摘要
Clearly understanding the structure-function relationship and rational design of efficient CO2 electrocatalysts are still the challenges.This article describes the molecular origin of high selectivity of formic acid on N-doped SnO2 nanoparticles,which obtained via thermal treatment of g-C3N4 and SnCl2·2H2O precursor.Combined with density functional theory(DFT)calculations,we discover that N-doping effectively introduces oxygen vacancies and increases the charge density of Sn sites,which plays a positive role in CO2 activation.In addition,N-doping further regulates the adsorption energy of^*OCHO,^*COOH,^*H and promotes HCOOH generation.Benefited from above modulation,the obtained N-doped SnO2 catalysts with oxygen vacancies(Ov-N-SnO2)exhibit faradaic efficiency of 93% for C1 formation,88% for HCOOH production and well-suppression of H2 evolution over a wide range of potentials.
Clearly understanding the structure-function relationship and rational design of efficient CO2 electrocatalysts are still the challenges.This article describes the molecular origin of high selectivity of formic acid on N-doped SnO2 nanoparticles,which obtained via thermal treatment of g-C3N4 and SnCl2·2H2O precursor.Combined with density functional theory（DFT）calculations,we discover that N-doping effectively introduces oxygen vacancies and increases the charge density of Sn sites,which plays a positive role in CO2 activation.In addition,N-doping further regulates the adsorption energy of*OCHO,*COOH,*H and promotes HCOOH generation.Benefited from above modulation,the obtained N-doped SnO2 catalysts with oxygen vacancies（Ov-N-SnO2）exhibit faradaic efficiency of 93% for C1 formation,88% for HCOOH production and well-suppression of H2 evolution over a wide range of potentials.
基金
supported by the National Key R&D Program of China (2016YFB0600901)
the National Natural Science Foundation of China (21525626, 21606169, 21722608)
the Program of Introducing Talents of Discipline to Universities (B06006)
