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

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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.

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Acknowledgements

The work was financially supported by the National Natural Science Foundation of China (Nos. 52072260, 21931007, 21790052, and U21A20317), the Science and Technology Support Program for Youth Innovation in Universities of Shangdong Province (No. 2020KJA012), the Tianjin Natural Science Foundation (Nos. 21JCZXJC00130 and B2021201074), the Haihe Laboratory of Sustainable Chemical Transformations, National Key R&D Program of China (No. 2017YFA0700104), and the University Synergy Innovation Program of Anhui Province (No. GXXT-2020-001). Supercomputing of Anhui University and National Supercomputing Center in Shanghai was acknowledged for computational support.

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

Authors and Affiliations

  1. 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

    Meijie Tan, Xiaoqian Han, Chao Zhang, Zhouru Ji, Zhaolin Shi, Guomeng Qiao, Yunying Wang, Ruixue Cui, Jiqing Jiao & Tongbu Lu

  2. Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601, China

    Sen Ru & Qiquan Luo

  3. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin, 300192, China

    Jiqing Jiao & Tongbu Lu

  4. College of Materials Science and Engineering, State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, Qingdao, 266071, China

    Jiqing Jiao

  5. 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

    Yaguang Li

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  1. Meijie Tan
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Correspondence to Qiquan Luo or Jiqing Jiao.

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

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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 Res. 16, 2059–2064 (2023). https://doi.org/10.1007/s12274-022-4878-3

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