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
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
The path to searching for sustainable energy has never stopped since thedepletion of fossil fuels can lead to serious environmental pollution andenergy shortages.Using water electrolysis to produce hydrogen has beenpr...The path to searching for sustainable energy has never stopped since thedepletion of fossil fuels can lead to serious environmental pollution andenergy shortages.Using water electrolysis to produce hydrogen has beenproven to be a prioritized approach for green resource production.It is highlycrucial to explore inexpensive and high-performance electrocatalysts foraccelerating hydrogen evolution reaction(HER)and apply them to industrialcases on a large scale.Here,we summarize the different mechanisms of HERin different pH settings and review recent advances in non-noble-metal-basedelectrocatalysts.Then,based on the previous efforts,we discuss severaluniversal strategies for designing pH-independent catalysts and showdirections for the future design of pH-universal 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
Traditional petroleum system theories emphasize the restoration of the accumulation process from“source”to“trap”.The main oil and gas resources in the concept are conventional oil and gas,lacking the concept and r...Traditional petroleum system theories emphasize the restoration of the accumulation process from“source”to“trap”.The main oil and gas resources in the concept are conventional oil and gas,lacking the concept and research of unconventional oil and gas enrichment mechanism.The whole petroleum system is developed from the traditional petroleum system.Combined with unconventional oil and gas exploration practices and discoveries such as shale oil and gas,the whole petroleum system adds the research content of unconventional oil and gas.Although the study of the whole petroleum system is still in three aspects:geological elements,dynamic evolution and oil and gas distribution,its research ideas and research contents are very different,including the following three aspects.(1)In terms of geological elements,the traditional petroleum system studies the characteristics of source rocks and hydrocarbon generation evolution,and the reservoir properties,traps,migration and preservation conditions of conventional oil and gas.On the basis of the above research,the whole petroleum system has increased the quantitative evaluation of retained hydrocarbons,unconventional reservoir characterization,source reservoir configuration and other research contents.(2)In terms of dynamic evolution,the petroleum system studies the matching between the evolution of conventional oil and gas source rocks and the formation period of traps,while the whole petroleum system has increased the research content of the matching of unconventional reservoir densification and oil and gas charging,and the later transformation of unconventional oil and gas reservoirs.(3)In terms of oil and gas distribution,the petroleum system takes buoyancy-drived accumulation mechanism as the core to study the migration,accumulation and distribution of conventional oil and gas.The whole petroleum system adds unconventional oil and gas self-sealing accumulation mechanism and conventional-unconventional oil and gas distribution sequence,so as to determine the oil and gas distribution characteristics of the whole petroleum system.展开更多
Water splitting with proton exchange membrane water electrolyzers(PEMWE)is regarded as a promising pathway for sustainable hydrogen conversion.Additionally,oxygen evolution reaction(OER)is considered as the dominant f...Water splitting with proton exchange membrane water electrolyzers(PEMWE)is regarded as a promising pathway for sustainable hydrogen conversion.Additionally,oxygen evolution reaction(OER)is considered as the dominant factor during the whole process due to the sluggish kinetics.Among the catalysts,Rubased catalysts draw special attention because of their excellent activity and relatively low price.However,the limited stability impedes their further commercialization and tremendous efforts have been devoted to overcome this challenge.This review firstly introduces the basic mechanisms of OER.Then the evaluation protocols and techniques to investigate the stability of Ru-based catalysts are summarized.A detailed elucidation of the possible degradation mechanisms is also critically analyzed.Furthermore,effective strategies to design durable Ru-based catalysts for acidic OER are discussed.Such as heteroatom doping,phase and facet engineering,heterostructure building and support optimization.Finally,promises,perspectives and challenges in developing highly durable Ru-based catalysts for acidic OER are outlined.展开更多
