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Research Article

PdAg bimetallic electrocatalyst for highly selective reduction of CO2 with low COOH* formation energy and facile CO desorption

Rui Lin1,§, Xuelu Ma2,§, Weng-Chon Cheong1, Chao Zhang1, Wei Zhu3, Jiajing Pei3, Kaiyue Zhang4, Bin Wang5, Shiyou Liang6, Yuxi Liu4, Zhongbin Zhuang3, Rong Yu6, Hai Xiao1( ), Jun Li1, Dingsheng Wang1, Qing Peng1, Chen Chen1( ), Yadong Li1
Department of ChemistryTsinghua UniversityBeijing100084China
School of Chemical & Environment EngineeringChina University of Mining & TechnologyBeijing100083China
College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing100029China
College of Environmental and Energy EngineeringBeijing University of TechnologyBeijing100124China
Sinopec Beijing Research Institute of Chemical IndustryBeijing100013China
School of Materials Science and EngineeringNational Center for Electron Microscopy in BeijingTsinghua UniversityBeijing100084China

§ Rui Lin and Xuelu Ma contributed equally to this work.

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Abstract

For electrocatalytic reduction of CO2 to CO, the stabilization of intermediate COOH* and the desorption of CO* are two key steps. Pd can easily stabilize COOH*, whereas the strong CO* binding to Pd surface results in severe poisoning, thus lowering catalytic activity and stability for CO2 reduction. On Ag surface, CO* desorbs readily, while COOH* requires a relatively high formation energy, leading to a high overpotential. In light of the above issues, we successfully designed the PdAg bimetallic catalyst to circumvent the drawbacks of sole Pd and Ag. The PdAg catalyst with Ag-terminated surface not only shows a much lower overpotential (-0.55 V with CO current density of 1 mA/cm2) than Ag (-0.76 V), but also delivers a CO/H2 ratio 18 times as high as that for Pd at the potential of -0.75 V vs. RHE. The issue of CO poisoning is significantly alleviated on Ag-terminated PdAg surface, with the stability well retained after 4 h electrolysis at -0.75 V vs. RHE. Density functional theory (DFT) calculations reveal that the Ag-terminated PdAg surface features a lowered formation energy for COOH* and weakened adsorption for CO*, which both contribute to the enhanced performance for CO2 reduction.

Keywords

CO2 reductionbimetalliclow overpotentialCO desorption

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Nano Research
Volume 12 Issue 11,
November 2019
Pages 2866-2871
DOI: 10.1007/s12274-019-2526-1
Cite this article:
Lin R, Ma X, Cheong W-C, et al. PdAg bimetallic electrocatalyst for highly selective reduction of CO2 with low COOH* formation energy and facile CO desorption. Nano Research, 2019, 12(11): 2866-2871. https://doi.org/10.1007/s12274-019-2526-1
Topics:
Binary alloysCarbon dioxideCatalyst activityDensity functional theoryElectrocatalystsSelective catalytic reductionSilver

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Received: 28 June 2019
Revised: 18 September 2019
Accepted: 27 September 2019
Published: 17 October 2019
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019
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