Water electrolysis has been considered as a sustainable way for producing renewable energy of hydrogen.However,this process requires a low-cost and high-efficient hydrogen evolution reaction(HER)catalyst to improve th...Water electrolysis has been considered as a sustainable way for producing renewable energy of hydrogen.However,this process requires a low-cost and high-efficient hydrogen evolution reaction(HER)catalyst to improve the overall reaction efficiency.Molybdenum(Mo)-based electrocatalysts are regarded as the promising candidates to replace the benchmark but expensive Ptbased HER catalysts,due to their high activity and stability in a wide pH range.In this review,we present a comprehensive and critical summary on the recent progress in the Mo-based electrodes for HER,including molybdenum alloys,molybdenum sulfides,molybdenum selenides,molybdenum carbides,molybdenum phosphides,molybdenum borides,molybdenum nitrides,and molybdenum oxides.Particular attention is mainly focused on the synthetic methods of Mo-based materials,the strategies for increasing the catalytic activity,and the relationship between structure/composition and electrocatalytic performance.Finally,the future development and perspectives of Mo-based electrocatalysts toward high HER performance are proposed.展开更多
Rechargeable aqueous zinc-ion batteries(ZIBs) featuring the merits of low cost,eco-friendliness,and enhanced safety have attracted extensive interests and considered as the most promising energy storage system.However...Rechargeable aqueous zinc-ion batteries(ZIBs) featuring the merits of low cost,eco-friendliness,and enhanced safety have attracted extensive interests and considered as the most promising energy storage system.However,much efforts are devoted to the exploration of cathode materials and their storage mechanisms in this system,and inadequate attentions are received in regard to anode side especially in neutral or mild acidic electrolyte.Therefore,in this review,the fundamental understanding of existing issues including dendrite formation,corrosion,and hydrogen evolution are mainly revealed,as well as their interaction in neutral or mild acidic medium.In addition,the currently existing solution strategies on the anode are summarized and the mechanisms that contained are simultaneously investigated.Finally,perspectives on future anode modification and innovation direction are provided for the further development and research of Zn-based ZIBs.展开更多
Hydrogen production from water splitting using renewable electric energy is an interesting topic towards the carbon neutral future.Single atom catalysts(SACs)have emerged as a new frontier in the field of catalysis su...Hydrogen production from water splitting using renewable electric energy is an interesting topic towards the carbon neutral future.Single atom catalysts(SACs)have emerged as a new frontier in the field of catalysis such as hydrogen evolution reaction(HER),owing to their intriguing properties like high activity and excellent chemical selectivity.The catalytic active moiety is often comprised of a single metal atom and its neighboring environment from the supports.Recent published reviews about electricdriven HER tend to classify these SACs by the species of active center atom,nevertheless the influence of their neighboring coordinated atoms from the supports is somehow neglected.Thus we classify the SACs for HER through the type of supports,highlighting the electronic metal–support interaction and their coordination environment from support.Then,we put forward some structural designing strategies including regulating of the central atoms,coordination environments,and metal-support interactions.Finally,the current challenges and future research perspectives of SACs for HER are briefly proposed.展开更多
Aqueous zinc-ion batteries(ZIBs)have been intensively investigated as potential energy storage devices on account of their low cost,environmental benignity,and intrinsically safe merits.With the exploitation of highpe...Aqueous zinc-ion batteries(ZIBs)have been intensively investigated as potential energy storage devices on account of their low cost,environmental benignity,and intrinsically safe merits.With the exploitation of highperformance cathode materials,electrolyte systems,and in-depth mechanism investigation,the electrochemical performances of ZIBs have been greatly enhanced.However,there are still some challenges that need to be overcome before its commercialization.Among them,the obstinate dendrites,corrosion,and hydrogen evolution reaction(HER)on Zn anodes are critical issues that severely limit the practical applications of ZIBs.To address these issues,various strategies have been proposed,and tremendous progress has been achieved in the past few years.In this article,we analyze the origins and effects of the dendrites,corrosion,and HER on Zn anodes in neutral and mildly acid aqueous solutions at first.And then,a scientific understanding of the fundamental design principles and strategies to suppress these problems are emphasized.Apart from these,this article also puts forward some requirements for the practical applications of Zn anodes as well as several cost-effectivemodifying strategies.Finally,perspectives on the future development of Zn anodes in aqueous solutions are also briefly anticipated.This article provides pertinent insights into the challenges on anodes for the development of highperformance ZIBs,which will greatly contribute to their practical applications.展开更多
The Ni-W-WC composite-coating electrode was prepared by electrolytic compos- ite-deposition. The characterization for the hydrogen evolution reaction(HER) was compared in 7 mol· L -1 KOH solution by steady-state ...The Ni-W-WC composite-coating electrode was prepared by electrolytic compos- ite-deposition. The characterization for the hydrogen evolution reaction(HER) was compared in 7 mol· L -1 KOH solution by steady-state polarization and AC impedance technique. The results show that the composite-coating electrode is catalytically more active than Ni-W electrode. The electro- catalytic activities of the composite-coating electrode are attributed to the increase in the real surface areas and the decrease in the standard free energy of activation. The stability test of the compos- ite-coating electrode shows excellent stability during long-term continuous electrolysis and good re- sistance against frequent power interruption on this electrode.展开更多
