Aqueous zinc-ion batteries(AZIBs)are promising for large-scale energy storage,but their development is plagued by inadequate cycle life.Here,for the first time,we reveal an unusual phenomenon of cathodic underpotentia...Aqueous zinc-ion batteries(AZIBs)are promising for large-scale energy storage,but their development is plagued by inadequate cycle life.Here,for the first time,we reveal an unusual phenomenon of cathodic underpotential deposition(UPD)of Zn,which is highly irreversible and considered the origin of the inferior cycling stability of AZIBs.Combining experimental and theoretical simulation approaches,we propose that the UPD process agrees with a two-dimensional nucleation and growth model,following a thermodynamically feasible mechanism.Furthermore,the universality of Zn UPD is identified in systems,including VO_(2)//Zn,TiO_(2)//Zn,and SnO_(2)//Zn.In practice,we propose and successfully implement removing cathodic Zn UPD and substantially mitigate the degradation of the battery by controlling the end-ofdischarge voltage.This work provides new insights into AZIBs degradation and brings the cathodic UPD behavior of rechargeable batteries into the limelight.展开更多
基金supported by the National Key Research and Development Program of China(2020YFA0715000 and 2016YFA0202603)the National Natural Science Foundation of China(51832004,51521001,and 22109029)。
文摘Aqueous zinc-ion batteries(AZIBs)are promising for large-scale energy storage,but their development is plagued by inadequate cycle life.Here,for the first time,we reveal an unusual phenomenon of cathodic underpotential deposition(UPD)of Zn,which is highly irreversible and considered the origin of the inferior cycling stability of AZIBs.Combining experimental and theoretical simulation approaches,we propose that the UPD process agrees with a two-dimensional nucleation and growth model,following a thermodynamically feasible mechanism.Furthermore,the universality of Zn UPD is identified in systems,including VO_(2)//Zn,TiO_(2)//Zn,and SnO_(2)//Zn.In practice,we propose and successfully implement removing cathodic Zn UPD and substantially mitigate the degradation of the battery by controlling the end-ofdischarge voltage.This work provides new insights into AZIBs degradation and brings the cathodic UPD behavior of rechargeable batteries into the limelight.
