polymer for investigating thermochemical evolution mechanisms.Howe...Starch,as a typical polysaccharide with natural spherical morphology,is not only a preferred precursor for preparing carbon materials but also a model polymer for investigating thermochemical evolution mechanisms.However,starch usually suffers from severe foaming and low carbon yield during direct pyrolysis.Herein,we report a simple and eco-friendly dry strategy,by maleic anhydride initiating the esterification of starch,to design carbon microspheres against the starch foaming.Moreover,the infuence of ester grafting on the pyrolytic behavior of starch is also focused.The formation of ester groups in precursor guarantees the structural stability of starch-based intermediate because it can promote the accumulation of unsaturated species and accelerate the water elimination during pyrolysis.Meanwhile,the esterification and dehydration reactions greatly deplete the primary hydroxyl groups in the starch molecules and thus the rapid levoglucosan release is inhibited,which well keeps the spherical morphology of starch and ensures the high carbon yield.In further exploration as anode materials for Lithium-ion batteries,the obtained carbon microspheres exhibit good cyclability and rate performance with a reversible capacity of 444 m Ah g^(-1)at 50 m A g^(-1).This work provides theoretical fundamentals for the controllable thermal transformation of biomass towards wide applications.展开更多
As each type of satellite network has different link features, its data transmission must be designed based on its link features to improve the efficiency of data transferring. The transmission of navigation integrate...As each type of satellite network has different link features, its data transmission must be designed based on its link features to improve the efficiency of data transferring. The transmission of navigation integrated services information (NISI) in a global navigation satellite system (GNSS) with inter-satellite links (ISLs) is studied by taking the real situation of inter-satellite communication links into account. An on-demand computing and buffering centralized route strategy is proposed based on dynamic grouping and the topology evolution law of the GNSS network within which the satellite nodes are operated in the manner of dynamic grouping. Dynamic grouping is based on satellites spatial relationships and the group role of the satellite node changes by turns due to its spatial relationships. The route strategy provides significant advantages of high efficiency, low complexity, and flexi- ble configuration, by which the established GNSS can possess the features and capabilities of feasible deployment, efficient transmission, convenient management, structural invulnerability and flexible expansion.展开更多
Petrographic analysis combined with various techniques, such as thin section identification, fluid inclusions, isotopic data, petro-physical property testing and oil testing results, was used to study diagenetic evolu...Petrographic analysis combined with various techniques, such as thin section identification, fluid inclusions, isotopic data, petro-physical property testing and oil testing results, was used to study diagenetic evolution and its effect on reservoir-quality of fan delta reservoirs of Es4s in the Bonan sag. The diagenesis is principally characterized by strong compaction, undercompaction, multi-phase of dissolution and cementation. Compaction played a more important role than cementation in destroying the primary porosity of the sandstones. The reservoirs have experienced complicated diagenetic environment evolution of "weak alkalineacid-alkalinity-acid-weak alkalinity" and two-stage of hydrocarbon filling. The diagenetic sequences are summarized as "early compaction/early pyrite/gypsum/calcite/dolomite cementation→feldspar dissolution/the first stage of quartz overgrowth → early hydrocarbon filling→quartz dissolution/anhydrite/Fe-carbonate cementation→Fe-carbonate dissolution/feldspar dissolution/ the second stage of quartz overgrowth→later hydrocarbon filling→later pyrite cementation. In the same diagenetic context, the diagenetic evolution processes that occurred in different sub/micro-facies during progressive burial have resulted in heterogeneous reservoir properties and oiliness. The braided channel reservoirs in fan delta plain are poorly sorted with high matrix contents. The physical properties decrease continually due to the principally strong compaction and weak dissolution. The present properties of braided channel reservoirs are extremely poor, which is evidenced by few oil layers developed in relatively shallow strata while dry layers entirely in deep. The reservoirs both in the underwater distributary channels and mouth bars are well sorted and have a strong ability to resist compaction. Abundant pores are developed in medium-deep strata because of modifications by two-stage of acidic dissolution and hydrocarbon filling. The present properties are relatively well both in the underwater distributary channels and mouth bars and plenty of oil layers are developed in different burial depth. The present reservoir properties both in interdistributary channel and pre-fan delta are poor caused by extensively cementation. Small amounts of oil layers, oil-water layers and oil-bearing layers are developed in relatively shallow strata while dry layers totally in deep.展开更多
