Abstract
Highly selective production of value-added multicarbon(C2+)products via electrochemical CO2 reduction reaction(eCO2RR)on polycrystalline copper(Cu)remains challenging.Herein,the facile surface modifi-cation using poly(α-ethyl cyanoacrylate)(PECA)is presented to greatly enhance the C2+selectivity for eCO2RR over polycrystalline Cu,with Faradaic efficiency(FE)towards C2+products increased from 30.1％for the Cu electrode to 72.6％for the obtained Cu-PECA electrode at-1.1 V vs.reversible hydrogen electrode(RHE).Given the well-determined FEs towards C2+products,the partial current densities for C2+production could be estimated to be-145.4 mA cm-2 for the Cu-PECA electrode at-0.9 V vs.RHE in a homemade flow cell.In-situ spectral characterizations and theoretical calculations reveal that PECA fea-tured with electron-accepting-C≡N and-COOR groups decorated onto the Cu electrode could inhibit the adsorption of*H intermediates and stabilize the*CO intermediates,given the redistributed interfacial electron density and the raised energy level of d-band center(Ed)of Cu active sites,thus facilitating the C-C coupling and then the C2+selective production.This study is believed to be guidable to the modifi-cation of electrocatalysts and electrodes with polymers to steer the surface adsorption behaviors of reac-tion intermediates to realize practical eCO2RR towards value-added C2+products with high activity and selectivity.
基金项目
National Natural Science Foundation of China(52225606)
National Natural Science Foundation of China(52488201)
Fundamental Research Funds for the Central Universities()
Youth Innovation Team of Shaanxi Universities()
NETL
NSTL
万方数据