Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO2 to C2:Synergistic catalysis or tandem catalysis?

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外文摘要：The activity and selectivity of electrocatalytic CO2 reduction reaction(CO2RR)to C2 products on metal catalysts can be regulated by molecular surfactants.However,the mechanism behind it remains elusive and debatable.Herein,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalo-cyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO2 and CO2RR intermediates were explored by density functional theory(DFT)calculations.It was found that the selectivity and activity of CO2RR towards C2 products on Cu NWs were considerably enhanced from 35.2％to 69.9％by surface dec-oration of CoPc.DFT calculations revealed that CO2RR can proceed in the interphase between Cu substrate and CoPc,and the CO2RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO2,CO and CO2RR intermediates,thus reducing the free energy for CO-CO coupling towards C2 products.The synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker syner-gistic interaction of CO intermediates with MPc and Cu substrate and only a slight enhancement of CO2RR towards C2 products were observed.This study demonstrates a synergistic catalysis pathway for CO2RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO2RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.

外文关键词：

CO2 reduction reactionRaman spectroscopySynergistic catalysisDFT calculation

作者：

Yan Luo、Jun Yang、Jundi Qin、Kanghua Miao、Dong Xiang、Aidar Kuchkaev、Dmitry Yakhvarov、Chuansheng Hu、Xiongwu Kang

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作者单位：

New Energy Research Institute,School of Environment and Energy,South China University of Technology,Higher Education Mega Center,Guangzhou 510006,Guangdong,China

Guangdong University of Petrochemical Technology,School of Chemical Engineering,Maoming 525000,Guangdong,China

Arbuzov Institute of Organic and Physical Chemistry,FRC Kazan Scientific Center of RAS,Arbuzov Street 8,Kazan 420088,Russian Federation

National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,Anhui,China

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基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of China

项目编号：

U203215122272059

出版年：

2024

DOI：

10.1016/j.jechem.2024.01.008

能源化学

中国科学院大连化学物理研究所中国科学院成都有机化学研究所

能源化学

CSTPCDEI

影响因子：0.654

ISSN：2095-4956

年,卷(期)：2024.92(5)