High-entropy materials(HEMs)have attracted considerable research attention in battery applications due to exceptional properties such as remarkable structural stability,enhanced ionic conductivity,superior mechanical ...High-entropy materials(HEMs)have attracted considerable research attention in battery applications due to exceptional properties such as remarkable structural stability,enhanced ionic conductivity,superior mechanical strength,and outstanding catalytic activity.These distinctive characteristics render HEMs highly suitable for various battery components,such as electrodes,electrolytes,and catalysts.This review systematically examines recent advances in the application of HEMs for energy storage,beginning with fundamental concepts,historical development,and key definitions.Three principal categories of HEMs,namely high-entropy alloys,high-entropy oxides,and highentropy MXenes,are analyzed with a focus on electrochemical performance metrics such as specific capacity,energy density,cycling stability,and rate capability.The underlying mechanisms by which these materials enhance battery performance are elucidated in the discussion.Furthermore,the pivotal role of machine learning in accelerating the discovery and optimization of novel high-entropy battery materials is highlighted.The review concludes by outlining future research directions and potential breakthroughs in HEM-based battery technologies.展开更多
High-entropy materials(HEMs)show exceptional mechanical properties,highly adjustable chemical characteristics,and outstanding stability,making them suitable for energy storage.However,the broad compositional space and...High-entropy materials(HEMs)show exceptional mechanical properties,highly adjustable chemical characteristics,and outstanding stability,making them suitable for energy storage.However,the broad compositional space and intricate chemical interactions in HEMs present challenges to traditional trial-and-error research methods,restricting their efficacy in swift screening and synthesis.Hence,the application of machine learning(ML)to the realm of high-entropy materials and energy storage becomes imperative.ML demonstrates its formidable capabilities for navigating the complexity of HEMs,with their diverse metal components,structures and property combinations,to advance energy storage applications.This review comprises the following sections:a concise introduction to the general process of ML in the energy materials field,a summary of HEMs in the energy storage field,a review of the latest achievements of ML in the HEMs and energy storage field,and finally,an exploration of current challenges and prospects in this interdisciplinary arena.With the advent of ML,the precision of its predictions and the efficiency of its screening methods have offered novel perspectives for material research,expediting the discovery and application of new materials.This article contributes to the advancement of research in related fields,hastening the development of novel materials to meet the escalating energy demands and promote sustainable development goals.展开更多
High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailo...High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.展开更多
Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy...Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy Applications:Innovations in Energy Conversion and Storage.”This collection highlights the latest research developments in the preparation,optimizing properties,and exploring potential applications of high-entropy materials(HEMs)and other com-pounds with increased configurational entropy.展开更多
The pursuit of highly efficient electrocatalysts is of utmost significance in the relentless drive to enhance the electrochemical performance of lithium-sulfur batteries.These electrocatalysts enable a predominant con...The pursuit of highly efficient electrocatalysts is of utmost significance in the relentless drive to enhance the electrochemical performance of lithium-sulfur batteries.These electrocatalysts enable a predominant contribution(~75%)to the overall discharge capacity during cycling by facilitating the rapid conversion of long-chain lithium polysulfides into insoluble short-chain products(Li_(2)S_(2)and Li_(2)S).Herein,high entropy sulfides derived from high entropy metal glycerate templates are synthesized and utilized as electrocatalysts.Among the evaluated materials,high entropy sulfides containing Ni,Co,Fe,Mg,and Ti(GS-3)showcases modulated spherical morphology,uniform elemental distribution,and efficient catalytic properties,outperforming high entropy sulfides containing Ni,Co,Fe,Mg,and Zn(GS-1)and high entropy sulfides containing Ni,Co,Cu,Mg,and Zn(GS-2).Consequently,a typical lithium-sulfur battery incorporating the GS-3/S/KB cathode(S loading~2.3 mg cm^(-2))demonstrates a high initial discharge capacity of~1061 mAh g^(-1)at 0.5 C and stable cycling(1500 cycles)at the lowest capacity decay rate of 0.032%per cycle.The results are superior to the electrochemical performance of GS-1/S/KB(~945 mAh g^(-1),0.034%),GS-2/S/KB(~909 mAh g^(-1),0.086%),and S/KB(~748 mAh g^(-1),0.19%)cells.This work highlights the incorporation of titanium and other metal elements into the sulfide structure,forming high entropy sulfides(i.e.,GS-3)that facilitates efficient catalytic conversion and enhances the cycling performance of lithium-sulfur batteries.展开更多