Renewable energy conversion as well as water electrolysis technologies are constrained by the fact that kinetics are always slow in the electrocatalytic oxygen evolution reaction(OER).There are numerous means and stra...Renewable energy conversion as well as water electrolysis technologies are constrained by the fact that kinetics are always slow in the electrocatalytic oxygen evolution reaction(OER).There are numerous means and strategies for the enhancement of OER activity.In this paper,we systematically review the important role of anionic vacancies in enhancing the OER activity of catalysts:increasing catalyst conductivity,improving electrical conductivity,and enhancing intermediate adsorption.In order to better detect the presence of vacancies in the samples,the principle of vacancy detection is reviewed in detail in terms of both spectroscopic and microscopic characterization,and the methods of vacancy formation as well as the factors influencing the concentration of vacancies are summarized in detail.In addition,the challenges and new directions for the study of anionic vacancies are provided.Lei Wang was awarded a Ph.D.in chemistry from Jilin University in 2006 under the supervision of Prof.Shouhua Feng.He worked as a Postdoctoral Scholar in Shandong University,the State Key Laboratory of Crystal Materials from 2008 to 2010.He is currently a professor at Qingdao University of Science and Technology.His research interests mainly focus on the design and synthesis of functional organic-inorganic hybrids and porous MOFs materials,as well as their applications in photocatalysis,electrocatalysis,lithium-ion battery,etc.Jingqi Chi received her B.S.degree and Ph.D.degree from the State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China).She is currently an associate professor at Qing dao University of Science and Technology.Her research interests focus on the design and synthesis of transition metal-based nanostructures and porous MOFs materials for electrochemical applications.展开更多
Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to thei...Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.展开更多
Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous i...Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous interfacial catalyst,Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH,using a simple two-step method.In situ Raman and X-ray photoelectron spectroscopy(XPS)measurements revealed the dynamic phase change occurring during the OER process.The FeOOH layer on Ni(OH)_(2)/NiCo(OH)_(6)altered the electronic structure,facilitating the emergence of the active NiOOH phase and markedly improving OER kinetics.Significantly,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1 catalyst demonstrated a current density of 10 mA·cm^(-2)at an overpotential of merely 208 mV,accompanied by a Tafel slope of 37.72 mV·dec-1,exhibiting exceptional stability over a duration of 100 h at 10 mA·cm^(-2).Furthermore,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1(+)lIPt/C(-)electrolyzer cell showcased a remarkably low driving voltage of 1.52 V to achieve 10 mA·cm^(-2),while also displaying impressive durability under alkaline conditions for over100 h.This work enhances our understanding of the interfacial structure-activity relationship in composite catalysts,aiding the design of efficient catalysts with rapid kinetics.展开更多
Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant c...Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant challenge for practical application.Recently,twodimensional transition metal dichalcogenides(2D-TMDs)have emerged as attractive and cost-effective alternatives for efficient electrocatalysis in the HER.Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs.This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods.Subsequently,recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized.Finally,the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed.We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.展开更多
Direct electrolysis of seawater to produce green hydrogen is a more environmentally friendly process than freshwater electrolysis.The renewable energy sector exhibits tremendous interest in practical seawater electrol...Direct electrolysis of seawater to produce green hydrogen is a more environmentally friendly process than freshwater electrolysis.The renewable energy sector exhibits tremendous interest in practical seawater electrolysis techniques due to its substantial capacity to mitigate the need for freshwater consumption.With the low catalytic efficiency of the current seawater splitting process and the poor reliability of its operation,the process suffers from severe corrosion caused by chloride ions,as well as anodic competition between oxygen evolution and chlorine oxidation reactions.This review provides an overview of the latest electrocatalyst developments for promoting selectivity and stability in seawater electrolysis.Using the characterization and simulation results,as well as active machine learning,advanced electrocatalytic materials can be designed and developed,a research direction that will become increasingly important in the future.A variety of strategies are discussed in detail for designing advanced electrocatalysts in seawater electrolysis,including the surface protective layer,structural regulation by heteroatom doping and vacancies,porous structure,core-shell construction,and 3D hetero-structure construction to hinder chlorine evolution reactions.Finally,future perspectives and challenges for green hydrogen production from seawater electrolysis are also described.展开更多