The development of inexpensive and efficient electrocatalysts is key to commercializing energy-related electrocatalytic techniques such as water electrolyzers and metal-air batteries.In particular,novel oxygen evoluti...The development of inexpensive and efficient electrocatalysts is key to commercializing energy-related electrocatalytic techniques such as water electrolyzers and metal-air batteries.In particular,novel oxygen evolution reaction(OER)pre-catalysts,such as transition metal chalcogenides(TMCs)and phosphides(TMPs),have evolved in recent years from traditional stable OER electrocatalysts,which show superior OER electrocatalytic performance compared with transition metal oxides(TMOs)or(oxy)hydroxides(TMOHs).In this feature article,we summarize recent advances in the development of TMCand TMP-based OER electrocatalysts,as well as approaches to improve the OER performance in terms of morphology,structure,composition,surface engineering,lattice-strained and in-situ transformation in the electrolysis process.In particular,the electrochemical stability of TMCs and TMPs in alkaline electrolytes and the evolution of morphology,structure and composition under OER conditions are discussed.In the last section,we discuss the challenges that need to be addressed in this specific area of research and the implications for further research.展开更多
Learning control has been recognized as a powerful approach in quantum information technology. In this paper, we extend the application of differential evolution (DE) to design optimal control for various quantum sy...Learning control has been recognized as a powerful approach in quantum information technology. In this paper, we extend the application of differential evolution (DE) to design optimal control for various quantum systems. Various DE methods are introduced and analyzed, and EMSDE featuring in equally mixed strategies is employed for quantum control. Two classes of quantum control problems, including control of four-level open quantum ensembles and quantum superconducting systems, are investigated to demonstrate the performance of EMSDE for learning control of quantum systems. Numerical results verify the effectiveness of the FMSDE method for various quantum systems and show the potential for complex quantum control problems.展开更多
Northeast China, as the most important production base of agriculture, forestry, and livestock-breeding as well as the old industrial base in the whole country, has been playin a key role in the construction and deve...Northeast China, as the most important production base of agriculture, forestry, and livestock-breeding as well as the old industrial base in the whole country, has been playin a key role in the construction and development of China's economy. However, after the policy of reform and open-up was taken in China. the economic development speed and efficiency ofthis area have turned to be evidently lower than those of coastal area and the national average level as well, which is so-called 'Northeast Phenomenon' and 'Neo-Northeast Phenomenon'. In terms of those phenomena, this paper firstly reviews the spatial and temporal features of the regional evolution of this area so as to unveil the profound forming causes of 'Northeast Phenomena' and 'Neo-Northeast Phenomena'. And then the paper makes a further exploration into the status quo of this region and its forming causes by analyzing its economy gross, industrial structure, product structure, regional eco-categories, etc. At the end of the paper, the authors put forward the basic coordinated development strategies for Northeast China. namely we can revitalize this area by means of adjustment of economic structure, regional coordination, planning urban and rural areas as a whole, institutional innovation, etc.展开更多
The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution ...The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution depends on the development of low-cost and highly active electrocatalysts.Molybdenum carbides(MoxC),as a typical of earth-abundant transition-metal material,have accumulated great attention due to their low cost,earth abundance,electrical conductivity,similar d-band state to Pt,and regulated morphology/electronic structures.In this paper,recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology,electronic structure,and electrode interface step by step.Briefly,modulation of morphology influence the apparent activity of catalyst,modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics,and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the activity.Besides the above methods discussed,perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.展开更多
基金financially supported by the National Natural Science Foundation of China(52302084)the National Key Research and Development Program of China(2022YFE0138900)+1 种基金Fundamental Research Funds for the Central Universities(2232025D-24)the Qin Shen Scholar Program of Jiaxing University。
文摘The development of economical,highly efficient,and stable bifunctional electrocatalysts for both the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR)remains a critical focus in advancing rechargeable metal-air battery systems.Significant progress has been made in the design of high-performance bifunctional electrocatalysts,the development of novel oxygen electrode architectures,and the in-depth understanding of electrocatalytic mechanisms through combined experimental and computational studies.This work provides a comprehensive review of recent advancements in design strategies for oxygen catalysts,including homogeneous electrodes,asymmetric electrodes,and biomimetic electrodes,are thoroughly discussed and summarized.Then,the advanced catalyst modification strategies for ORR/OER are summarized,focusing on critical factors such as enhancement effect of metal/nonmental and synergistic enhancement effect in multiple catalyst.Subsequently,a representative performance evaluation is presented,based on the reported oxygen electrodes used in rechargeable metal-air battery applications.By focusing on these key areas,the review outlines the current challenges and future prospects for the development of bifunctional oxygen electrocatalysts,aiming to guide the design of high-performance bifunctional electrocatalysts and to elucidate the underlying mechanisms involved.
