Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical tran...Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.展开更多
Recently,rechargeable zinc-ion batteries have been considered as the future development direction of large-scale energy storage due to their low price,safety,environmental friendliness,and excellent electrochemical pe...Recently,rechargeable zinc-ion batteries have been considered as the future development direction of large-scale energy storage due to their low price,safety,environmental friendliness,and excellent electrochemical performance.However,highcapacity,long-cycle stable cathode materials that can meet the demand are still to be developed.Herein,the hollow mesoporous ZnMn2O4/C microsphere cathode material with carbon nanotubes embedded in the shell was prepared by spray pyrolysis for the first time.Its capacity remained at 209.71 mAh·g−1 after 150 cycles at a rate of 0.5 A·g−1,and still maintained a specific capacity of 100.06 mAh·g−1 at a rate of 1 A·g−1 after 1,000 cycles.The outstanding performance is attributed to the hollow structure that can effectively buffer large volume changes caused by ion intercalation and deintercalation,excellent porosity,cationic defects,and high electrical conductivity of carbon nanotubes and its strong adsorption to ZnMn2O4 nanoparticles.展开更多
基金the National Natural Science Foundation of China(Nos.21871005 and 22171005)the University Synergy Innovation Program of Anhui Province(Nos.GXXT-2020-005,GXXT-2021-012,and GXXT-2021-013).
文摘Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.
基金This work was supported by the National Natural Science Foundation of China(Nos.21871005 and 22171005)the University Synergy Innovation Program of Anhui Province(Nos.GXXT-2020-005,GXXT-2021-012,and GXXT-2021-013)Open project of Shanghai Institute of Technical Physics(No.IIMOKFJJ-19-09).
文摘Recently,rechargeable zinc-ion batteries have been considered as the future development direction of large-scale energy storage due to their low price,safety,environmental friendliness,and excellent electrochemical performance.However,highcapacity,long-cycle stable cathode materials that can meet the demand are still to be developed.Herein,the hollow mesoporous ZnMn2O4/C microsphere cathode material with carbon nanotubes embedded in the shell was prepared by spray pyrolysis for the first time.Its capacity remained at 209.71 mAh·g−1 after 150 cycles at a rate of 0.5 A·g−1,and still maintained a specific capacity of 100.06 mAh·g−1 at a rate of 1 A·g−1 after 1,000 cycles.The outstanding performance is attributed to the hollow structure that can effectively buffer large volume changes caused by ion intercalation and deintercalation,excellent porosity,cationic defects,and high electrical conductivity of carbon nanotubes and its strong adsorption to ZnMn2O4 nanoparticles.