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Research Article

Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO2 reduction

Wenxuan Zhang1Mengran Zhang1Hongjuan Wang1( )Wen Zhang2( )Min Zhang1,2
MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion, School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China
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Graphical Abstract

A novel bimetallic palladium complex (BPB-Pd2) with π-conjugated backbone was designed and synthesized. The calculations revealed that the outstanding activity of BPB-Pd2 toward CO2 reduction reaction (CO2RR) was the electronic effect between the two palladium sites which reduces the free energy change of CO2RR process.

Abstract

Double-site catalysts have attracted widespread attention in the field of electrocatalysis due to their high metal loading, adjustable active centres, and electronic valence states. However, the development of bimetallic sites catalysts that coordinate with definite atoms is still in the exploratory stage. Here, we designed and synthesized a bimetallic palladium complex (BPB-Pd2) with conjugated backbone. The supported BPB-Pd2 was applied to electrochemical CO2 reduction reaction (CO2RR) for the first time. The as-obtained BPB-Pd2 gives an exceptional Faradaic efficiency of CO (FECO) of 94.4% at −0.80 V vs. reversible hydrogen electrode (RHE), which is significantly superior to monoatomic palladium catalyst (BPB-Pd1). The density functional theory (DFT) calculations revealed that the essential reason for the outstanding activity of BPB-Pd2 toward CO2RR was that the electronic effect between diatomic palladium reduces the free energy change for CO2RR process. Thus, BPB-Pd2 exhibits moderate free energy change to form COOH* intermediate, which was beneficial for the generation of CO in CO2RR.

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Nano Research
Pages 4850-4855
Cite this article:
Zhang W, Zhang M, Wang H, et al. Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO2 reduction. Nano Research, 2024, 17(6): 4850-4855. https://doi.org/10.1007/s12274-024-6458-z
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Received: 24 November 2023
Revised: 21 December 2023
Accepted: 28 December 2023
Published: 08 February 2024
© Tsinghua University Press 2024
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