基金funding from the National Natural Science Foundation of China(22378289)the Key Central Government Guides Local Funds for Science and Technology Development(YDZJSX2022A021)the special fund for Science and Technology Innovation Teams of Shanxi Province(202304051001026)。
文摘The oxygen evolution reaction(OER)suffers from sluggish kinetics,necessitating efficient electrocatalysts to reduce overpotentials in water splitting.Currently recognized OER mechanisms primarily include the adsorbate evolution mechanism(AEM),lattice oxygen mechanism(LOM),and oxide path mechanism(OPM).Compared to AEM,limited by scaling relationships,and LOM,constrained by stability issues,the OPM offers a promising alternative by enabling direct O-O bond formation via dual active sites,thus bypassing^(*)OOH intermediates and lattice O involvement and achieving a balance between activity and durability.However,activating the OPM process requires precise control over the spatial and electronic structure of active sites,making the design of OPM-based catalysts challenging.While previous reviews have focused on homo/heteronuclear diatomic perspectives of OPM-based catalysts,it is urgent to systematically summarize design strategies to provide a rational reference for their development.Herein,a review of design strategies for OPM-based OER catalysts across three scales is comprehensively presented,including in-situ engineering,doping-enabled sites reconstruction,and introducing new sites for nanoparticles,direct synthesis or post-treatments for molecular catalysts,and doping or template strategies for atom pairs or arrays.The unique advantage of atom arrays is also highlighted,and their future research directions and possible strategies are discussed.This review provides a systematic summary and forward-looking perspectives for rationally designing high-performance OPM-based OER catalysts.
基金supported by the National Natural Science Foundation of China(21476145)
文摘An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to regulate the p H of the solution and slow down the release of OH^-, effectively regulating the phase, nanostructure, interlayer spacing, surface area, thickness, and the performance of binary Ni –Co hydroxide. The ion-slow-release mechanism is conducive to the formation of α-phase with larger interlayer spacing and thinner flakes rather than β-phase. Attributed to the enlarged interlayer spacing, thinner nanosheets, and more exposed active sites, the resultant α-phase hydroxides(NCNS-5.2), displayed much lower over potential of 285 mV with respect to the dense-stacked β-phase hydroxides(362 mV) for OER at 10 mA/cm^2. It also exhibited high specific capacitance of 1474.2 F/g, when tested at 0.5 A/g within a voltage range of 0–0.45 Vvs. Hg/Hg O. This composite was also stable for water oxidation reaction and supercapacitor. The proof-of-concept of using controlled-release agent may provide suggestive insights for the material innovation and a variety of applications.
文摘The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed a precursor-modified strategy for the synthesis of graphitic CN with highly efficient photocatalytic performance.The precursor dicyandiamide reformed by different acids undergoes a basic structural change and transforms into diverse new precursors.The thin porous amino-rich HNO_(3)-CN(5H-CN)was calcined by dicyandiamidine nitrate,formed by concentrated nitric acid modified dicyandiamide,and presented the best photocatalytic degradation rate of Rh B,more than 34 times that of bulk graphitic CN.Moreover,the photocatalytic hydrogen evolution rate of 5H-CN significantly improved.The TG-DSC-FTIR analyses indicated that the distinguishing thermal polymerization process of 5H-CN led to its thin porous amino-rich structure,and the theoretical calculations revealed that the negative conduction band potential of 5H-CN was attributed to its amino-rich structure.It is anticipated that the thin porous structure and the negative conduction band position of 5H-CN play important roles in the improvement of the photocatalytic performance.This study demonstrates that precursor modification is a promising project to induce a new thermal polycondensation process for the synthesis of CN with enhanced photocatalytic performance.
