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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.
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.