With the recent development of high entropy materials, an alternative approach to develop advanced functional materials with distinctive properties that show improved values compared to conventional materials has been...With the recent development of high entropy materials, an alternative approach to develop advanced functional materials with distinctive properties that show improved values compared to conventional materials has been provided. The high entropy concept was later successfully transferred to metal fluorides and high entropy fluorides(HEFs) were successfully synthesized. Owing to their high theoretical specific capacities in energy storage applications, HEFs were utilized as cathode materials for lithiumion batteries(LIBs) and their underlying storage mechanisms were investigated. Instead of a step-bystep reduction of each individual metal cation, the HEFs seem to exhibit a single-step reduction process,indicating a solid solution compound instead of merely a mixture of different metal fluorides. It was also observed that the electrochemical behavior of the HEFs depends on each individual incorporated element. Therefore, by altering the elemental composition, new materials that exhibit improved electrochemical properties can be designed. Remarkably, HEFs with seven incorporated metal elements exhibited a better cycling stability as well as a lower hysteresis compared to binary metal fluorides.These findings offer new guidelines for material design and tailoring towards high performance LIBs.展开更多
Recently, high-entropy materials(HEMs) have gained increasing interest in the field of energy storage technology on account of their unique structural characteristics and possibilities for tailoring functional propert...Recently, high-entropy materials(HEMs) have gained increasing interest in the field of energy storage technology on account of their unique structural characteristics and possibilities for tailoring functional properties. Herein, the development of this class of materials for electrochemical energy storage have been reviewed, especially the fundamental understanding of entropy-dominated phase-stabilization effects and prospective applications are presented. Subsequently, critical comments of HEMs on the different aspects of battery and supercapacitor are summarized with the underlying principles for the observed properties. In addition, we also summarize their potential advantages and remaining challenges, which will ideally provide some general guidelines and principles for researchers to study and develop advanced HEMs. The diversity of material design contributed by the entropy-mediated concept provides the researchers numerous ideas of new candidates for practical applications and ensures further research in the emerging field of energy storage.展开更多
High-entropy materials are composed of five or more metal elements with equimolar or near-equimolar concentrations within one crystal structure,which offer remarkable structural properties for many applications.Despit...High-entropy materials are composed of five or more metal elements with equimolar or near-equimolar concentrations within one crystal structure,which offer remarkable structural properties for many applications.Despite previously reported entropy-driven stabilization mechanisms,many high-entropy materials still tend to decompose to produce a variety of derivatives under operating conditions.In this study,we use transition-metal(Ni,Co,Ni,Zn,V)-based high-entropy metal-organic frameworks(HE-MOFs)as the precursors to produce different derivatives under acidic/alkaline treatment.We have shown that HE-MOFs and derivatives have shown favorable kinetics for N_(2)electrofixation in different pH electrolytes,specifically cathodic nitrogen reduction reaction in acidic media and anodic oxygen evolution reaction in alkaline media.To buffer the pH mismatch,we have further constructed an asymmetric acidic/alkaline device prototype by using bipolar membranes.As expected,the prototype showed remarkable activities,with an NH_(3)yield rate of 42.76μg h^(−1)mg^(−1),and Faradaic efficiency of 14.75%and energy efficiency of 2.59%,which are 14.4 and 4.4 times larger than those of its symmetric acidic and alkaline counterparts,respectively.展开更多
