Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of prot...Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of proton transport in transition metal oxides,which dates back to 1971[3]when RuO_(2) was discovered to be capable of storing protons via reversible redox reactions[4].In aqueous electrolytes,the thin film RuO_(2) electrode exhibits a surface pseudocapacitive behavior[5],which could be modified by the structural water in its hydrated form due to the facile Grotthuss hopping mode of protons along the established hydrogen bonds inside the bulk phase[6].Soon later,Goodenough et al.reported the capacitor-like behavior of amorphous MnO_(2)·xH_(2)O electrode in an aqueous KCl electrolyte[7],and further studies on the hydrated MnO_(2) electrodes prepared by sol-gel processes have soon discovered that the intercalation of protons from aqueous electrolytes plays an indispensable role in the charge storage mechanism[8].In recent years,the research interest on rechargeable aqueous batteries has fueled the renaissance of mechanistic study of proton transport in transition metal oxides[9],which can operate as cathodes or anodes via a topotactic insertion mechanism similar to that in Li-ion batteries[10].However,due to the challenges for experimental detection of local chemical environments of the inserted protons,a comprehensive understanding of proton dynamic behavior in these electrodes remains largely lacking.展开更多
基金financial support from the National Natural Science Foundation of China(22109003)the Basic and Applied Basic Research Foundation of Guangdong Province(2023A1515011391)+1 种基金Soft Science Research Project of Guangdong Province(No.2017B030301013)the Major Science and Technology Infrastructure Project of Material Genome Big-science Facilities Platform supported by Municipal Development and Reform Commission of Shenzhen.
文摘Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of proton transport in transition metal oxides,which dates back to 1971[3]when RuO_(2) was discovered to be capable of storing protons via reversible redox reactions[4].In aqueous electrolytes,the thin film RuO_(2) electrode exhibits a surface pseudocapacitive behavior[5],which could be modified by the structural water in its hydrated form due to the facile Grotthuss hopping mode of protons along the established hydrogen bonds inside the bulk phase[6].Soon later,Goodenough et al.reported the capacitor-like behavior of amorphous MnO_(2)·xH_(2)O electrode in an aqueous KCl electrolyte[7],and further studies on the hydrated MnO_(2) electrodes prepared by sol-gel processes have soon discovered that the intercalation of protons from aqueous electrolytes plays an indispensable role in the charge storage mechanism[8].In recent years,the research interest on rechargeable aqueous batteries has fueled the renaissance of mechanistic study of proton transport in transition metal oxides[9],which can operate as cathodes or anodes via a topotactic insertion mechanism similar to that in Li-ion batteries[10].However,due to the challenges for experimental detection of local chemical environments of the inserted protons,a comprehensive understanding of proton dynamic behavior in these electrodes remains largely lacking.
