Preferential Formation of Ethylene via Electrocatalytic CO_(2) Reduction on Mesoporous Cu_(2)O Nanoparticles:Synergistic Effects of Pore Structure Confinement and Surface Amine  

作　　者：Haifeng Zhang Dun Li Zhifang Chen Yingying Wang Haoyu Sun Feng Liu Maochang Liu Yiqun Zheng Hongwen Huang 

机构地区：[1]School of Chemistry,Chemical Engineering and Materials,Jining University,Qufu,Shandong 273155,China [2]College of Materials Science and Engineering,Hunan University,Changsha,Hunan 410082,China [3]Health Management Department,Shandong Vocational College of Light Industry,Zibo,Shandong 255300,China [4]International Research Center for Renewable Energy National Key Laboratory of Multiphase Flow in Power Engineering,Xi'an Jiotong University,Xi'an,Shaanxi 710049,China

出　　处：《Chinese Journal of Chemistry》2024年第16期1846-1852,共7页中国化学（英文版）

基　　金：financially supported by Shandong Provincial Natural Science Foundation(No.ZR2022MB120&ZR2020MB048);the University Feature Laboratory for Energy Conversion and Nanocatalysis of Shandong Province;Hundred Outstanding Talent Program of Jining University(No.2020ZYRC05).

摘　　要：We present a facile synthetic strategy to create mesoporous Cu_(2)O nanocrystals with tunable pore structures and surface functional groups of amine derivatives for efficient and preferable electrochemical conversion of CO_(2) into ethylene.The structural characteristics of theseCu_(2)O nanocrystals can be manipulated using a set of amine derivatives,such as pyridine,4,4'-bipyridine,and hexamethylenetetramine,during the oxidative etching process of Cu nanocrystals by bubbling gaseous oxygen in N,N-dimethylformamide solution.These amine derivatives not only serve as surface functional groups but also significantly affect the resulting pore structures.The synergistic effect of pore structure confinement and surface amine functionalization leads to the superb Faradaic efficiency(FE)of 51.9% for C_(2)H_(4),respectively,together with the C_(2)H_(4) partial current density of -209.4 mA·cm^(-2) at -0.8 V vs.reversible hydrogen electrode(RHE).The relatively high selectivity towards C_(2)H_(4) was investigated using DFT simulations,where 4,4'-bipyridine functionalized Cu_(2)O seemed to favor the C_(2)H_(4) formation with the low free energy of the intermediates.This study provides a feasible strategy to manipulate the pore structure and surface functionalization of mesoporous Cu_(2)O nanocrystals by regulating the oxidative etching process,which sheds light on the rational preparation of high-performance CO_(2)RR electrocatalysts.

关 键 词：AMINES ETHYLENE Cuprous oxide CO_(2)reduction Mesoporous materials 

分 类 号：O643.3[理学—物理化学]