The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need...The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need to develop advanced electrocatalysts able to show high activity and withstand industrially-relevant operating conditions for a prolonged period of time.In this regard,high entropy materials(HEMs),including high entropy alloys and high entropy oxides,comprising five or more homogeneously distributed metal components,have emerged as a new class of electrocatalysts owing to their unique properties such as low atomic diffusion,structural stability,a wide variety of adsorption energies and multi-component synergy,making them promising catalysts for challenging electrochemical reactions,including those involved in WE.This review begins with a brief overview about WE technologies and a short introduction to HEMs including their synthesis and general physicochemical properties,followed by a nearly exhaustive summary of HEMs catalysts reported so far for the hydrogen evolution reaction,the oxygen evolution reaction and the overall water splitting in both alkaline and acidic conditions.The review concludes with a brief summary and an outlook about the future development of HEM-based catalysts and further research to be done to understand the catalytic mechanism and eventually deploy HEMs in practical water electrolysers.展开更多
The structure, magnetic and magnetocaloric properties of the Ge-rich Gd5Ge2.05-xSi1.95-xMn2x （x=0.01 and 0.03） alloys were investigated by scanning electron microscopy, X-ray powder diffraction, differential scannin...The structure, magnetic and magnetocaloric properties of the Ge-rich Gd5Ge2.05-xSi1.95-xMn2x （x=0.01 and 0.03） alloys were investigated by scanning electron microscopy, X-ray powder diffraction, differential scanning calorimeter （DSC） and magnetization measurements. The results of energy dispersive X-ray analysis （EDX） and X-ray diffraction analyses showed that the composition and crystal structure of the alloys were desired. DSC measurements were performed to determine the transformation temperatures for each alloy. Both alloys exhibited the first order phase transition around room temperature. The alloys showed an anti-ferromagnetic transition around 60 K. The isothermal magnetic entropy changes of the alloys were determined from the isothermal magnetization measurements by using the Maxwell relation. The maximum values of isothermal magnetic entropy change of the Gd5Ge2.05-xSi1.95-xMn2x alloy with x=0.01 was found to be -12.1 and -19.8 J/（kg·K） using Maxwell equation around 268 K in applied fields of 2 and 5 T, respectively.展开更多
Developing noble-metal-free oxygen evolution reaction(OER)electrocatalysts with stable performance at large working current is an imperative and yet formidable challenge for practical large scale water splitting.In th...Developing noble-metal-free oxygen evolution reaction(OER)electrocatalysts with stable performance at large working current is an imperative and yet formidable challenge for practical large scale water splitting.In this study,by inheriting hierarchical nanostructure and elemental homogeneity of Prussian blue analogues,a series of medium entropy transition metal phosphides(METMP)OER catalysts with high cost-effectivity,efficiency and stability were precisely prepared.Specifically,the METMP-based((FeCoNi)P/Ni_(2)P-NF)catalyst demonstrates exceptional performance with an overpotential of only 232 mV at 50 mA·cm^(-2)and a Tafel slope of 52.7 mV·dec^(-1),significantly superior to its less entropy counterparts and commercial RuO_(2-).Moreover,it even maintains stability at the industrial standard current density of 500 mA·cm^(-2)for over 200 h.Density functional theory(DFT)calculations indicates that the synergistic effect of Fe,Co,Ni modulates electronic structure of METMPs,which effectively reduces the energy barrier for the rate-determining HOO*formation step,thereby considerably enhancing catalytic activity.This work not only contributes to the fundamental understanding of the role of medium/high entropy in catalysis but also paves the way for the development of next-generation electrocatalysts for energy-related applications.展开更多
Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is...Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is therefore in urgent demand.Electrochemical oxidation provides a convenient and reliable route to attain efficient utilization of ammonia.Here,we report that the high entropy(Mn,Fe,Co,Ni,Cu)_(3)O_(4)oxides can achieve high electrocatalytic activity for ammonia oxidation reaction(AOR)in non-aqueous solutions.The AOR onset overpotential of(Mn,Fe,Co,Ni,Cu)_(3)O_(4)is 0.70 V,which is nearly 0.2 V lower than that of their most active single metal cation counterpart.The mass spectroscopy study reveals that(Mn,Fe,Co,Ni,Cu)_(3)O_(4)preferentially oxidizes ammonia to environmentally friendly diatomic nitrogen with a Faradic efficiency of over 85%.The Xray photoelectron spectroscopy(XPS)result indicates that the balancing metal d-band of Mn and Cu cations helps retain a longlasting electrocatalytic activity.Overall,this work introduces a new family of earth-abundant transition metal high entropy oxide electrocatalysts for AOR,thus heralding a new paradigm of catalyst design for enabling ammonia as an energy carrier.展开更多