文摘The issues of fossil energy shortage and environmental pollution caused by the excessive consumption of conventional fossil fuels necessitates the exploration of renewable and clean energy sources such as hydrogen,which is viable alternative to traditional energy sources in view of its high energy density and nonpolluting nature.In this regard,photocatalytic technology powered by inexhaustible solar energy is an ideal hydrogen production method.The recently developed copper-and zinc-based multinary metal sulfide(MMS)semiconductor photocatalysts exhibit the advantages of suitable bandgap,wide light-harvesting range,and flexible elemental composition,thus possessing great potential for achieving considerable photocatalytic hydrogen evolution(PHE)performance.Despite great progress has been achieved,the current photocatalysts still cannot meet the commercial application demands,which highlights the mechanisms understanding and optimization strategies for efficient PHE.Herein,the basic mechanisms of PHE,and effective optimization strategies are firstly introduced.Afterwards,the research process and the performance of copper-and zinc-based MMS photocatalysts,are thoroughly reviewed.Finally,the unresolved issues,and challenges hindering the achievement of overall water splitting have been discussed.
基金This work was supported by the Fundamental Research Funds for the Central Universities(DUT20LAB123 and DUT20LAB307)the Natural Science Foundation of Jiangsu Province(BK20191167).
文摘Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO_(2) surface coating is proposed.Yttrium doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond energy.LiYO_(2) nanocoating has the function of structural constraint and protection,that protecting the lattice oxygen exposed to the surface,thus avoiding irreversible oxidation.As an Li^(+) conductor,LiYO_(2) nano-coating can provide a fast Li^(+) transfer channel,which enables the sample to have excellent rate performance.The synergistic effect of Y doping and nano-LiYO_(2) coating integration suppresses the oxygen release from the surface,accelerates the diffusion of Li^(+)from electrolyte to electrode and decreases the interfacial side reactions,enabling the lithium ion batteries to obtain good electrochemical performance.The lithium-ion full cell employing the Y-1 sample(cathode)and commercial graphite(anode)exhibit an excellent specific energy density of 442.9 Wh kg^(-1) at a current density of 0.1C,with very stable safety performance,which can be used in a wide temperature range(60 to-15℃)stable operation.This result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.
基金supported by the National Natural Science Foundation of China(72471240).
文摘When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution mechanisms that allow for unmanned clusters to maximize their overall task effective-ness under the condition of strategic diversity.This paper ana-lyzes these task requirements from three perspectives:the diver-sity of the decision space,information network construction,and the autonomous collaboration mechanism.Then,this paper pro-poses a method for solving the problem of strategy selection diversity under two network structures.Next,this paper presents a Moran-rule-based evolution dynamics model for unmanned cluster strategies and a vision-driven-mechanism-based evolu-tion dynamics model for unmanned cluster strategy in the con-text of strategy selection diversity according to various unmanned cluster application scenarios.Finally,this paper pro-vides a simulation analysis of the effects of relevant parameters such as the payoff factor and cluster size on cooperative evolu-tion in autonomous cluster collaboration for the two types of models.On this basis,this paper presents advice for effectively addressing diverse choices in unmanned cluster tasks,thereby providing decision support for practical applications of unmanned cluster tasks.
