文献类型：期刊文献

英文题名：Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field

作者：Guo, Weihua[1,2];Zhang, Siwei[3,4];Zhang, Junjie[5];Wu, Haoran[6];Ma, Yangbo[1];Song, Yun[1];Cheng, Le[1];Chang, Liang[7];Li, Geng[1];Liu, Yong[1];Wei, Guodan[7];Gan, Lin[7];Zhu, Minghui[6];Xi, Shibo[8];Wang, Xue[9];Yakobson, Boris I.[5];Tang, Ben Zhong[3,4,10];Ye, Ruquan[1,2]

机构：[1]City Univ Hong Kong, Dept Chem, State Key Lab Marine Pollut, Hong Kong 999077, Peoples R China;[2]City Univ Hong Kong, Shenzhen Res Inst, Shenzhen 518057, Guangdong, Peoples R China;[3]Hong Kong Univ Sci & Technol, Dept Chem, Hong Kong 999077, Peoples R China;[4]Hong Kong Univ Sci & Technol, Chinese Natl EngineeringResearch Ctr Tissue Restor, Hong Kong Branch, Hong Kong 999077, Peoples R China;[5]Rice Univ, Dept Mat Sci & Nano Engn, 6100 Main St, Houston, TX 77005 USA;[6]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[7]Tsinghua Univ, Inst Mat Res, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Guangdong, Peoples R China;[8]ASTAR, Inst Chem & Engn Sci, Singapore 627833, Singapore;[9]City Univ Hong Kong, Sch Energy & Environm, Hong Kong 999077, Peoples R China;[10]Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen 518172, Guangdong, Peoples R China

年份：2023

卷号：14

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001126873300004)】；

基金：R.Y. acknowledges support from Guangdong Basic and Applied Basic Research Fund (2022A1515011333), Hong Kong Research Grant Council (11309723), the Shenzhen Science and Technology Program (JCYJ20220818101204009) and State Key Laboratory of Marine Pollution (SKLMP/IRF/0029). B.Z.T. acknowledges support from Shenzhen Key Laboratory of Functional Aggregate Materials (ZDSYS20211021111400001), the Science Technology Innovation Commission of Shenzhen Municipality (KQTD20210811090142053, JCYJ20220818103007014).

语种：英文

摘要：Regulating electron transport rate and ion concentrations in the local microenvironment of active site can overcome the slow kinetics and unfavorable thermodynamics of CO2 electroreduction. However, simultaneous optimization of both kinetics and thermodynamics is hindered by synthetic constraints and poor mechanistic understanding. Here we leverage laser-assisted manufacturing for synthesizing CuxO bipyramids with controlled tip angles and abundant nanograins, and elucidate the mechanism of the relationship between electron transport/ion concentrations and electrocatalytic performance. Potassium/OH- adsorption tests and finite element simulations corroborate the contributions from strong electric field at the sharp tip. In situ Fourier transform infrared spectrometry and differential electrochemical mass spectrometry unveil the dynamic evolution of critical *CO/*OCCOH intermediates and product profiles, complemented with theoretical calculations that elucidate the thermodynamic contributions from improved coupling at the Cu+/Cu2+ interfaces. Through modulating the electron transport and ion concentrations, we achieve high Faradaic efficiency of 81% at similar to 900 mA cm(-2) for C2+ products via CO2RR. Similar enhancement is also observed for nitrate reduction reaction (NITRR), achieving 81.83 mg h(-1) ammonia yield rate per milligram catalyst. Coupling the CO2RR and NITRR systems demonstrates the potential for valorizing flue gases and nitrate wastes, which suggests a practical approach for carbon-nitrogen cycling.