As low-altitude airspace becomes increasingly accessible and eVTOL(electric vertical take-off and landing)technologies advance,the low-altitude economy has emerged as a transformative frontier in urban mobility and in...As low-altitude airspace becomes increasingly accessible and eVTOL(electric vertical take-off and landing)technologies advance,the low-altitude economy has emerged as a transformative frontier in urban mobility and industrial restructuring.Although countries face comparable technological opportunities,their development paths diverge significantly.This divergence is shaped not only by policy choices and innovation capacity but also by underlying differences in institutional architectures,resource configurations,and implementation mechanisms.This paper proposes a Development Path Evolution Model grounded in four structural elements:technological capability,institutional systems,infrastructure,and application scenarios.Based on this framework,the study identifies three archetypal path types(technology-led,institution-led,and scenario-driven)and empirically validates the model through comparative case studies of the United States,Europe,and Japan.Applying the model to China reveals a distinct"hybrid scenario-driven path",characterized by demand-responsive pilots,decentralized institutional flexibility,and strong engineering capacity.Using Shanghai as a representative case,the study outlines five strategic levers to guide its transition from a localized pilot zone to a platform-based governance hub with national and international relevance.The research contributes to theoretical understanding of path differentiation in emerging industries and provides actionable insights for developing economies with strong mobilization capacity and industrial ecosystems.展开更多
Proton exchange membrane water electrolysis(PEMWE)is a favorable technology for producing highpurity hydrogen under high current density using intermittent renewable energy.The performance of PEMWE is largely determin...Proton exchange membrane water electrolysis(PEMWE)is a favorable technology for producing highpurity hydrogen under high current density using intermittent renewable energy.The performance of PEMWE is largely determined by the oxygen evolution reaction(OER),a sluggish four-electron reaction with a high reaction barrier.Nowadays,iridium(Ir)-based catalysts are the catalysts of choice for OER due to their excellent activity and durability in acidic solution.However,its high price and unsatisfactory electrochemical performance severely restrict the PEMWE’s practical application.In this review,we initiate by introducing the current OER reaction mechanisms,namely adsorbate evolution mechanism and lattice oxygen mechanism,with degradation mechanisms discussed.Optimized strategies in the preparation of advanced Ir-based catalysts are further introduced,with merits and potential problems also discussed.The parameters that determine the performance of PEMWE are then introduced,with unsolved issues and related outlooks summarized in the end.展开更多
The transition to renewable energy sources has elevated the importance of SIBs(SIBs)as cost-effective alternatives to lithium-ion batteries(LIBs)for large-scale energy storage.This review examines the mechanisms of ga...The transition to renewable energy sources has elevated the importance of SIBs(SIBs)as cost-effective alternatives to lithium-ion batteries(LIBs)for large-scale energy storage.This review examines the mechanisms of gas generation in SIBs,identifying sources from cathode materials,anode materials,and electrolytes,which pose safety risks like swelling,leakage,and explosions.Gases such as CO_(2),H_(2),and O_(2) primarily arise from the instability of cathode materials,side reactions between electrode and electrolyte,and electrolyte decomposition under high temperatures or voltages.Enhanced mitigation strategies,encompassing electrolyte design,buffer layer construction,and electrode material optimization,are deliberated upon.Accordingly,subsequent research endeavors should prioritize long-term high-precision gas detection to bolster the safety and performance of SIBs,thereby fortifying their commercial viability and furnishing dependable solutions for large-scale energy storage and electric vehicles.展开更多
