Polyacrylate modified Cu electrode for selective electrochemical CO_(2) reduction towards multicarbon products  

聚丙烯酸酯修饰铜电极用于电化学二氧化碳还原选择性生成多碳产物

作　　者：Yuchuan Shi Kaini Zhang Chung-Li Dong Ta Thi Thuy Nga Miao Wang Daixing Wei Jialin Wang Yiqing Wang Shaohua Shen 石玉川;张凯妮;董崇礼;Ta Thi Thuy Nga;汪淼;魏代星;王佳琳;王亦清;沈少华

机构地区：[1]International Research Center for Renewable Energy,State Key Laboratory of Multiphase Flow in Power Engineering,Xi’an Jiaotong University,Xi’an 710049,China [2]Department of Physics,Tamkang University,New Taipei City 25137,China

出　　处：《Science Bulletin》2024年第15期2395-2404,共10页科学通报（英文版）

基　　金：supported by the National Natural Science Foundation of China(52225606,52488201);the Fundamental Research Funds for the Central Universities;The Youth Innovation Team of Shaanxi Universities。

摘　　要：Highly selective production of value-added multicarbon(C^(2+))products via electrochemical CO_(2) reduction reaction(eCO_(2)RR)on polycrystalline copper(Cu)remains challenging.Herein,the facile surface modification using poly(α-ethyl cyanoacrylate)(PECA)is presented to greatly enhance the C^(2+)selectivity for eCO_(2)RR over polycrystalline Cu,with Faradaic efficiency(FE)towards C^(2+)products increased from30.1%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 C^(2+)products,the partial current densities for C^(2+)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 featured 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(E_(d))of Cu active sites,thus facilitating the C-C coupling and then the C^(2+)selective production.This study is believed to be guidable to the modification of electrocatalysts and electrodes with polymers to steer the surface adsorption behaviors of reaction intermediates to realize practical eCO_(2)RR towards value-added C^(2+)products with high activity and selectivity.

关 键 词：Electrochemical CO_(2)reduction Polymer modification Electron transfer C_(2+)products 

分 类 号：O646[理学—物理化学] X701[理学—化学]