The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfa...The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfactory Coulombic efficiency and low Zn utilization.Therefore,exploiting appropriate insertion-type anodes with fast charge-transfer kinetics is of great importance,and many modifications focusing on the improvement of electron transport and bulk Zn^(2+)diffusion have been proposed.However,the interfacial Zn^(2+)transfer determined by the desolvation process actually dominates the kinetics of overall battery reactions,which is mainly overlooked.Herein,the interlayer structure of Mo S_(2)is rationally co-intercalated with water and ethylene glycol(EG)molecules(Mo S2@EG),giving rise to a fast non-desolvation Zn^(2+)storage mechanism,which is verified by the extraordinarily smaller activation energy of interfacial Zn^(2+)transfer(4.66 k J mol^(-1))compared with that of pristine Mo S_(2)(56.78 k J mol^(-1)).Furthermore,the results of theoretical calculations,in-situ Raman and ex-situ characterizations also indicate the enhanced structural integrity of Mo S2@EG during cycling due to the enlarged interlayer spacing and charge screening effect induced by interlaminar EG molecules.Consequently,the Mo S_(2)@EG anode enables excellent cycling stability of both high-energy-density Mo_S2@EG||PVO(polyaniline intercalated V_(2)O_(5))and high-voltage Mo S2@EG||Na_(3)V_(2)(PO_(4))_2O_(2)F(NVPF)full batteries with neglectable capacity decay at-20℃.展开更多
基金supported by the National Natural Science Foundation of China(22109030,22021001)the Fundamental Research Funds for the Central Universities(20720220073)+3 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Fujian Industrial Technology Development and Application Plan(2022I0002)the Guangdong Basic and Applied Basic Research Foundation(2019A1515111069,2021A1515010177)the financial support from Guangdong Basic and Applied Basic Research Foundation(2020A1515010886)。
文摘The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfactory Coulombic efficiency and low Zn utilization.Therefore,exploiting appropriate insertion-type anodes with fast charge-transfer kinetics is of great importance,and many modifications focusing on the improvement of electron transport and bulk Zn^(2+)diffusion have been proposed.However,the interfacial Zn^(2+)transfer determined by the desolvation process actually dominates the kinetics of overall battery reactions,which is mainly overlooked.Herein,the interlayer structure of Mo S_(2)is rationally co-intercalated with water and ethylene glycol(EG)molecules(Mo S2@EG),giving rise to a fast non-desolvation Zn^(2+)storage mechanism,which is verified by the extraordinarily smaller activation energy of interfacial Zn^(2+)transfer(4.66 k J mol^(-1))compared with that of pristine Mo S_(2)(56.78 k J mol^(-1)).Furthermore,the results of theoretical calculations,in-situ Raman and ex-situ characterizations also indicate the enhanced structural integrity of Mo S2@EG during cycling due to the enlarged interlayer spacing and charge screening effect induced by interlaminar EG molecules.Consequently,the Mo S_(2)@EG anode enables excellent cycling stability of both high-energy-density Mo_S2@EG||PVO(polyaniline intercalated V_(2)O_(5))and high-voltage Mo S2@EG||Na_(3)V_(2)(PO_(4))_2O_(2)F(NVPF)full batteries with neglectable capacity decay at-20℃.