基金supported by the National Natural Science Foundation of China(22108306,22478432 and 22406191)Taishan Scholars Program of Shandong Province(tsqn201909065)the Natural Science Foundation of Shandong Province(ZR2024JQ004,ZR2021YQ15)。
文摘The development of atomically dispersed platinum-based catalysts with high performance and welldefined active site structures is crucial for the commercialization of water electrolysis for hydrogen production.Herein,we propose a coordination dual-shell synergistic regulation mechanism of coal pitchderived carbon-supported single atom Pt-N_(x)O_(y)-S_(1)catalytic sites by a self-assembly-pyrolysis strategy for promoting hydrogen evolution reaction(HER).The Pt-N_(3)O1-S_(1)sites exhibited the highest HER performance,with an overpotential of 92 mV at a current density of 400 mA cm^(-2).At 50 mV,the turnover frequency was 34.04 s^(-1)and the mass activity was 22.83 A mg_(Pt)^(-l),which is 63.4 times that of the 20%Pt/C catalyst.Theoretical calculations revealed that the coordination dual-shell impacts the electronic structure of the Pt atoms and the adsorption strength towards reactants synergistically.The S atoms in the second coordination shell weakened the strength of Pt-N first shell,resulting the more surface valence electrons around Pt atoms,exhibiting the most suitable adsorption free energy and enhancing the adsorption of H^(+)on Pt-N_(3)O_(1)-S_(1)sites,thus enhancing the electrocatalytic HER process by promoting Volmer step.This work reveals that coordination dual-shell synergistic regulation is an effective strategy for enhancing the electrocatalytic reaction process.
文摘Overall figures of rural settlement landscapes on Guanzhong Plain were summarized,material components of these landscapes were classified into living landscape facilities and production landscape facilities,and then introduced respectively.From the perspective of rural central landscapes,rural yard landscapes,rural cluster landscapes and rural road landscapes,evolution of rural landscape spatial forms on Guanzhong Plain was analyzed.Moreover,problems of present rural landscapes were proposed,necessity and urgency of controlling evolution of rural settlement landscapes were stressed,and a rural landscape control mode in view of regional characteristics of Guanzhong Plain was given.
基金supported by the National Natural Science Foundation of China(Grant Nos.41671519 and 41771560)
文摘In China, rural settlements are usually multifunctional complex of natural societies and they also play important productive function. This study explored the spatiotemporal evolution of the productive function of three rural settlements, i.e.,Hetaoyuan, Dawengshan, and Gaoqiao, in the Yimeng Mountain in Shandong province of eastern China.Residents lived in this three types of rural settlements were all involved in agricultural production(i.e., grain threshing, drying and storage), which had remained dominant in Hetaoyuan. Dawengshan became an industrial-oriented settlement, while Gaoqiao became a commercial-oriented settlement. This evolution was reflected in the livelihood strategy changes of rural households and the transition of rural settlements changes. The choice of livelihood strategy was affected by the livelihood assets and policies, which resulted in the spatiotemporal evolution of the productive function of rural settlements. This study can provide references for the implementation and adjustment of rural residential land consolidation policies and the improvement of production and the quality of rural life in future.
基金supported by the National Natural Science Foundation of China(Grant Nos.61004098 and 11222543)the Program for New Century Excellent Talentsin Universities of China(Grant No.NCET-11-0070)+2 种基金the Special Project of Youth Science and Technology Innovation Research Team of Sichuan ProvinceChina(Grant No.2013TD0006)the Research Foundation of UESTC and Scholars Program of Hong Kong(Grant No.G-YZ4D)
文摘Repeated games describe situations where players interact with each other in a dynamic pattern and make decisions ac- cording to outcomes of previous stage games. Very recently, Press and Dyson have revealed a new class of zero-determinant (ZD) strategies for the repeated games, which can enforce a fixed linear relationship between expected payoffs of two play- ers, indicating that a smart player can control her unwitting co-player's payoff in a unilateral way [Proc. Acad. Natl. Sci. USA 109, 10409 (2012)]. The theory of ZD strategies provides a novel viewpoint to depict interactions among players, and fundamentally changes the research paradigm of game theory. In this brief survey, we first introduce the mathematical framework of ZD strategies, and review the properties and constrains of two specifications of ZD strategies, called pinning strategies and extortion strategies. Then we review some representative research progresses, including robustness analysis, cooperative ZD strategy analysis, and evolutionary stability analysis. Finally, we discuss some significant extensions to ZD strategies, including the multi-player ZD strategies, and ZD strategies under noise. Challenges in related research fields are also listed.
文摘Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.
