Material strain and reconstruction effects are critical for catalysis reactions,but current insights into operando strain effects during reaction and means to master catalyst reconstruction are still lacking.Here,we p...Material strain and reconstruction effects are critical for catalysis reactions,but current insights into operando strain effects during reaction and means to master catalyst reconstruction are still lacking.Here,we propose a facile thermal-induced phase-segregation strategy to simultaneously master material operando strain and reconstruction effects for enhanced oxygen-evolving reaction(OER).Specifically,self-assembled and controllable layered LiCoO_(2)phase and Co_(3)O_(4)spinel can be generated from pristine Li2Co_(2)O_(4)spinel via Li and O volatilization under different temperatures,realizing controllable proportions of two phases by calcination temperature.Combined operando and ex-situ characterizations reveal that obvious tensile strain along(003)plane appears on layered LixCoO_(2)phase during OER,while low-valence Co_(3)O_(4)phase transforms into high-valence CoOOHx,realizing simultaneous operando strain and reconstruction effects.Further experimental and computational investigations demonstrate that both strained LixCoO_(2)phase and reconstructed CoOOHxcompound contribute to the beneficial adsorption of important OH-reactants,while respective roles in activity and stability are uncovered by exploring their latticeoxygen participation mechanism.This work not only reveals material operando strain effects during OER,but also inaugurates a new thermal-induced phase-segregation strategy to artificially master material operando strain and reconstruction effects,which will enlighten rational material design for many potential reactions and applications.展开更多
基金funded by the Australian Research Council Discovery Projects(DP160104835,Z.Shao)the Guangdong Basic and Applied Basic Research Foundation(2023A1515012878,D.Guan)+1 种基金the PolyU Distinguished Postdoctoral Fellowship Scheme(1-YWBU,D.Guan)the support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials。
文摘Material strain and reconstruction effects are critical for catalysis reactions,but current insights into operando strain effects during reaction and means to master catalyst reconstruction are still lacking.Here,we propose a facile thermal-induced phase-segregation strategy to simultaneously master material operando strain and reconstruction effects for enhanced oxygen-evolving reaction(OER).Specifically,self-assembled and controllable layered LiCoO_(2)phase and Co_(3)O_(4)spinel can be generated from pristine Li2Co_(2)O_(4)spinel via Li and O volatilization under different temperatures,realizing controllable proportions of two phases by calcination temperature.Combined operando and ex-situ characterizations reveal that obvious tensile strain along(003)plane appears on layered LixCoO_(2)phase during OER,while low-valence Co_(3)O_(4)phase transforms into high-valence CoOOHx,realizing simultaneous operando strain and reconstruction effects.Further experimental and computational investigations demonstrate that both strained LixCoO_(2)phase and reconstructed CoOOHxcompound contribute to the beneficial adsorption of important OH-reactants,while respective roles in activity and stability are uncovered by exploring their latticeoxygen participation mechanism.This work not only reveals material operando strain effects during OER,but also inaugurates a new thermal-induced phase-segregation strategy to artificially master material operando strain and reconstruction effects,which will enlighten rational material design for many potential reactions and applications.
