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Research Article

Unraveling the interfacial effect of PdBi bimetallic catalysts on promoting CO2 electroreduction to formate

Wenhui Liu1,§, Lingtong Ding2,3,§, Minmin Liu1(), Xiao Wang2,3(), Zhengrong Zhang1, Tian-Wen Jiang4, Shengjuan Huo1(), Wen-Bin Cai4
International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Institute for Sustainable Energy, College of Sciences, Shanghai University, Shanghai 200444, China
Shenzhen Key Laboratory of Nanobiomechanics, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
Paul C. Lauterbur Research Center for Biomedical Imaging, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Department of Chemistry, Fudan University, Shanghai 200438, China

§ Wenhui Liu and Lingtong Ding contributed equally to this work.

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Graphical Abstract

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In-situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations confirmed that bimetallic PdBi interface could regulate the intrinsic property of Pd catalyzing CO2 to CO at relatively negative potential by weakening the adsorption of *CO on the catalyst surface and lowering the energy barrier toward formate, resulting in high selectivity and stability for formate production, even in flow cells.

Abstract

Through interface engineering and content control strategy, a PdBi bimetallic interface structure was constructed for the first time to selectively convert CO2 to formate with a remarkably high Faraday efficiency (FEformate) of 94% and a partial current density (jformate) of 34 mA·cm−2 at −0.8 V vs. reversible hydrogen electrode (RHE) in an H-cell. Moreover, the PdBi interface electrocatalyst even exhibited a high current density of 180 mA·cm−2 with formate selectivity up to 92% in a flow cell and could steadily operate for at least 20 h. Electrochemical in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirmed that the PdBi interface could greatly weaken the adsorption of *CO intermediates due to electronic and geometric effects. Density functional theory (DFT) calculations also established that the PdBi interface regulated the CO2-to-formate pathway by reducing the energy barrier toward HCOOH and largely weakening the adsorption of *CO intermediates on the catalyst surface. This study reveals that the unique PdBi bimetallic interface can provide a novel platform to study the reaction mechanism through combining in-situ ATR-SEIRAS and DFT calculations.

Keywords

carbon dioxide reduction reactionbimetallic PdBiinterface engineeringformatein-situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS)

Electronic Supplementary Material

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Nano Research
Volume 16 Issue 8,
August 2023
Pages 10822-10831
DOI: 10.1007/s12274-023-5829-1
Cite this article:
Liu W, Ding L, Liu M, et al. Unraveling the interfacial effect of PdBi bimetallic catalysts on promoting CO2 electroreduction to formate. Nano Research, 2023, 16(8): 10822-10831. https://doi.org/10.1007/s12274-023-5829-1
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