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Research Article

Low-loading gold in situ doped with sulfur by biomolecule-assisted approach for promoted electrochemical carbon dioxide reduction

Meijie Tan1,§, Xiaoqian Han1,§, Sen Ru2, Chao Zhang1, Zhouru Ji1, Zhaolin Shi1, Guomeng Qiao1, Yunying Wang1, Ruixue Cui1, Qiquan Luo2( ), Jiqing Jiao1,3,4( ), Yaguang Li5, Tongbu Lu1,3
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
Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, China
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
College of Materials Science and Engineering, State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, Qingdao 266071, China
Hebei Key Lab of Optic-electronic Information and Materials, College of Physics Science and Technology, Institute of Life Science and Green Development, Hebei University, Baoding 071002, China

§ Meijie Tan and Xiaoqian Han contributed equally to this work.

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Graphical Abstract

The in situ S-doped Au/NC nanocomposites display high activity and selectivity for CO in CO2 reduction reaction (CO2RR) with a Au loading as low as 0.4 wt.%.

Abstract

For electrochemical carbon dioxide reduction (CO2RR), CO2-to-CO conversion is considered an ideal route towards carbon neutrality for practical applications. Gold (Au) is known as a promising catalyst with high selectivity for CO; however, it suffers from high cost and low mass-specific activity. In this study, we design and prepare a catalyst featuring uniform S-doped Au nanoparticles on N-doped carbon support (denoted as S-Au/NC) by an in situ synthesis strategy using biomolecules. The S-Au/NC displays high activity and selectivity for CO in CO2RR with a Au loading as low as 0.4 wt.%. The Faradaic efficiency of CO (FECO) for S-Au/NC is above 95% at −0.75 V (vs. RHE); by contrast, the FECO of Au/NC (without S) is only 58%. The Tafel slope is 77.4 mV·dec−1, revealing a favorable kinetics process. Furthermore, S-Au/NC exhibits an excellent long-term stability for CO2RR. Density functional theory (DFT) calculations reveal that the S dopant can boost the activity by reducing the free energy change of the potential-limiting step (formation of the *COOH intermediate). This work not only demonstrates a model catalyst featuring significantly reduced use of noble metals, but also establishes an in situ synthesis strategy for preparing high-performance catalysts.

Keywords

electrochemical CO2 reductionnanocompositesheterogeneous catalystin situ sulfuredheteroatoms

Electronic Supplementary Material

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Nano Research
Volume 16 Issue 2,
February 2023
Pages 2059-2064
DOI: 10.1007/s12274-022-4878-3
Cite this article:
Tan M, Han X, Ru S, et al. Low-loading gold in situ doped with sulfur by biomolecule-assisted approach for promoted electrochemical carbon dioxide reduction. Nano Research, 2023, 16(2): 2059-2064. https://doi.org/10.1007/s12274-022-4878-3
Topics:
Cost effectivenessElectrocatalysis

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Received: 01 July 2022
Revised: 05 August 2022
Accepted: 07 August 2022
Published: 18 October 2022
© Tsinghua University Press 2022
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