基金supported by the National Science Foundation for Excellent Young Scholars of China(21922815)the Key Research and Development(R&D)Projects of Shanxi Province(201903D121180)the National Key Research and Development(R&D)Program of China。
文摘Starch,as a typical polysaccharide with natural spherical morphology,is not only a preferred precursor for preparing carbon materials but also a model polymer for investigating thermochemical evolution mechanisms.However,starch usually suffers from severe foaming and low carbon yield during direct pyrolysis.Herein,we report a simple and eco-friendly dry strategy,by maleic anhydride initiating the esterification of starch,to design carbon microspheres against the starch foaming.Moreover,the infuence of ester grafting on the pyrolytic behavior of starch is also focused.The formation of ester groups in precursor guarantees the structural stability of starch-based intermediate because it can promote the accumulation of unsaturated species and accelerate the water elimination during pyrolysis.Meanwhile,the esterification and dehydration reactions greatly deplete the primary hydroxyl groups in the starch molecules and thus the rapid levoglucosan release is inhibited,which well keeps the spherical morphology of starch and ensures the high carbon yield.In further exploration as anode materials for Lithium-ion batteries,the obtained carbon microspheres exhibit good cyclability and rate performance with a reversible capacity of 444 m Ah g^(-1)at 50 m A g^(-1).This work provides theoretical fundamentals for the controllable thermal transformation of biomass towards wide applications.
文摘As each type of satellite network has different link features, its data transmission must be designed based on its link features to improve the efficiency of data transferring. The transmission of navigation integrated services information (NISI) in a global navigation satellite system (GNSS) with inter-satellite links (ISLs) is studied by taking the real situation of inter-satellite communication links into account. An on-demand computing and buffering centralized route strategy is proposed based on dynamic grouping and the topology evolution law of the GNSS network within which the satellite nodes are operated in the manner of dynamic grouping. Dynamic grouping is based on satellites spatial relationships and the group role of the satellite node changes by turns due to its spatial relationships. The route strategy provides significant advantages of high efficiency, low complexity, and flexi- ble configuration, by which the established GNSS can possess the features and capabilities of feasible deployment, efficient transmission, convenient management, structural invulnerability and flexible expansion.
基金Project(41102058)supported by the National Natural Science Foundation of ChinaProject(2011ZX05006-003)supported by National Oil&Gas Major Project of China+1 种基金Project(U1262203)supported by Key Program for National Natural Science Foundation of ChinaProject(LW140101A)for Excellent Doctoral Dissertation supported by China University of Petroleum,China
文摘Petrographic analysis combined with various techniques, such as thin section identification, fluid inclusions, isotopic data, petro-physical property testing and oil testing results, was used to study diagenetic evolution and its effect on reservoir-quality of fan delta reservoirs of Es4s in the Bonan sag. The diagenesis is principally characterized by strong compaction, undercompaction, multi-phase of dissolution and cementation. Compaction played a more important role than cementation in destroying the primary porosity of the sandstones. The reservoirs have experienced complicated diagenetic environment evolution of "weak alkalineacid-alkalinity-acid-weak alkalinity" and two-stage of hydrocarbon filling. The diagenetic sequences are summarized as "early compaction/early pyrite/gypsum/calcite/dolomite cementation→feldspar dissolution/the first stage of quartz overgrowth → early hydrocarbon filling→quartz dissolution/anhydrite/Fe-carbonate cementation→Fe-carbonate dissolution/feldspar dissolution/ the second stage of quartz overgrowth→later hydrocarbon filling→later pyrite cementation. In the same diagenetic context, the diagenetic evolution processes that occurred in different sub/micro-facies during progressive burial have resulted in heterogeneous reservoir properties and oiliness. The braided channel reservoirs in fan delta plain are poorly sorted with high matrix contents. The physical properties decrease continually due to the principally strong compaction and weak dissolution. The present properties of braided channel reservoirs are extremely poor, which is evidenced by few oil layers developed in relatively shallow strata while dry layers entirely in deep. The reservoirs both in the underwater distributary channels and mouth bars are well sorted and have a strong ability to resist compaction. Abundant pores are developed in medium-deep strata because of modifications by two-stage of acidic dissolution and hydrocarbon filling. The present properties are relatively well both in the underwater distributary channels and mouth bars and plenty of oil layers are developed in different burial depth. The present reservoir properties both in interdistributary channel and pre-fan delta are poor caused by extensively cementation. Small amounts of oil layers, oil-water layers and oil-bearing layers are developed in relatively shallow strata while dry layers totally in deep.
