Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze...Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze CO2 reduction reaction(CO2RR)still cannot meet the requirements of commercial-scale applications.Therefore developing Snbased catalyst is of vital importance.Herein,the sheet-like heterophase Sn O2/Sn3O4 with a high density of phase interfaces has been first engineered by a facile hydrothermal process,with Sn3O4 as the dominant phase.The evidences from experiments and theoretical simulation indicate that the charge redistribution and built-in electric field at heterophase interfaces boost CO2 adsorption and HCOO*formation,accelerate the charge transfer between the catalysts and reactants,and ultimately greatly elevate the intrinsic activity of the heterophase Sn O2/Sn3O4 towards CO2 RR.Meanwhile,the in-situ generated porous structure and metal Sn during CO2 RR improve the mass transmission within the interlayer volume and the conductivity of Sn O2/Sn3O4.The heterophase Sn O2/Sn3O4 displays high activity and selectivity for CO2 RR,achieving an improvement in CO2 reduction current density,88.3%Faradaic efficiency of HCOOH conversion at-0.9 VRHE,along with a long-term tolerance in CO2 RR.This study demonstrates that heterophase interface engineering is an efficient strategy to regulate advanced catalysts for different applications.展开更多
基金supported by the National Natural Science Foundation of China(20973048)Key Laboratory of Superlight Material and Surface Technology of Ministry of Education of China+1 种基金Heilongjiang Postdoc Foundation,China(LBH-Q06091)Fund of Harbin Engineering University,China(HEUFT07030,HEUFT07051)~~
基金the National Natural Science Foundation of China(21573062,21631004 and 21901065)the Natural Science Foundation of Heilongjiang Province(B2018008)+1 种基金the Youth Science and Technology Innovation Team Project of Heilongjiang Province(2018-KYYWF-1593)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2018009)。
文摘Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze CO2 reduction reaction(CO2RR)still cannot meet the requirements of commercial-scale applications.Therefore developing Snbased catalyst is of vital importance.Herein,the sheet-like heterophase Sn O2/Sn3O4 with a high density of phase interfaces has been first engineered by a facile hydrothermal process,with Sn3O4 as the dominant phase.The evidences from experiments and theoretical simulation indicate that the charge redistribution and built-in electric field at heterophase interfaces boost CO2 adsorption and HCOO*formation,accelerate the charge transfer between the catalysts and reactants,and ultimately greatly elevate the intrinsic activity of the heterophase Sn O2/Sn3O4 towards CO2 RR.Meanwhile,the in-situ generated porous structure and metal Sn during CO2 RR improve the mass transmission within the interlayer volume and the conductivity of Sn O2/Sn3O4.The heterophase Sn O2/Sn3O4 displays high activity and selectivity for CO2 RR,achieving an improvement in CO2 reduction current density,88.3%Faradaic efficiency of HCOOH conversion at-0.9 VRHE,along with a long-term tolerance in CO2 RR.This study demonstrates that heterophase interface engineering is an efficient strategy to regulate advanced catalysts for different applications.