Precision medicine has become a cornerstone in modern therapeutic strategies, with nucleic acid aptamers emerging aspivotal tools due to their unique properties. These oligonucleotide fragments, selected through the S...Precision medicine has become a cornerstone in modern therapeutic strategies, with nucleic acid aptamers emerging aspivotal tools due to their unique properties. These oligonucleotide fragments, selected through the Systematic Evolution ofLigands by Exponential Enrichment process, exhibit high affinity and specificity toward their targets, such as DNA, RNA,proteins, and other biomolecules. Nucleic acid aptamers offer significant advantages over traditional therapeutic agents,including superior biological stability, minimal immunogenicity, and the capacity for universal chemical modifications thatenhance their in vivo performance and targeting precision. In the realm of osseous tissue repair and regeneration, a complexphysiological process essential for maintaining skeletal integrity, aptamers have shown remarkable potential in influencingmolecular pathways crucial for bone regeneration, promoting osteogenic differentiation and supporting osteoblast survival. Byengineering aptamers to regulate inflammatory responses and facilitate the proliferation and differentiation of fibroblasts,these oligonucleotides can be integrated into advanced drug delivery systems, significantly improving bone repair efficacywhile minimizing adverse effects. Aptamer-mediated strategies, including the use of siRNA and miRNA mimics or inhibitors,have shown efficacy in enhancing bone mass and microstructure. These approaches hold transformative potential for treatinga range of orthopedic conditions like osteoporosis, osteosarcoma, and osteoarthritis. This review synthesizes the molecularmechanisms and biological roles of aptamers in orthopedic diseases, emphasizing their potential to drive innovative andeffective therapeutic interventions.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
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“Pioneer” and “Leading Goose” R&D Program of Zhejiang Province,Grant/Award Numbers:2021C01SA301612, 2023C01235Zhejiang Provincial Key Research and Development Program,Grant/Award Number:2020C01030
文摘The path to searching for sustainable energy has never stopped since thedepletion of fossil fuels can lead to serious environmental pollution andenergy shortages.Using water electrolysis to produce hydrogen has beenproven to be a prioritized approach for green resource production.It is highlycrucial to explore inexpensive and high-performance electrocatalysts foraccelerating hydrogen evolution reaction(HER)and apply them to industrialcases on a large scale.Here,we summarize the different mechanisms of HERin different pH settings and review recent advances in non-noble-metal-basedelectrocatalysts.Then,based on the previous efforts,we discuss severaluniversal strategies for designing pH-independent catalysts and showdirections for the future design of pH-universal 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.
基金Supported by the Fundamental Project of China National Petroleum Corporation(2021DJ0101)。
文摘Traditional petroleum system theories emphasize the restoration of the accumulation process from“source”to“trap”.The main oil and gas resources in the concept are conventional oil and gas,lacking the concept and research of unconventional oil and gas enrichment mechanism.The whole petroleum system is developed from the traditional petroleum system.Combined with unconventional oil and gas exploration practices and discoveries such as shale oil and gas,the whole petroleum system adds the research content of unconventional oil and gas.Although the study of the whole petroleum system is still in three aspects:geological elements,dynamic evolution and oil and gas distribution,its research ideas and research contents are very different,including the following three aspects.(1)In terms of geological elements,the traditional petroleum system studies the characteristics of source rocks and hydrocarbon generation evolution,and the reservoir properties,traps,migration and preservation conditions of conventional oil and gas.On the basis of the above research,the whole petroleum system has increased the quantitative evaluation of retained hydrocarbons,unconventional reservoir characterization,source reservoir configuration and other research contents.(2)In terms of dynamic evolution,the petroleum system studies the matching between the evolution of conventional oil and gas source rocks and the formation period of traps,while the whole petroleum system has increased the research content of the matching of unconventional reservoir densification and oil and gas charging,and the later transformation of unconventional oil and gas reservoirs.(3)In terms of oil and gas distribution,the petroleum system takes buoyancy-drived accumulation mechanism as the core to study the migration,accumulation and distribution of conventional oil and gas.The whole petroleum system adds unconventional oil and gas self-sealing accumulation mechanism and conventional-unconventional oil and gas distribution sequence,so as to determine the oil and gas distribution characteristics of the whole petroleum system.