Machine learning and computational methods can accelerate materials discovery by accurately predicting material properties at low cost.Nevertheless,input data to algorithms and structure model parameters remains a key...Machine learning and computational methods can accelerate materials discovery by accurately predicting material properties at low cost.Nevertheless,input data to algorithms and structure model parameters remains a key obstacle.The limitations of conventional battery materials could be overcome by high-entropy materials,a unique class of special valuable materials.The knowledge of designing the crystal structure of high-entropy materials is advancing the design and fabrication of new materials for batteries and supercapacitors,even before chemical synthesis,through the use of learning algorithms and quantum computing.In this review,we first focus on quantum computing and the structure of high-entropy materials,especially high-entropy MXenes.We then discuss how to encode and decode the crystal structure of materials,which is a key factor in creating a database for high-entropy materials.We also discuss how to utilize deep learning algorithms for material discovery prior to synthesis,as well as how to employ these algorithms to identify high-entropy materials suitable for batteries and supercapacitors.Finally,we discuss the potential of new quantum computing and artificial intelligence approaches for determining the structure of high-entropy materials in the energy fields.展开更多
A reformation in energy is underway to replace fossil fuels with renewable sources,driven by the development of new,robust,and multi-functional materials.High-entropy materials(HEMs)have emerged as promising candidate...A reformation in energy is underway to replace fossil fuels with renewable sources,driven by the development of new,robust,and multi-functional materials.High-entropy materials(HEMs)have emerged as promising candidates for various green energy applications,having unusual chemistries that give rise to remarkable functionalities.This review examines recent innovations in HEMs,focusing on hydrogen generation/storage,fuel cells,batteries,semiconductors/electronics,and catalysis—where HEMs have demonstrated the ability to outperform state-of-the-art materials.We present new master plots that illustrate the superior performance of HEMs compared to conventional systems for hydrogen generation/storage and heat-to-electricity conversion.We highlight the role of computational methods,such as density functional theory and machine learning,in accelerating the discovery and optimization of HEMs.The review also presents current challenges and proposes future directions for the field.We emphasize the need for continued integration of modeling,data,and experiments to investigate and leverage the underlying mechanisms of the HEMs that are powering progress in sustainable energy.展开更多
基金supported by the Fujian Provincial Science and Technology Planning Project(No.2022HZ027006,No.2024HZ021023)National Natural Science Foundation of China(No.U22A20118).
文摘High-entropy materials(HEMs)have attracted considerable research attention in battery applications due to exceptional properties such as remarkable structural stability,enhanced ionic conductivity,superior mechanical strength,and outstanding catalytic activity.These distinctive characteristics render HEMs highly suitable for various battery components,such as electrodes,electrolytes,and catalysts.This review systematically examines recent advances in the application of HEMs for energy storage,beginning with fundamental concepts,historical development,and key definitions.Three principal categories of HEMs,namely high-entropy alloys,high-entropy oxides,and highentropy MXenes,are analyzed with a focus on electrochemical performance metrics such as specific capacity,energy density,cycling stability,and rate capability.The underlying mechanisms by which these materials enhance battery performance are elucidated in the discussion.Furthermore,the pivotal role of machine learning in accelerating the discovery and optimization of novel high-entropy battery materials is highlighted.The review concludes by outlining future research directions and potential breakthroughs in HEM-based battery technologies.
