Tuning the Microenvironment in Monolayer MgAl Layered Double Hydroxide for CO2 -to-Ethylene Electrocatalysis in Neutral Media

Yi Ning Xu; Wenjing Li; Huai Qin Fu; Xin Yu Zhang; Jia Yue Zhao; Xuefeng Wu; Hai Yang Yuan; Minghui Zhu; Sheng Dai; Peng Fei Liu; Hua Gui Yang

doi:10.1002/anie.202217296

Tuning the Microenvironment in Monolayer MgAl Layered Double Hydroxide for CO₂ -to-Ethylene Electrocatalysis in Neutral Media

Angew Chem Int Ed Engl. 2023 May 2;62(19):e202217296. doi: 10.1002/anie.202217296. Epub 2023 Apr 4.

Authors

Affiliations

¹ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
² Centre for Catalysis and Clean Energy, Gold Coast Campus, Griffith University, Gold Coast, QLD 4222, Australia.
³ State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
⁴ China Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

PMID: 36912381
DOI: 10.1002/anie.202217296

Abstract

The electrocatalytic reduction of carbon dioxide provides a feasibility to achieve a carbon-neutral energy cycle. However, there are a number of bottleneck issues to be resolved before industrial application, such as the low conversion efficiency, selectivity and reaction rate, etc. Engineering local environment is a critical way to address these challenges. Here, a monolayer MgAl-LDH was proposed to optimize the local environment of Cu for stimulating industrial-current-density CO₂ -to-C₂ H₄ electroreduction in neutral media. In situ spectroscopic results and theoretical study demonstrated that the Cu electrode modified by MgAl-LDH (MgAl-LDH/Cu) displayed a much higher surface pH value compared to the bare Cu, which could be attributed to the decreased energy barrier for hydrolysis on MgAl-LDH sites with more OH^- ions on the surface of the electrode. As a result, MgAl-LDH/Cu achieved a C₂ H₄ Faradaic efficiency of 55.1 % at a current density up to 300 mA cm^-2 in 1.0 M KHCO₃ electrolyte.

Keywords: CO2 Electrocatalysis; Ethylene Selectivity; MgAl-LDH; Microenvironment; Water Dissociation.

Abstract

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