Mg secondary batteries are promising scalable secondary batteries for next-generation energy storage.However,Mg-storage cathode materials are greatly demanded to construct high-performance Mg batteries.Electrochemical...Mg secondary batteries are promising scalable secondary batteries for next-generation energy storage.However,Mg-storage cathode materials are greatly demanded to construct high-performance Mg batteries.Electrochemical conversion reaction provides plenty of cathode options,and strategy for cathode selection and performance optimization is of special significance.In this work,Ni0.85Se with nanostructures of dispersive hexagonal nanosheets(D-Ni0.85Se)and flower-like assembled nanosheets(F-Ni0.85Se)is synthesized and investigated as Mg-storage cathodes.Compared with F-Ni0.85Se,D-Ni0.85Se delivers a higher specific capacity of 168 mAh g^-1 at 50 mA g^-1 as well as better rate performance,owing to its faster Mg^2+-diffusion and lower resistance.D-Ni0.85Se also exhibits a superior cycling stability over 500cycles.An investigation on mechanism indicates an evolution of Ni0.85Se towards NiSe with cycling,and the Mg-storage reaction occurs between NiSe and metallic Ni^0.The present work demonstrates that advanced conversion-type Mg battery cathode materials could be constructed by soft selenide anions,and the electrochemical properties could be manipulated by rational material morphology optimization.展开更多
Due to the unique interface and electronic structure,metal/metal oxide composite electrocatalysts have been designed and exploited for electrocatalytic oxygen evolution reaction(OER)in alkaline solution.However,how to...Due to the unique interface and electronic structure,metal/metal oxide composite electrocatalysts have been designed and exploited for electrocatalytic oxygen evolution reaction(OER)in alkaline solution.However,how to fabricate metal/metal oxides with abundant interfaces and well-dispersed metal phases is a challenge,and the synergistic effect between metal and metal oxides on boosting the electrocatalytic activities is still ambiguous.Herein,by controlling the lithium-induced conversion reaction of metal oxides,metal/metal oxide composites with plentiful interfaces and excellent electrical interconnection are fabricated,which can enhance the active sites,and accelerate the mass transfer during the electrocatalytic reaction.As a result,the electrocatalytic oxygen evolution activities of the as-fabricated metal/metal oxide composite catalysts including NiCo/NiCo2O4,NiMn/NiMn2O4 and CoMn/CoMn2O4 are greatly improved.The catalytic mechanism is also explored using the in-situ X-ray and Raman spectroscopic tracking to uncover the real active centers and the synergistic effect between the metal and metal oxides during water oxidation.Density functional theory plus U(DFT+U)calculation confirms the metal in the composite can optimize the catalytic reaction path and reduce the reaction barrier,thus boosting the electrocatalytic kinetics.展开更多
Lithium sulfur(Li-S)batteries are poised to be the next generation of high-density energy storage devices.In recent years,the concept of“electrocatalysis”has been introduced into the field of Li-S batteries,and some...Lithium sulfur(Li-S)batteries are poised to be the next generation of high-density energy storage devices.In recent years,the concept of“electrocatalysis”has been introduced into the field of Li-S batteries,and some transition metals have been proved to catalyze the electrochemical conversion reaction of sulfur species.In this study,carbon encapsulated nickel nanoparticles(Ni@C)with a specific surface area of 146 m^(2)/g are shown to play a definitive electrocatalytic role for the sulfur cathode.With Ni@C incorporated,the Ni@C/G-S electrode achieved a better electrochemical performance than the G-S electrode.Moreover,the reversible capacity and cycle stability were further improved through chemical modifications of the carbon shell.The influence of doping with different elements on the Li-S battery performance was also investigated in detail.Higher specific capacities of 1229 mA·h/g,927 mA·h/g,and 830 mA·h/g were achieved at 0.2 C,0.5 C,and 1.0 C for the N-Ni@C-G/S electrode.Besides,the B-Ni@C-G/S electrode possessed a best cycle stability.展开更多