基金supported by the National Natural Science Foundation of China(22005072,21965006)Guiyang Guian science and Technology Personnel Training Project(2024-2-13)+1 种基金Guizhou Provincial Key Technology R&D Program(Qian Ke He support(2023)General 122)Guizhou Provincial Science and Technology Foundation(ZD2025049,KXJZ2024029).
文摘High-entropy materials(HEMs)show exceptional mechanical properties,highly adjustable chemical characteristics,and outstanding stability,making them suitable for energy storage.However,the broad compositional space and intricate chemical interactions in HEMs present challenges to traditional trial-and-error research methods,restricting their efficacy in swift screening and synthesis.Hence,the application of machine learning(ML)to the realm of high-entropy materials and energy storage becomes imperative.ML demonstrates its formidable capabilities for navigating the complexity of HEMs,with their diverse metal components,structures and property combinations,to advance energy storage applications.This review comprises the following sections:a concise introduction to the general process of ML in the energy materials field,a summary of HEMs in the energy storage field,a review of the latest achievements of ML in the HEMs and energy storage field,and finally,an exploration of current challenges and prospects in this interdisciplinary arena.With the advent of ML,the precision of its predictions and the efficiency of its screening methods have offered novel perspectives for material research,expediting the discovery and application of new materials.This article contributes to the advancement of research in related fields,hastening the development of novel materials to meet the escalating energy demands and promote sustainable development goals.
基金supported by the Guangdong Basic and Applied Basic Research Fund Project(2022A1515140061,No.11000-2344014)Startup Foundation for Postdoctor by Dongguan University of Technology(No.11000-221110149)the High-level Talents Program(contract number 2023JC10L014)of the Department of Science and Technology of Guangdong Province。
文摘High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.
文摘Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy Applications:Innovations in Energy Conversion and Storage.”This collection highlights the latest research developments in the preparation,optimizing properties,and exploring potential applications of high-entropy materials(HEMs)and other com-pounds with increased configurational entropy.
基金supported by the National Natural Science Foundation of China(52372289,52102368)the Guangdong Special Fund for key Areas(20237DZX3042)the Shenzhen Stable Support Project.
文摘The pursuit of highly efficient electrocatalysts is of utmost significance in the relentless drive to enhance the electrochemical performance of lithium-sulfur batteries.These electrocatalysts enable a predominant contribution(~75%)to the overall discharge capacity during cycling by facilitating the rapid conversion of long-chain lithium polysulfides into insoluble short-chain products(Li_(2)S_(2)and Li_(2)S).Herein,high entropy sulfides derived from high entropy metal glycerate templates are synthesized and utilized as electrocatalysts.Among the evaluated materials,high entropy sulfides containing Ni,Co,Fe,Mg,and Ti(GS-3)showcases modulated spherical morphology,uniform elemental distribution,and efficient catalytic properties,outperforming high entropy sulfides containing Ni,Co,Fe,Mg,and Zn(GS-1)and high entropy sulfides containing Ni,Co,Cu,Mg,and Zn(GS-2).Consequently,a typical lithium-sulfur battery incorporating the GS-3/S/KB cathode(S loading~2.3 mg cm^(-2))demonstrates a high initial discharge capacity of~1061 mAh g^(-1)at 0.5 C and stable cycling(1500 cycles)at the lowest capacity decay rate of 0.032%per cycle.The results are superior to the electrochemical performance of GS-1/S/KB(~945 mAh g^(-1),0.034%),GS-2/S/KB(~909 mAh g^(-1),0.086%),and S/KB(~748 mAh g^(-1),0.19%)cells.This work highlights the incorporation of titanium and other metal elements into the sulfide structure,forming high entropy sulfides(i.e.,GS-3)that facilitates efficient catalytic conversion and enhances the cycling performance of lithium-sulfur batteries.
