Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production

Huai Chen, Yangyang Xiong, Jun Li, Jehad Abed, Da Wang, Adrián Pedrazo-Tardajos, Yueping Cao, Yiting Zhang, Ying Wang, Mohsen Shakouri, Qunfeng Xiao, Yongfeng Hu, Sara Bals, Edward H. Sargent, Cheng-Yong Su () and Zhenyu Yang ()
Additional contact information
Huai Chen: Sun Yat-sen University
Yangyang Xiong: Sun Yat-sen University
Jun Li: University of Toronto
Jehad Abed: University of Toronto
Da Wang: University of Antwerp
Adrián Pedrazo-Tardajos: University of Antwerp
Yueping Cao: Sun Yat-sen University
Yiting Zhang: Sun Yat-sen University
Ying Wang: Chinese University of Hong Kong
Mohsen Shakouri: Canadian Light Source, Inc. (CLSI)
Qunfeng Xiao: Canadian Light Source, Inc. (CLSI)
Yongfeng Hu: Canadian Light Source, Inc. (CLSI)
Sara Bals: University of Antwerp
Edward H. Sargent: University of Toronto
Cheng-Yong Su: Sun Yat-sen University
Zhenyu Yang: Sun Yat-sen University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon’s rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H2 yields of 4.7 mol g(Co)−1 and 4.4 mol g(Co)−1, respectively. Moreover, the H2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 × 104 for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.

Date: 2023
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DOI: 10.1038/s41467-023-37401-3

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