The formaldehyde oxidation reaction(FOR)on a Cu-based electrocatalyst enables hydrogen(H_(2))at the anode in OH−solution,facilitating a bipolar H_(2) production system at ultra-low electrolysis voltage.However,the spe...The formaldehyde oxidation reaction(FOR)on a Cu-based electrocatalyst enables hydrogen(H_(2))at the anode in OH−solution,facilitating a bipolar H_(2) production system at ultra-low electrolysis voltage.However,the specific impact of*OH adsorption on the Cu surface regarding the FOR has been rarely investigated.Herein,the strong*OH adsorption Cu(S-OH Cu)electrode,which exhibits high activity and excellent stability of FOR,is developed to investigate the specific impact of*OH adsorption on the Cu surface during the FOR process.Impressively,the increased*OH adsorption on the Cu electrode,typically regarded as a poisoning effect that diminishes inherent FOR activity by reducing the adsorption of intermediate reactants,is firstly revealed as an OH-induced favorable reconstruction effect that significantly improves FOR stability.Specifically,the dual functions of OH-induced favoring reconstruction include accelerating the phase transition of the Cu(0)/Cu(I)redox cycle to refresh the active site and optimizing surface reconstruction to preferentially generate Cu(220)with stronger adsorption energy for H_(2)C(OH)O*and lower C−H barrier energy during FOR.This work provides a promising strategy for designing stable Cu electrocatalysts for FOR to produce hydrogen with extremely low energy input.展开更多
基金the National Natural Science Foundation of China(No.22372104)the Shenzhen Science and Technology Program(Nos.ZDSYS20220527171401003 and KQTD20190929173914967)+1 种基金Guangdong College Students Science and Technology Innovation Cultivation Special Fund Project(No.pdjh2024a315)The authors also acknowledge the Instrumental Analysis Center of Shenzhen University(Xili Campus)for their assistance on TEM observation.
文摘The formaldehyde oxidation reaction(FOR)on a Cu-based electrocatalyst enables hydrogen(H_(2))at the anode in OH−solution,facilitating a bipolar H_(2) production system at ultra-low electrolysis voltage.However,the specific impact of*OH adsorption on the Cu surface regarding the FOR has been rarely investigated.Herein,the strong*OH adsorption Cu(S-OH Cu)electrode,which exhibits high activity and excellent stability of FOR,is developed to investigate the specific impact of*OH adsorption on the Cu surface during the FOR process.Impressively,the increased*OH adsorption on the Cu electrode,typically regarded as a poisoning effect that diminishes inherent FOR activity by reducing the adsorption of intermediate reactants,is firstly revealed as an OH-induced favorable reconstruction effect that significantly improves FOR stability.Specifically,the dual functions of OH-induced favoring reconstruction include accelerating the phase transition of the Cu(0)/Cu(I)redox cycle to refresh the active site and optimizing surface reconstruction to preferentially generate Cu(220)with stronger adsorption energy for H_(2)C(OH)O*and lower C−H barrier energy during FOR.This work provides a promising strategy for designing stable Cu electrocatalysts for FOR to produce hydrogen with extremely low energy input.