With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and...With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and development of high-performance catalysts remains rather challenging.As the compositions and structures of catalyst interfaces have paramount influences on the catalytic performances,the central topic here has always been to design and engineer the interface structures via rational routes so as to boost the activities and stabilities of electrocatalysts on hydrogen evolution reaction(HER).Here in this review,we focus on the design and preparation of multi-scale catalysts specifically catering to HER applications.We start from the design and structure-activity relationship of catalytic nanostructures,summarize the research progresses related to HER nanocatalysts,and interpret their high activities from the atomistic perspective;then,we review the studies regarding the design,preparation,HER applications and structure-activity relationship of single-atom site catalysts(SASCs),and thereupon discuss the future directions in designing HER-oriented SASCs.At the end of this review,we present an outlook on the development trends and faced challenges of catalysts for electrochemical HER.展开更多
Transition metal phosphides (TMPs) are promising candidates for noble metal free electrocatalysts in water splitting applicati ons. In this work, we prese nt the facile syn thesis of nickel cobalt phosphide electrocat...Transition metal phosphides (TMPs) are promising candidates for noble metal free electrocatalysts in water splitting applicati ons. In this work, we prese nt the facile syn thesis of nickel cobalt phosphide electrocatalyst with three-dime nsional nano structure (3D-NiCoP) on the nickel foam, via hydrothermal reaction and phosphorization. The as-prepared electrocatalyst exhibits an excellent activity for hydrogen evolution reaction (HER) in both acidic and alkaline electrolytes, with small overpotentials to drive 10 mA/cm^2 (80 mV for 0.5 M H2SO4, 105 mV for 1 M KOH), small Tafel slopes (37 mV/dec for 0.5 M H2SO4, 79 mV/dec for 1 M KOH), and satisfying durability in long-term electrolysis. 3D-NiCoP also shows a superior HER activity compared to single metal phosphide, such as cobalt phosphide and nickel phosphide. The outstanding performa nee for HER suggests the great pote ntial of 3D-NiCoP as a highly efficient electrocatalyst for water splitting technology.展开更多
The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corro...The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.展开更多
The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we desi...The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.展开更多
Nanocarbons are of progressively increasing importance in energy electrocatalysis, including oxygen reduction, oxygen evolution, hydrogen evolution, COreduction, etc. Precious-metal-free or metal-free nanocarbon-based...Nanocarbons are of progressively increasing importance in energy electrocatalysis, including oxygen reduction, oxygen evolution, hydrogen evolution, COreduction, etc. Precious-metal-free or metal-free nanocarbon-based electrocatalysts have been revealed to potentially have effective activity and remarkable durability, which is promising to replace precious metals in some important energy technologies,such as fuel cells, metal–air batteries, and water splitting. In this review, rather than overviewing recent progress completely, we aim to give an in-depth digestion of present achievements, focusing on the different roles of nanocarbons and material design principles. The multifunctionalities of nanocarbon substrates(accelerating the electron and mass transport, regulating the incorporation of active components,manipulating electron structures, generating confinement effects, assembly into 3 D free-standing electrodes) and the intrinsic activity of nanocarbon catalysts(multi-heteroatom doping, hierarchical structure,topological defects) are discussed systematically, with perspectives on the further research in this rising research field. This review is inspiring for more insights and methodical research in mechanism understanding, material design, and device optimization, leading to a targeted and high-efficiency development of energy electrocatalysis.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51772249 and 51821091)the Fundamental Research Funds for the Central Universities(Nos.G2017KY0308 and 3102019JC005)+2 种基金the Natural Science Foundation of Shaanxi Province(Nos.2018JM5092 and 2019JLM-26)the Innovation Program for Talent(No.2019KJXX066)the Post-doctoral Program of Shaanxi Province(No.2018BSHTDZZ16)
文摘Water electrolysis has been considered as a sustainable way for producing renewable energy of hydrogen.However,this process requires a low-cost and high-efficient hydrogen evolution reaction(HER)catalyst to improve the overall reaction efficiency.Molybdenum(Mo)-based electrocatalysts are regarded as the promising candidates to replace the benchmark but expensive Ptbased HER catalysts,due to their high activity and stability in a wide pH range.In this review,we present a comprehensive and critical summary on the recent progress in the Mo-based electrodes for HER,including molybdenum alloys,molybdenum sulfides,molybdenum selenides,molybdenum carbides,molybdenum phosphides,molybdenum borides,molybdenum nitrides,and molybdenum oxides.Particular attention is mainly focused on the synthetic methods of Mo-based materials,the strategies for increasing the catalytic activity,and the relationship between structure/composition and electrocatalytic performance.Finally,the future development and perspectives of Mo-based electrocatalysts toward high HER performance are proposed.