基金financially supported by National Natural Science Foundation of China(Nos.22122202,22072051,21972051)。
文摘Water splitting with proton exchange membrane water electrolyzers(PEMWE)is regarded as a promising pathway for sustainable hydrogen conversion.Additionally,oxygen evolution reaction(OER)is considered as the dominant factor during the whole process due to the sluggish kinetics.Among the catalysts,Rubased catalysts draw special attention because of their excellent activity and relatively low price.However,the limited stability impedes their further commercialization and tremendous efforts have been devoted to overcome this challenge.This review firstly introduces the basic mechanisms of OER.Then the evaluation protocols and techniques to investigate the stability of Ru-based catalysts are summarized.A detailed elucidation of the possible degradation mechanisms is also critically analyzed.Furthermore,effective strategies to design durable Ru-based catalysts for acidic OER are discussed.Such as heteroatom doping,phase and facet engineering,heterostructure building and support optimization.Finally,promises,perspectives and challenges in developing highly durable Ru-based catalysts for acidic OER are outlined.
文摘Renewable energy conversion as well as water electrolysis technologies are constrained by the fact that kinetics are always slow in the electrocatalytic oxygen evolution reaction(OER).There are numerous means and strategies for the enhancement of OER activity.In this paper,we systematically review the important role of anionic vacancies in enhancing the OER activity of catalysts:increasing catalyst conductivity,improving electrical conductivity,and enhancing intermediate adsorption.In order to better detect the presence of vacancies in the samples,the principle of vacancy detection is reviewed in detail in terms of both spectroscopic and microscopic characterization,and the methods of vacancy formation as well as the factors influencing the concentration of vacancies are summarized in detail.In addition,the challenges and new directions for the study of anionic vacancies are provided.Lei Wang was awarded a Ph.D.in chemistry from Jilin University in 2006 under the supervision of Prof.Shouhua Feng.He worked as a Postdoctoral Scholar in Shandong University,the State Key Laboratory of Crystal Materials from 2008 to 2010.He is currently a professor at Qingdao University of Science and Technology.His research interests mainly focus on the design and synthesis of functional organic-inorganic hybrids and porous MOFs materials,as well as their applications in photocatalysis,electrocatalysis,lithium-ion battery,etc.Jingqi Chi received her B.S.degree and Ph.D.degree from the State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China).She is currently an associate professor at Qing dao University of Science and Technology.Her research interests focus on the design and synthesis of transition metal-based nanostructures and porous MOFs materials for electrochemical applications.
基金financial support by the National Natural Science Foundation of China(No.52102241)Doctor of Suzhou University Scientific Research Foundation(Nos.2022BSK019,2020BS015)+2 种基金the Primary Research and Development Program of Anhui Province(No.201904a05020087)the Natural Science Research Project in Universities of Anhui Province in China(Nos.2022AH051386,KJ2021A1114)the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking Qilu University of Technology。
文摘Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
基金financially supported by the National Natural Science Foundation of China(Nos.52306142,52272202 and W2421027)Yunnan Major Scientific and Technological Projects(No.202202AG050017-02)+2 种基金Yunnan Fundamental Research Projects(No.202101BE070001-017)the Science and Technology Innovation and Entrepreneurship Fund of China Coal Technology&Engineering Group Co.,Ltd.(Nos.2022-MS002 and 2023-TD-MS007)Bintuan Science and Technology Program(No.2022DB009)
文摘Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous interfacial catalyst,Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH,using a simple two-step method.In situ Raman and X-ray photoelectron spectroscopy(XPS)measurements revealed the dynamic phase change occurring during the OER process.The FeOOH layer on Ni(OH)_(2)/NiCo(OH)_(6)altered the electronic structure,facilitating the emergence of the active NiOOH phase and markedly improving OER kinetics.Significantly,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1 catalyst demonstrated a current density of 10 mA·cm^(-2)at an overpotential of merely 208 mV,accompanied by a Tafel slope of 37.72 mV·dec-1,exhibiting exceptional stability over a duration of 100 h at 10 mA·cm^(-2).Furthermore,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1(+)lIPt/C(-)electrolyzer cell showcased a remarkably low driving voltage of 1.52 V to achieve 10 mA·cm^(-2),while also displaying impressive durability under alkaline conditions for over100 h.This work enhances our understanding of the interfacial structure-activity relationship in composite catalysts,aiding the design of efficient catalysts with rapid kinetics.