基金financially supported by Intergovernmental International Science and Technology Innovation Cooperation Project(2019YFE010186)the Hubei Provincial Natural Science Foundation(2019CFB452 and 2019CFB620)the Fundamental Research Funds for the Central Universities。
文摘Mg secondary batteries are promising scalable secondary batteries for next-generation energy storage.However,Mg-storage cathode materials are greatly demanded to construct high-performance Mg batteries.Electrochemical conversion reaction provides plenty of cathode options,and strategy for cathode selection and performance optimization is of special significance.In this work,Ni0.85Se with nanostructures of dispersive hexagonal nanosheets(D-Ni0.85Se)and flower-like assembled nanosheets(F-Ni0.85Se)is synthesized and investigated as Mg-storage cathodes.Compared with F-Ni0.85Se,D-Ni0.85Se delivers a higher specific capacity of 168 mAh g^-1 at 50 mA g^-1 as well as better rate performance,owing to its faster Mg^2+-diffusion and lower resistance.D-Ni0.85Se also exhibits a superior cycling stability over 500cycles.An investigation on mechanism indicates an evolution of Ni0.85Se towards NiSe with cycling,and the Mg-storage reaction occurs between NiSe and metallic Ni^0.The present work demonstrates that advanced conversion-type Mg battery cathode materials could be constructed by soft selenide anions,and the electrochemical properties could be manipulated by rational material morphology optimization.
基金the National Natural Science Foundation of China(21603157)Young Elite Scientists Sponsorship Program by CAST(2018QNRC001)the support of Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies and Soochow University Analysis and Testing Center。
文摘Due to the unique interface and electronic structure,metal/metal oxide composite electrocatalysts have been designed and exploited for electrocatalytic oxygen evolution reaction(OER)in alkaline solution.However,how to fabricate metal/metal oxides with abundant interfaces and well-dispersed metal phases is a challenge,and the synergistic effect between metal and metal oxides on boosting the electrocatalytic activities is still ambiguous.Herein,by controlling the lithium-induced conversion reaction of metal oxides,metal/metal oxide composites with plentiful interfaces and excellent electrical interconnection are fabricated,which can enhance the active sites,and accelerate the mass transfer during the electrocatalytic reaction.As a result,the electrocatalytic oxygen evolution activities of the as-fabricated metal/metal oxide composite catalysts including NiCo/NiCo2O4,NiMn/NiMn2O4 and CoMn/CoMn2O4 are greatly improved.The catalytic mechanism is also explored using the in-situ X-ray and Raman spectroscopic tracking to uncover the real active centers and the synergistic effect between the metal and metal oxides during water oxidation.Density functional theory plus U(DFT+U)calculation confirms the metal in the composite can optimize the catalytic reaction path and reduce the reaction barrier,thus boosting the electrocatalytic kinetics.
基金This work was financially supported by the China Petrochemical Corporation(218025-9).
文摘Lithium sulfur(Li-S)batteries are poised to be the next generation of high-density energy storage devices.In recent years,the concept of“electrocatalysis”has been introduced into the field of Li-S batteries,and some transition metals have been proved to catalyze the electrochemical conversion reaction of sulfur species.In this study,carbon encapsulated nickel nanoparticles(Ni@C)with a specific surface area of 146 m^(2)/g are shown to play a definitive electrocatalytic role for the sulfur cathode.With Ni@C incorporated,the Ni@C/G-S electrode achieved a better electrochemical performance than the G-S electrode.Moreover,the reversible capacity and cycle stability were further improved through chemical modifications of the carbon shell.The influence of doping with different elements on the Li-S battery performance was also investigated in detail.Higher specific capacities of 1229 mA·h/g,927 mA·h/g,and 830 mA·h/g were achieved at 0.2 C,0.5 C,and 1.0 C for the N-Ni@C-G/S electrode.Besides,the B-Ni@C-G/S electrode possessed a best cycle stability.