基金the financial support received from the China Scholarship Council(CSC)MERAGEM graduate school and the Ministry of Science,Research and Arts of the State of Baden-Wu rttemberg for funding research+4 种基金the support of the German Research Foundation(DFG)project(SE 1407/4-2)the support of the En ABLES,a project funded by the European Union’s Horizon 2020 research and innovation program under grant agreement(730957)the support of Epi Store project under grant agreement(101017709)the Centre for Electrochemical Energy Storage Ulm-Karlsruhe(CELEST)the support from the Karlsruhe Nano Micro Facility(KNMF)。
文摘With the recent development of high entropy materials, an alternative approach to develop advanced functional materials with distinctive properties that show improved values compared to conventional materials has been provided. The high entropy concept was later successfully transferred to metal fluorides and high entropy fluorides(HEFs) were successfully synthesized. Owing to their high theoretical specific capacities in energy storage applications, HEFs were utilized as cathode materials for lithiumion batteries(LIBs) and their underlying storage mechanisms were investigated. Instead of a step-bystep reduction of each individual metal cation, the HEFs seem to exhibit a single-step reduction process,indicating a solid solution compound instead of merely a mixture of different metal fluorides. It was also observed that the electrochemical behavior of the HEFs depends on each individual incorporated element. Therefore, by altering the elemental composition, new materials that exhibit improved electrochemical properties can be designed. Remarkably, HEFs with seven incorporated metal elements exhibited a better cycling stability as well as a lower hysteresis compared to binary metal fluorides.These findings offer new guidelines for material design and tailoring towards high performance LIBs.
基金financially supported by the China Postdoctoral Science Foundation(2019M650173,2020M672261)the National Natural Science Foundation of China(21975225,22005274,51902293)。
文摘Recently, high-entropy materials(HEMs) have gained increasing interest in the field of energy storage technology on account of their unique structural characteristics and possibilities for tailoring functional properties. Herein, the development of this class of materials for electrochemical energy storage have been reviewed, especially the fundamental understanding of entropy-dominated phase-stabilization effects and prospective applications are presented. Subsequently, critical comments of HEMs on the different aspects of battery and supercapacitor are summarized with the underlying principles for the observed properties. In addition, we also summarize their potential advantages and remaining challenges, which will ideally provide some general guidelines and principles for researchers to study and develop advanced HEMs. The diversity of material design contributed by the entropy-mediated concept provides the researchers numerous ideas of new candidates for practical applications and ensures further research in the emerging field of energy storage.
基金Fundamental Research Funds for the Central Universities,Grant/Award Numbers:30920041113,30921013103Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20190460+2 种基金Jiangsu innovative/entre‐preneurial talent program,Grant/Award Number:2019Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China,Grant/Award Number:51888103National Natural Science Foundation of China,Grant/Award Numbers:52006105,92163124。
文摘High-entropy materials are composed of five or more metal elements with equimolar or near-equimolar concentrations within one crystal structure,which offer remarkable structural properties for many applications.Despite previously reported entropy-driven stabilization mechanisms,many high-entropy materials still tend to decompose to produce a variety of derivatives under operating conditions.In this study,we use transition-metal(Ni,Co,Ni,Zn,V)-based high-entropy metal-organic frameworks(HE-MOFs)as the precursors to produce different derivatives under acidic/alkaline treatment.We have shown that HE-MOFs and derivatives have shown favorable kinetics for N_(2)electrofixation in different pH electrolytes,specifically cathodic nitrogen reduction reaction in acidic media and anodic oxygen evolution reaction in alkaline media.To buffer the pH mismatch,we have further constructed an asymmetric acidic/alkaline device prototype by using bipolar membranes.As expected,the prototype showed remarkable activities,with an NH_(3)yield rate of 42.76μg h^(−1)mg^(−1),and Faradaic efficiency of 14.75%and energy efficiency of 2.59%,which are 14.4 and 4.4 times larger than those of its symmetric acidic and alkaline counterparts,respectively.
基金the financial support of the Mobilizador Programme(via Baterias 2030 project,Grant No.POCI-010247-FEDER-046109)from the National Innovation Agency of Portugalpartially supported by the start-up project of the Songshan lake Materials Laboratory(Grant No.Y2D1051Z311).
