This work creates a droplet battery model based on the electrolyte performance in the porous electrode, studies the current density on the mesoscopic scale, and explains how the mesoscopic structure of the porous elec...This work creates a droplet battery model based on the electrolyte performance in the porous electrode, studies the current density on the mesoscopic scale, and explains how the mesoscopic structure of the porous electrode influences the current density on the air-diffusion electrode. Near the three-phase line, there is a strong band containing nearly 80% current. For porous electrodes, the total current is proportional to the length of the strong band. Thus, it can be inferred that on the macroscopic scale, the longer the total length of the strong band on unit area is, the larger the current density is.展开更多
The explore and development of electrocatalysts have gained significant attention due to their indispensable status in energy storage and conversion systems, such as fuel cells, metal–air batteries and solar water sp...The explore and development of electrocatalysts have gained significant attention due to their indispensable status in energy storage and conversion systems, such as fuel cells, metal–air batteries and solar water splitting cells. Layered double hydroxides(LDHs) and their derivatives(e.g., transition metal alloys, oxides, sulfides, nitrides and phosphides) have been adopted as catalysts for various electrochemical reactions, such as oxygen reduction, oxygen evolution, hydrogen evolution, and COreduction, which show excellent activity and remarkable durability in electrocatalytic process. In this review, the synthesis strategies, structural characters and electrochemical performances for the LDHs and their derivatives are described. In addition, we also discussed the effect of electronic and geometry structures to their electrocatalytic activity. The further development of high-performance electrocatalysts based on LDHs and their derivatives is covered by both a short summary and future outlook from the viewpoint of the material design and practical application.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
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav...The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.展开更多
With the rapid development of wearable and intelligent flexible electronic devices(FEDs),the demand for flexible energy storage/conversion devices(ESCDs)has also increased.Rechargeable flexible metal‐air batteries(MA...With the rapid development of wearable and intelligent flexible electronic devices(FEDs),the demand for flexible energy storage/conversion devices(ESCDs)has also increased.Rechargeable flexible metal‐air batteries(MABs)are expected to be one of the most ideal ESCDs due to their high theoretical energy density,cost advantage,and strong deformation adaptability.With the improvement of the device design,material assemblies,and manufacturing technology,the research on the electrochemical performance of flexible MABs has made significant progress.However,achieving the high mechanical flexibility,high safety,and wearable comfortability required by FEDs while maintaining the high performance of flexible MABs are still a daunting challenge.In this review,flexible Zn‐air and Li‐air batteries are mainly exemplified to describe the most recent progress and challenges of flexible MABs.We start with an overview of the structure and configuration of the flexible MABs and discuss their impact on battery performance and function.Then it focuses on the research progress of flexible metal anodes,gel polymer electrolytes,and air cathodes.Finally,the main challenges and future research perspectives involving flexible MABs for FEDs are proposed.展开更多
Electrochemical transformation processes involving carbon,hydrogen,oxygen,nitrogen,and small-molecule chemistries represent a promising means to store renewable energy sources in the form of chemical energy.However,th...Electrochemical transformation processes involving carbon,hydrogen,oxygen,nitrogen,and small-molecule chemistries represent a promising means to store renewable energy sources in the form of chemical energy.However,their widespread deployment is hindered by a lack of efficient,selective,durable,and affordable electrocatalysts.Recently,grain boundary(GB)engineering as one category of defect engineering,has emerged as a viable and powerful pathway to achieve improved electrocatalytic performances.This review presents a timely and comprehensive overview of recent advances in GB engineering for efficient electrocatalysis.The beneficial effects of introducing GBs into electrocatalysts are discussed,followed by an overview of the synthesis and characterization of GB-enriched electrocatalysts.Importantly,the latest developments in leveraging GB engineering for enhanced electrocatalysis are thoroughly examined,focusing on the electrochemical utilization cycles of carbon,hydrogen,oxygen,and nitrogen.Future research directions are proposed to further advance the understanding and application of GB engineering for improved electrocatalysis.展开更多
Graphene, with unique two-dimensional form and numerous appealing properties, promises to remarkably increase the energy density and power density of electrochemical energy storage devices(EESDs),ranging from the popu...Graphene, with unique two-dimensional form and numerous appealing properties, promises to remarkably increase the energy density and power density of electrochemical energy storage devices(EESDs),ranging from the popular lithium ion batteries and supercapacitors to next-generation high-energy batteries. Here, we review the recent advances of the state-of-the-art graphene-based materials for EESDs,including lithium ion batteries, supercapacitors, micro-supercapacitors, high-energy lithium-air and lithium-sulfur batteries, and discuss the importance of the pore, doping, assembly, hybridization and functionalization of different nano-architectures in improving electrochemical performance. The major roles of graphene are highlighted as(1) a superior active material,(2) ultrathin 2D flexible support,and(3) an inactive yet electrically conductive additive. Furthermore, we address the enormous potential of graphene for constructing new-concept emerging graphene-enabled EESDs with multiple functionalities of lightweight, ultra-flexibility, thinness, and novel cell configurations. Finally, future perspectives and challenges of graphene-based EESDs are briefly discussed.展开更多
文摘This work creates a droplet battery model based on the electrolyte performance in the porous electrode, studies the current density on the mesoscopic scale, and explains how the mesoscopic structure of the porous electrode influences the current density on the air-diffusion electrode. Near the three-phase line, there is a strong band containing nearly 80% current. For porous electrodes, the total current is proportional to the length of the strong band. Thus, it can be inferred that on the macroscopic scale, the longer the total length of the strong band on unit area is, the larger the current density is.
