首页|A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO2 to C2+Products

A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO2 to C2+Products

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Driven by renewable or excess electrical energy,electrochemical CO2 reduction reaction(eCO2RR)represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO2 and H2O.C2+products are one of the most economically valuable products among the reduction species of eCO2RR,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 eCO2RR to yield C2+products with the Faradaic efficiency(C2+)of 52.5％and a current density of 660 mA/cm2 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 C2+products.

Metal-organic frameworkCarbon dioxide ElectroreductionC2+productMetal-azolate framework

LIU Yuan-Yuan、ZHU Hao-Lin、LIAO Pei-Qin、CHEN Xiao-Ming

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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

Chemistry and Chemical Engineering Guangdong Laboratory,Shantou 515031,P.R.China

National Key Research and Development Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaSpecial Fund Project for Science and Technology Innovation Strategy of Guangdong Province,ChinaGuangzhou Science and Technology Program,China

2021YFA1500401218903802182100322371304223B2123STKJ2023078SL2023A04J01767

2024

10.1007/s40242-024-4113-6

高等学校化学研究(英文版)
吉林大学

高等学校化学研究(英文版)

CSTPCD
影响因子：0.871
ISSN：1005-9040
年,卷(期)：2024.40(4)