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

LIU Yuan-Yuan ¹ZHU Hao-Lin ¹LIAO Pei-Qin ¹CHEN Xiao-Ming²

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作者信息

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. 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
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Abstract

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.

Key words

Metal-organic framework/Carbon dioxide Electroreduction/C2+product/Metal-azolate framework

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基金项目

National Key Research and Development Program of China(2021YFA1500401)

National Natural Science Foundation of China(21890380)

National Natural Science Foundation of China(21821003)

National Natural Science Foundation of China(22371304)

National Natural Science Foundation of China(223B2123)

Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province,China(STKJ2023078)

Guangzhou Science and Technology Program,China(SL2023A04J01767)

出版年

2024

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

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