A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO_(2)to C_(2+)Products  

作　　者：LIU Yuan-Yuan ZHU Hao-Lin LIAO Pei-Qin CHEN Xiao-Ming 

机构地区：[1]Key Laboratory of Bioinorganic and Synthetic Chemistry,Ministry of Education,GBRCE for Functional Molecular Engineering,School of Chemistry,IGCME,Sun Yat-sen University,Guangzhou,510275,P.R.China [2]Chemistry and Chemical Engineering Guangdong Laboratory,Shantou,515031,P.R.China

出　　处：《Chemical Research in Chinese Universities》2024年第4期664-669,共6页高等学校化学研究（英文版）

基　　金：supported by the National Key Research and Development Program of China(No.2021YFA1500401);the National Natural Science Foundation of China(Nos.21890380,21821003,22371304,223B2123);the Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province,China(No.STKJ2023078);the Guangzhou Science and Technology Program,China(No.SL2023A04J01767).

摘　　要：Driven by renewable or excess electrical energy,electrochemical CO_(2)reduction reaction(eCO_(2)RR)represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO_(2)and H_(2)O.C_(2+)products are one of the most economically valuable products among the reduction species of eCO_(2)RR,but there are still some challenges,such as low selectivity or low current density.In this work,we showed that a copper-based metal-azolate framework(MAF),denoted as MAF-203,exhibits the high performance of eCO_(2)RR to yield C_(2+)products with the Faradaic efficiency(C_(2+))of 52.5%and a current density of 660 mA/cm^(2)at-1.2 V vs.RHE in a flow cell device under alkaline condition.Controlled experiment,in situ infrared spectroscopy and the density functional theory(DFT)calculations showed that the electron donating effect of methyl substituents on organic ligands of the copper-based MAF could enhance the ligand field and activation of key intermediates(*CO and*CHO species),thus promoting the coupling of*CO and*CHO for yielding C_(2+)products.

关 键 词：Metal-organic framework Carbon dioxide ELECTROREDUCTION C_(2+)product Metal-azolate framework 

分 类 号：O62[理学—有机化学]