基金supported by the National Key Projects for Fundamental Research and Development of China(2021YFA1500803)the National Natural Science Foundation of China(51825205,52120105002,22088102,22279150,22209186)+1 种基金the Beijing Natural Science Foundation(2222080)the Youth Innovation Promotion Association of the CAS(Y2021011)。
文摘Hydrogen evolution reaction(HER)plays a crucial role in developing clean and renewable hydrogen energy technologies.However,conventional HER catalysts rely on expensive and scarce noble metals,which is a significant challenge for practical application.Recently,twodimensional transition metal dichalcogenides(2D-TMDs)have emerged as attractive and cost-effective alternatives for efficient electrocatalysis in the HER.Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs.This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods.Subsequently,recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized.Finally,the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed.We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.
基金part of a research project, PIF 726175Alfaisal University and its Office of Research & Innovation for their continuous support throughout this study。
文摘Direct electrolysis of seawater to produce green hydrogen is a more environmentally friendly process than freshwater electrolysis.The renewable energy sector exhibits tremendous interest in practical seawater electrolysis techniques due to its substantial capacity to mitigate the need for freshwater consumption.With the low catalytic efficiency of the current seawater splitting process and the poor reliability of its operation,the process suffers from severe corrosion caused by chloride ions,as well as anodic competition between oxygen evolution and chlorine oxidation reactions.This review provides an overview of the latest electrocatalyst developments for promoting selectivity and stability in seawater electrolysis.Using the characterization and simulation results,as well as active machine learning,advanced electrocatalytic materials can be designed and developed,a research direction that will become increasingly important in the future.A variety of strategies are discussed in detail for designing advanced electrocatalysts in seawater electrolysis,including the surface protective layer,structural regulation by heteroatom doping and vacancies,porous structure,core-shell construction,and 3D hetero-structure construction to hinder chlorine evolution reactions.Finally,future perspectives and challenges for green hydrogen production from seawater electrolysis are also described.
文摘As low-altitude airspace becomes increasingly accessible and eVTOL(electric vertical take-off and landing)technologies advance,the low-altitude economy has emerged as a transformative frontier in urban mobility and industrial restructuring.Although countries face comparable technological opportunities,their development paths diverge significantly.This divergence is shaped not only by policy choices and innovation capacity but also by underlying differences in institutional architectures,resource configurations,and implementation mechanisms.This paper proposes a Development Path Evolution Model grounded in four structural elements:technological capability,institutional systems,infrastructure,and application scenarios.Based on this framework,the study identifies three archetypal path types(technology-led,institution-led,and scenario-driven)and empirically validates the model through comparative case studies of the United States,Europe,and Japan.Applying the model to China reveals a distinct"hybrid scenario-driven path",characterized by demand-responsive pilots,decentralized institutional flexibility,and strong engineering capacity.Using Shanghai as a representative case,the study outlines five strategic levers to guide its transition from a localized pilot zone to a platform-based governance hub with national and international relevance.The research contributes to theoretical understanding of path differentiation in emerging industries and provides actionable insights for developing economies with strong mobilization capacity and industrial ecosystems.
基金supported by the National Key Research and Development Program of China(No.2022YFB4004100)National Natural Science Foundation of China(Nos.U22A20396,22209168)+1 种基金Natural Science Foundation of Anhui Province(No.2208085UD04)Liaoning Binhai Laboratory(No.LBLF-2023-04),and Shandong Energy Institute(No.SEI U202307).
