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- Title
Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production.
- Authors
Chen, Huai; Xiong, Yangyang; Li, Jun; Abed, Jehad; Wang, Da; Pedrazo-Tardajos, Adrián; Cao, Yueping; Zhang, Yiting; Wang, Ying; Shakouri, Mohsen; Xiao, Qunfeng; Hu, Yongfeng; Bals, Sara; Sargent, Edward H.; Su, Cheng-Yong; Yang, Zhenyu
- 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. Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas.
- Subjects
SYNTHESIS gas; TURNOVER frequency (Catalysis); QUANTUM efficiency; CATALYSTS; CRYSTAL structure; PHOTOCATALYSIS; EPITAXY
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-37401-3