硅
外延
材料科学
光催化
合成气
催化作用
Atom(片上系统)
晶体硅
色散(光学)
纳米技术
化学工程
光化学
光电子学
化学
光学
物理
有机化学
图层(电子)
计算机科学
嵌入式系统
工程类
作者
Huai Chen,Yi Xiong,Jun Li,Jehad Abed,Da Wang,Adrián Pedrazo‐Tardajos,Yanhui Cao,Yiting Zhang,Ying Wang,Mohsen Shakouri,Qunfeng Xiao,Yongfeng Hu,Sara Bals,Edward H. Sargent,Cheng‐Yong Su,Zhenyu Yang
标识
DOI:10.1038/s41467-023-37401-3
摘要
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.
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