文摘Proton exchange membrane water electrolysis(PEMWE)is a favorable technology for producing highpurity hydrogen under high current density using intermittent renewable energy.The performance of PEMWE is largely determined by the oxygen evolution reaction(OER),a sluggish four-electron reaction with a high reaction barrier.Nowadays,iridium(Ir)-based catalysts are the catalysts of choice for OER due to their excellent activity and durability in acidic solution.However,its high price and unsatisfactory electrochemical performance severely restrict the PEMWE’s practical application.In this review,we initiate by introducing the current OER reaction mechanisms,namely adsorbate evolution mechanism and lattice oxygen mechanism,with degradation mechanisms discussed.Optimized strategies in the preparation of advanced Ir-based catalysts are further introduced,with merits and potential problems also discussed.The parameters that determine the performance of PEMWE are then introduced,with unsolved issues and related outlooks summarized in the end.
基金financial support of Shenzhen Science and Technology Program(No.KJZD20230923115005009)Xiangjiang Lab(22XJ01007)+3 种基金National Natural Science Foundation(NNSF)of China(No.52202269)Shenzhen Science and Technology program(No.20220810155330003)Shenzhen Science and Technology Program(NO.KJZD20230923115005009)Project of Department of Education of Guangdong Province(No.2022ZDZX3018).
文摘The transition to renewable energy sources has elevated the importance of SIBs(SIBs)as cost-effective alternatives to lithium-ion batteries(LIBs)for large-scale energy storage.This review examines the mechanisms of gas generation in SIBs,identifying sources from cathode materials,anode materials,and electrolytes,which pose safety risks like swelling,leakage,and explosions.Gases such as CO_(2),H_(2),and O_(2) primarily arise from the instability of cathode materials,side reactions between electrode and electrolyte,and electrolyte decomposition under high temperatures or voltages.Enhanced mitigation strategies,encompassing electrolyte design,buffer layer construction,and electrode material optimization,are deliberated upon.Accordingly,subsequent research endeavors should prioritize long-term high-precision gas detection to bolster the safety and performance of SIBs,thereby fortifying their commercial viability and furnishing dependable solutions for large-scale energy storage and electric vehicles.
基金Key research and development projects of Sichuan Science and Technology Plan Project(2024YFFK0135)Fujian Provincial Natural Science Foundation of China(2024J011450).
文摘Precision medicine has become a cornerstone in modern therapeutic strategies, with nucleic acid aptamers emerging aspivotal tools due to their unique properties. These oligonucleotide fragments, selected through the Systematic Evolution ofLigands by Exponential Enrichment process, exhibit high affinity and specificity toward their targets, such as DNA, RNA,proteins, and other biomolecules. Nucleic acid aptamers offer significant advantages over traditional therapeutic agents,including superior biological stability, minimal immunogenicity, and the capacity for universal chemical modifications thatenhance their in vivo performance and targeting precision. In the realm of osseous tissue repair and regeneration, a complexphysiological process essential for maintaining skeletal integrity, aptamers have shown remarkable potential in influencingmolecular pathways crucial for bone regeneration, promoting osteogenic differentiation and supporting osteoblast survival. Byengineering aptamers to regulate inflammatory responses and facilitate the proliferation and differentiation of fibroblasts,these oligonucleotides can be integrated into advanced drug delivery systems, significantly improving bone repair efficacywhile minimizing adverse effects. Aptamer-mediated strategies, including the use of siRNA and miRNA mimics or inhibitors,have shown efficacy in enhancing bone mass and microstructure. These approaches hold transformative potential for treatinga range of orthopedic conditions like osteoporosis, osteosarcoma, and osteoarthritis. This review synthesizes the molecularmechanisms and biological roles of aptamers in orthopedic diseases, emphasizing their potential to drive innovative andeffective therapeutic interventions.
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.