基金supported by National Natural Science Foundation of China(Grants 51972346,51802356,51932011,and 51872334)Innovation-Driven Project of Central South University(2020CX024)
文摘Rechargeable aqueous zinc-ion batteries(ZIBs) featuring the merits of low cost,eco-friendliness,and enhanced safety have attracted extensive interests and considered as the most promising energy storage system.However,much efforts are devoted to the exploration of cathode materials and their storage mechanisms in this system,and inadequate attentions are received in regard to anode side especially in neutral or mild acidic electrolyte.Therefore,in this review,the fundamental understanding of existing issues including dendrite formation,corrosion,and hydrogen evolution are mainly revealed,as well as their interaction in neutral or mild acidic medium.In addition,the currently existing solution strategies on the anode are summarized and the mechanisms that contained are simultaneously investigated.Finally,perspectives on future anode modification and innovation direction are provided for the further development and research of Zn-based ZIBs.
基金the National Key Research and Development Program of China(No.2018YFA0702003)the National Natural Science Foundation of China(Nos.21890383 and 21871159)+1 种基金the Science and Technology Key Project of Guangdong Province of China(No.2020B010188002)China Postdoctoral Science Foundation(2021M691834).
文摘Hydrogen production from water splitting using renewable electric energy is an interesting topic towards the carbon neutral future.Single atom catalysts(SACs)have emerged as a new frontier in the field of catalysis such as hydrogen evolution reaction(HER),owing to their intriguing properties like high activity and excellent chemical selectivity.The catalytic active moiety is often comprised of a single metal atom and its neighboring environment from the supports.Recent published reviews about electricdriven HER tend to classify these SACs by the species of active center atom,nevertheless the influence of their neighboring coordinated atoms from the supports is somehow neglected.Thus we classify the SACs for HER through the type of supports,highlighting the electronic metal–support interaction and their coordination environment from support.Then,we put forward some structural designing strategies including regulating of the central atoms,coordination environments,and metal-support interactions.Finally,the current challenges and future research perspectives of SACs for HER are briefly proposed.
基金This study was financially supported by the National Nature Science Foundation of China(No.:21975289,U19A2019,and 21905306)Hunan Provincial Research and Development Plan in Key Areas(No.:2019GK2033)Hunan Provincial Science and Technology Plan Project of China(No.:2017TP1001 and 2018RS3009).
文摘Aqueous zinc-ion batteries(ZIBs)have been intensively investigated as potential energy storage devices on account of their low cost,environmental benignity,and intrinsically safe merits.With the exploitation of highperformance cathode materials,electrolyte systems,and in-depth mechanism investigation,the electrochemical performances of ZIBs have been greatly enhanced.However,there are still some challenges that need to be overcome before its commercialization.Among them,the obstinate dendrites,corrosion,and hydrogen evolution reaction(HER)on Zn anodes are critical issues that severely limit the practical applications of ZIBs.To address these issues,various strategies have been proposed,and tremendous progress has been achieved in the past few years.In this article,we analyze the origins and effects of the dendrites,corrosion,and HER on Zn anodes in neutral and mildly acid aqueous solutions at first.And then,a scientific understanding of the fundamental design principles and strategies to suppress these problems are emphasized.Apart from these,this article also puts forward some requirements for the practical applications of Zn anodes as well as several cost-effectivemodifying strategies.Finally,perspectives on the future development of Zn anodes in aqueous solutions are also briefly anticipated.This article provides pertinent insights into the challenges on anodes for the development of highperformance ZIBs,which will greatly contribute to their practical applications.