文摘The production of hydrogen through water electrolysis(WE)from renewable electricity is set to revolutionise the energy sector that is at present heavily dependent on fossil fuels.However,there is still a pressing need to develop advanced electrocatalysts able to show high activity and withstand industrially-relevant operating conditions for a prolonged period of time.In this regard,high entropy materials(HEMs),including high entropy alloys and high entropy oxides,comprising five or more homogeneously distributed metal components,have emerged as a new class of electrocatalysts owing to their unique properties such as low atomic diffusion,structural stability,a wide variety of adsorption energies and multi-component synergy,making them promising catalysts for challenging electrochemical reactions,including those involved in WE.This review begins with a brief overview about WE technologies and a short introduction to HEMs including their synthesis and general physicochemical properties,followed by a nearly exhaustive summary of HEMs catalysts reported so far for the hydrogen evolution reaction,the oxygen evolution reaction and the overall water splitting in both alkaline and acidic conditions.The review concludes with a brief summary and an outlook about the future development of HEM-based catalysts and further research to be done to understand the catalytic mechanism and eventually deploy HEMs in practical water electrolysers.
文摘The structure, magnetic and magnetocaloric properties of the Ge-rich Gd5Ge2.05-xSi1.95-xMn2x （x=0.01 and 0.03） alloys were investigated by scanning electron microscopy, X-ray powder diffraction, differential scanning calorimeter （DSC） and magnetization measurements. The results of energy dispersive X-ray analysis （EDX） and X-ray diffraction analyses showed that the composition and crystal structure of the alloys were desired. DSC measurements were performed to determine the transformation temperatures for each alloy. Both alloys exhibited the first order phase transition around room temperature. The alloys showed an anti-ferromagnetic transition around 60 K. The isothermal magnetic entropy changes of the alloys were determined from the isothermal magnetization measurements by using the Maxwell relation. The maximum values of isothermal magnetic entropy change of the Gd5Ge2.05-xSi1.95-xMn2x alloy with x=0.01 was found to be -12.1 and -19.8 J/（kg·K） using Maxwell equation around 268 K in applied fields of 2 and 5 T, respectively.
基金the National Natural Science Foundation of China(Nos.52372170 , 92163209)the Beijing Natural Science Foundation(No.2232068)the Beijing-Tianjin-Hebei Basic Research Cooperation Special Project(No.B2024204027).
文摘Developing noble-metal-free oxygen evolution reaction(OER)electrocatalysts with stable performance at large working current is an imperative and yet formidable challenge for practical large scale water splitting.In this study,by inheriting hierarchical nanostructure and elemental homogeneity of Prussian blue analogues,a series of medium entropy transition metal phosphides(METMP)OER catalysts with high cost-effectivity,efficiency and stability were precisely prepared.Specifically,the METMP-based((FeCoNi)P/Ni_(2)P-NF)catalyst demonstrates exceptional performance with an overpotential of only 232 mV at 50 mA·cm^(-2)and a Tafel slope of 52.7 mV·dec^(-1),significantly superior to its less entropy counterparts and commercial RuO_(2-).Moreover,it even maintains stability at the industrial standard current density of 500 mA·cm^(-2)for over 200 h.Density functional theory(DFT)calculations indicates that the synergistic effect of Fe,Co,Ni modulates electronic structure of METMPs,which effectively reduces the energy barrier for the rate-determining HOO*formation step,thereby considerably enhancing catalytic activity.This work not only contributes to the fundamental understanding of the role of medium/high entropy in catalysis but also paves the way for the development of next-generation electrocatalysts for energy-related applications.
基金supported by the Energy Research Seed Grant from Duke Energy Initiative,the National Science Foundation(Nos.CHE-1565657 and CHE-1954838)the Army Research Office(W911NFN-18-2-004)+2 种基金S.H.and P.N.are both supported by fellowships from Department of Chemistry at Duke UniversityThis work was performed in part at the Duke University Shared Materials Instrumentation Facility(SMIF),a member of the North Carolina Research Triangle Nanotechnology Network(RTNN)which is supported by the National Science Foundation(award number ECCS-2025064)as part of the National Nanotechnology Coordinated Infrastructure(NNCI).