基金supported by the National Natural Science Foundation of China(Nos.U146211821601011)+2 种基金the 973 Program(Grant No.2014CB932102)the Fundamental Research Funds for the Central Universities(buctrc201506PYCC1704)
文摘The explore and development of electrocatalysts have gained significant attention due to their indispensable status in energy storage and conversion systems, such as fuel cells, metal–air batteries and solar water splitting cells. Layered double hydroxides(LDHs) and their derivatives(e.g., transition metal alloys, oxides, sulfides, nitrides and phosphides) have been adopted as catalysts for various electrochemical reactions, such as oxygen reduction, oxygen evolution, hydrogen evolution, and COreduction, which show excellent activity and remarkable durability in electrocatalytic process. In this review, the synthesis strategies, structural characters and electrochemical performances for the LDHs and their derivatives are described. In addition, we also discussed the effect of electronic and geometry structures to their electrocatalytic activity. The further development of high-performance electrocatalysts based on LDHs and their derivatives is covered by both a short summary and future outlook from the viewpoint of the material design and practical application.
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.
基金the Natural Science Foundation of China (22005250)National Key R D Program of China (2022YFB2502000)FWO (12ZV320N)。
文摘The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.
基金supported by the the National Natural This study was financially supported by the National Youth Top‐notch Talent Support Program,the State Key Laboratory of Pulp and Paper Engineering Funds(2020C03)the National Natural Science Foundation of China(31971614,32071714,21736003,and 52003083)+2 种基金Guangzhou Science and Technology Funds(201904010078 and 202002030167)the China Postdoctoral Science Foundation funded project(2019T120725,2019M652882,2019M662924,2020M682711,and 2020M682710)Guangdong Basic and Applied Basic Research Foundation(2020A1515110705)。
文摘With the rapid development of wearable and intelligent flexible electronic devices(FEDs),the demand for flexible energy storage/conversion devices(ESCDs)has also increased.Rechargeable flexible metal‐air batteries(MABs)are expected to be one of the most ideal ESCDs due to their high theoretical energy density,cost advantage,and strong deformation adaptability.With the improvement of the device design,material assemblies,and manufacturing technology,the research on the electrochemical performance of flexible MABs has made significant progress.However,achieving the high mechanical flexibility,high safety,and wearable comfortability required by FEDs while maintaining the high performance of flexible MABs are still a daunting challenge.In this review,flexible Zn‐air and Li‐air batteries are mainly exemplified to describe the most recent progress and challenges of flexible MABs.We start with an overview of the structure and configuration of the flexible MABs and discuss their impact on battery performance and function.Then it focuses on the research progress of flexible metal anodes,gel polymer electrolytes,and air cathodes.Finally,the main challenges and future research perspectives involving flexible MABs for FEDs are proposed.
基金Australian Research Council Discovery Projects,Grant/Award Numbers:DP200103332,DP200103315,DP230100685Australian Research Council Industrial Transformation Research Hubs,Grant/Award Number:IH220100012Australian Research Council Discovery Early Career Researcher Award,Grant/Award Number:DE240101013。
文摘Electrochemical transformation processes involving carbon,hydrogen,oxygen,nitrogen,and small-molecule chemistries represent a promising means to store renewable energy sources in the form of chemical energy.However,their widespread deployment is hindered by a lack of efficient,selective,durable,and affordable electrocatalysts.Recently,grain boundary(GB)engineering as one category of defect engineering,has emerged as a viable and powerful pathway to achieve improved electrocatalytic performances.This review presents a timely and comprehensive overview of recent advances in GB engineering for efficient electrocatalysis.The beneficial effects of introducing GBs into electrocatalysts are discussed,followed by an overview of the synthesis and characterization of GB-enriched electrocatalysts.Importantly,the latest developments in leveraging GB engineering for enhanced electrocatalysis are thoroughly examined,focusing on the electrochemical utilization cycles of carbon,hydrogen,oxygen,and nitrogen.Future research directions are proposed to further advance the understanding and application of GB engineering for improved electrocatalysis.
基金supported by the National Key Research and Development Program of China (2016YBF0100100, 2016YFA0200101, and 2016YFA0200200)the National Natural Science Foundation of China (51572259, 51325205, 51290273, and 51521091)+3 种基金the Natural Science Foundation of Liaoning Province (201602737)the Thousand Youth Talents Plan of China (Y5610121T3)China Postdoctoral Science Foundation (2016M601349)dedicated funds for methanol conversion from Dalian Institute of Chemical Physics, Chinese Academy of Sciences
文摘Graphene, with unique two-dimensional form and numerous appealing properties, promises to remarkably increase the energy density and power density of electrochemical energy storage devices(EESDs),ranging from the popular lithium ion batteries and supercapacitors to next-generation high-energy batteries. Here, we review the recent advances of the state-of-the-art graphene-based materials for EESDs,including lithium ion batteries, supercapacitors, micro-supercapacitors, high-energy lithium-air and lithium-sulfur batteries, and discuss the importance of the pore, doping, assembly, hybridization and functionalization of different nano-architectures in improving electrochemical performance. The major roles of graphene are highlighted as(1) a superior active material,(2) ultrathin 2D flexible support,and(3) an inactive yet electrically conductive additive. Furthermore, we address the enormous potential of graphene for constructing new-concept emerging graphene-enabled EESDs with multiple functionalities of lightweight, ultra-flexibility, thinness, and novel cell configurations. Finally, future perspectives and challenges of graphene-based EESDs are briefly discussed.