基金supported by the National Natural Science Foundation of China (No.22179014)the China Postdoctoral Science Foundation (No.2022 M720593)+2 种基金the Scientific Research Foundation of Chongqing University of Technology (Nos.2022ZDZ011,2022PYZ026)the Youth Project of Science and Technology Research Program of Chongqing Municipal Education Commission (No.KJQN202201127)the Project of Natural Science Foundation of Chongqing (No.2022NSCQ-MSX1123)。
文摘The development of inexpensive and efficient electrocatalysts is key to commercializing energy-related electrocatalytic techniques such as water electrolyzers and metal-air batteries.In particular,novel oxygen evolution reaction(OER)pre-catalysts,such as transition metal chalcogenides(TMCs)and phosphides(TMPs),have evolved in recent years from traditional stable OER electrocatalysts,which show superior OER electrocatalytic performance compared with transition metal oxides(TMOs)or(oxy)hydroxides(TMOHs).In this feature article,we summarize recent advances in the development of TMCand TMP-based OER electrocatalysts,as well as approaches to improve the OER performance in terms of morphology,structure,composition,surface engineering,lattice-strained and in-situ transformation in the electrolysis process.In particular,the electrochemical stability of TMCs and TMPs in alkaline electrolytes and the evolution of morphology,structure and composition under OER conditions are discussed.In the last section,we discuss the challenges that need to be addressed in this specific area of research and the implications for further research.
基金This paper is dedicated to Professor lan R. Petersen on the occasion of his 60th birthday. This work was supported by the National Natural Science Foundation of China (Nos. 61374092, 61432008), the National Key Research and Development Program of China (No. 2016YFD0702100) and the Australian Research Council's Discovery Projects funding scheme under Project DP130101658.
文摘Learning control has been recognized as a powerful approach in quantum information technology. In this paper, we extend the application of differential evolution (DE) to design optimal control for various quantum systems. Various DE methods are introduced and analyzed, and EMSDE featuring in equally mixed strategies is employed for quantum control. Two classes of quantum control problems, including control of four-level open quantum ensembles and quantum superconducting systems, are investigated to demonstrate the performance of EMSDE for learning control of quantum systems. Numerical results verify the effectiveness of the FMSDE method for various quantum systems and show the potential for complex quantum control problems.
基金Under the auspices of National Natural Science Foundation of China (No. 40471040)
文摘Northeast China, as the most important production base of agriculture, forestry, and livestock-breeding as well as the old industrial base in the whole country, has been playin a key role in the construction and development of China's economy. However, after the policy of reform and open-up was taken in China. the economic development speed and efficiency ofthis area have turned to be evidently lower than those of coastal area and the national average level as well, which is so-called 'Northeast Phenomenon' and 'Neo-Northeast Phenomenon'. In terms of those phenomena, this paper firstly reviews the spatial and temporal features of the regional evolution of this area so as to unveil the profound forming causes of 'Northeast Phenomena' and 'Neo-Northeast Phenomena'. And then the paper makes a further exploration into the status quo of this region and its forming causes by analyzing its economy gross, industrial structure, product structure, regional eco-categories, etc. At the end of the paper, the authors put forward the basic coordinated development strategies for Northeast China. namely we can revitalize this area by means of adjustment of economic structure, regional coordination, planning urban and rural areas as a whole, institutional innovation, etc.
基金financial support from Shandong Provincial Natural Science Foundation(ZR2017MB059)the National Natural Science Foundation of China(21776314)the Fundamental Research Funds for the Central Universities(18CX05016A)。
文摘The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution depends on the development of low-cost and highly active electrocatalysts.Molybdenum carbides(MoxC),as a typical of earth-abundant transition-metal material,have accumulated great attention due to their low cost,earth abundance,electrical conductivity,similar d-band state to Pt,and regulated morphology/electronic structures.In this paper,recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology,electronic structure,and electrode interface step by step.Briefly,modulation of morphology influence the apparent activity of catalyst,modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics,and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the activity.Besides the above methods discussed,perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.