文摘Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is therefore in urgent demand.Electrochemical oxidation provides a convenient and reliable route to attain efficient utilization of ammonia.Here,we report that the high entropy(Mn,Fe,Co,Ni,Cu)_(3)O_(4)oxides can achieve high electrocatalytic activity for ammonia oxidation reaction(AOR)in non-aqueous solutions.The AOR onset overpotential of(Mn,Fe,Co,Ni,Cu)_(3)O_(4)is 0.70 V,which is nearly 0.2 V lower than that of their most active single metal cation counterpart.The mass spectroscopy study reveals that(Mn,Fe,Co,Ni,Cu)_(3)O_(4)preferentially oxidizes ammonia to environmentally friendly diatomic nitrogen with a Faradic efficiency of over 85%.The Xray photoelectron spectroscopy(XPS)result indicates that the balancing metal d-band of Mn and Cu cations helps retain a longlasting electrocatalytic activity.Overall,this work introduces a new family of earth-abundant transition metal high entropy oxide electrocatalysts for AOR,thus heralding a new paradigm of catalyst design for enabling ammonia as an energy carrier.
基金supported by Khalifa University and a Natural Sciences and Engineering Research Council of Canada(NSERC)Discovery grant.This work is supported by NSERC Discovery grant.
文摘Machine learning and computational methods can accelerate materials discovery by accurately predicting material properties at low cost.Nevertheless,input data to algorithms and structure model parameters remains a key obstacle.The limitations of conventional battery materials could be overcome by high-entropy materials,a unique class of special valuable materials.The knowledge of designing the crystal structure of high-entropy materials is advancing the design and fabrication of new materials for batteries and supercapacitors,even before chemical synthesis,through the use of learning algorithms and quantum computing.In this review,we first focus on quantum computing and the structure of high-entropy materials,especially high-entropy MXenes.We then discuss how to encode and decode the crystal structure of materials,which is a key factor in creating a database for high-entropy materials.We also discuss how to utilize deep learning algorithms for material discovery prior to synthesis,as well as how to employ these algorithms to identify high-entropy materials suitable for batteries and supercapacitors.Finally,we discuss the potential of new quantum computing and artificial intelligence approaches for determining the structure of high-entropy materials in the energy fields.
基金sponsored by the Advanced Research Projects Agency-Energy(ARPA-E)(DE-AR0001787)G.Q.acknowledges support from the Ralph O'Connor Sustainable Energy Institute(ROSEI)at JHU+3 种基金X.X.acknowledges support from the Institute for Data-Intensive Engineering and Science(IDIES)at JHUK.C.acknowledges support from the Maryland Space Grant Consortium(MDSGC)the Space@Hopkins seed grant fundC.O.acknowledges support from Advanced Research Computing at Hopkins(ARCH).
文摘A reformation in energy is underway to replace fossil fuels with renewable sources,driven by the development of new,robust,and multi-functional materials.High-entropy materials(HEMs)have emerged as promising candidates for various green energy applications,having unusual chemistries that give rise to remarkable functionalities.This review examines recent innovations in HEMs,focusing on hydrogen generation/storage,fuel cells,batteries,semiconductors/electronics,and catalysis—where HEMs have demonstrated the ability to outperform state-of-the-art materials.We present new master plots that illustrate the superior performance of HEMs compared to conventional systems for hydrogen generation/storage and heat-to-electricity conversion.We highlight the role of computational methods,such as density functional theory and machine learning,in accelerating the discovery and optimization of HEMs.The review also presents current challenges and proposes future directions for the field.We emphasize the need for continued integration of modeling,data,and experiments to investigate and leverage the underlying mechanisms of the HEMs that are powering progress in sustainable energy.
