Acidic electroreduction CO_(2)to formic acid via interfacial modification of Bi nanoparticles at industrial-level current  

作　　者：Tian Dong Hongdong Li Zhenhui Wang Yanling Geng Rui Chang Xiaofeng Tian Jianping Lai Shouhua Feng Lei Wang 

机构地区：[1]Key Laboratory of Eco-Chemical Engineering,International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,China [2]Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection,College of Environment and Safety Engineering,Qingdao University of Science and Technology,Qingdao 266042,China

出　　处：《Nano Research》2024年第7期5817-5825,共9页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.52072197,22302108,21971132,and 52272222);Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2023KJ313);Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14);Major Scientific and Technological Innovation Project(No.2019JZZY020405);Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09);Natural Science Foundation of Qingdao(No.23-2-1-12-zyyd-jch);Qingdao Postdoctoral Researcher Applied Research Project(No.QDBSH20220202043).

摘　　要：Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes.However,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current densities.Here,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles electrode.Using a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 h.Combined with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.

关 键 词：acidic media CO_(2)electrolysis electrolyte additive hydrophobic interfacial microenvironment industrial-level current 

分 类 号：O64[理学—物理化学]