文摘The Ni-W-WC composite-coating electrode was prepared by electrolytic compos- ite-deposition. The characterization for the hydrogen evolution reaction(HER) was compared in 7 mol· L -1 KOH solution by steady-state polarization and AC impedance technique. The results show that the composite-coating electrode is catalytically more active than Ni-W electrode. The electro- catalytic activities of the composite-coating electrode are attributed to the increase in the real surface areas and the decrease in the standard free energy of activation. The stability test of the compos- ite-coating electrode shows excellent stability during long-term continuous electrolysis and good re- sistance against frequent power interruption on this electrode.
基金Acknowledgements This work was supported by the National Key R&D Program of China(2016YFA0202801,2017YFA0700101 and 2018YFA0702003)the National Natural Science Foundation of China(21925202,21872076 and 21890383)+4 种基金Beijing Natural Science Foundation(JQ18007)the Fundamental Research Funds for the Central Universities(19CX02008A)the Petro China Innovation Foundation(2019D-5007-0401)Taishan Scholars Program of Shandong Province(tsqn201909065)Tsinghua University Initiative Scientific Research Program.
文摘With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and development of high-performance catalysts remains rather challenging.As the compositions and structures of catalyst interfaces have paramount influences on the catalytic performances,the central topic here has always been to design and engineer the interface structures via rational routes so as to boost the activities and stabilities of electrocatalysts on hydrogen evolution reaction(HER).Here in this review,we focus on the design and preparation of multi-scale catalysts specifically catering to HER applications.We start from the design and structure-activity relationship of catalytic nanostructures,summarize the research progresses related to HER nanocatalysts,and interpret their high activities from the atomistic perspective;then,we review the studies regarding the design,preparation,HER applications and structure-activity relationship of single-atom site catalysts(SASCs),and thereupon discuss the future directions in designing HER-oriented SASCs.At the end of this review,we present an outlook on the development trends and faced challenges of catalysts for electrochemical HER.
基金the National Natural Science Foundation of China (No. 51702234).
文摘Transition metal phosphides (TMPs) are promising candidates for noble metal free electrocatalysts in water splitting applicati ons. In this work, we prese nt the facile syn thesis of nickel cobalt phosphide electrocatalyst with three-dime nsional nano structure (3D-NiCoP) on the nickel foam, via hydrothermal reaction and phosphorization. The as-prepared electrocatalyst exhibits an excellent activity for hydrogen evolution reaction (HER) in both acidic and alkaline electrolytes, with small overpotentials to drive 10 mA/cm^2 (80 mV for 0.5 M H2SO4, 105 mV for 1 M KOH), small Tafel slopes (37 mV/dec for 0.5 M H2SO4, 79 mV/dec for 1 M KOH), and satisfying durability in long-term electrolysis. 3D-NiCoP also shows a superior HER activity compared to single metal phosphide, such as cobalt phosphide and nickel phosphide. The outstanding performa nee for HER suggests the great pote ntial of 3D-NiCoP as a highly efficient electrocatalyst for water splitting technology.
基金supported by the National Natural Science Foundation of China(No.52071171)Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC1802005)+5 种基金Liaoning BaiQianWan Talents Program(LNBQW2018B0048)Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)Foundation for Young Scholars of Liaoning University(a252102001)Australian Research Council(ARC)Future Fellowship(FT210100298)CSIRO Energy Centre,Kick-Start Project and the Victorian Government’s support through the provision of a grant from veski-Study Melbourne Research Partnerships(SMRP)project.
文摘The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.
文摘The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.
基金supported by the National Key Research and Development Program (Nos. 2016YFA0202500 and 2016YFA0200102)the Natural Scientific Foundation of China (No. 21561130151)Royal Society for the award of a Newton Advanced Fellowship (Ref: NA140249)
文摘Nanocarbons are of progressively increasing importance in energy electrocatalysis, including oxygen reduction, oxygen evolution, hydrogen evolution, COreduction, etc. Precious-metal-free or metal-free nanocarbon-based electrocatalysts have been revealed to potentially have effective activity and remarkable durability, which is promising to replace precious metals in some important energy technologies,such as fuel cells, metal–air batteries, and water splitting. In this review, rather than overviewing recent progress completely, we aim to give an in-depth digestion of present achievements, focusing on the different roles of nanocarbons and material design principles. The multifunctionalities of nanocarbon substrates(accelerating the electron and mass transport, regulating the incorporation of active components,manipulating electron structures, generating confinement effects, assembly into 3 D free-standing electrodes) and the intrinsic activity of nanocarbon catalysts(multi-heteroatom doping, hierarchical structure,topological defects) are discussed systematically, with perspectives on the further research in this rising research field. This review is inspiring for more insights and methodical research in mechanism understanding, material design, and device optimization, leading to a targeted and high-efficiency development of energy electrocatalysis.
