Wang Ke, Cheng Ming, Xia Fanjie, Cao Ning, Zhang Fanxing, Ni Wenkang, Yue Xuanyu, Yan Keping, He Yi, Shi Yao, Dai Wenxin, Xie Pengfei
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China.
Small. 2023 Apr;19(14):e2207581. doi: 10.1002/smll.202207581. Epub 2023 Jan 17.
Overall photocatalytic conversion of CO and pure H O driven by solar irradiation into methanol provides a sustainable approach for extraterrestrial synthesis. However, few photocatalysts exhibit efficient production of CH OH. Here, BiOBr nanosheets supporting atomic Cu catalysts for CO reduction are reported. The investigation of charge dynamics demonstrates a strong built-in electric field established by isolated Cu sites as electron traps to facilitate charge transfer and stabilize charge carriers. As result, the catalysts exhibit a substantially high catalytic performance with methanol productivity of 627.66 µmol g h and selectivity of ≈90% with an apparent quantum efficiency of 12.23%. Mechanism studies reveal that the high selectivity of methanol can be ascribed to energy-favorable hydrogenation of *CO intermediate giving rise to *CHO. The unfavorable adsorption on Cu @BiOBr prevents methanol from being oxidized by photogenerated holes. This work highlights the great potential of single-atom photocatalysts in chemical transformation and energy storage reactions.
通过太阳辐射驱动将一氧化碳和纯水解离光催化转化为甲醇，为地外合成提供了一种可持续的方法。然而，很少有光催化剂能高效生产甲醇。在此，报道了负载原子铜催化剂用于一氧化碳还原的溴氧化铋纳米片。电荷动力学研究表明，孤立的铜位点作为电子陷阱建立了强大的内建电场，以促进电荷转移并稳定电荷载流子。结果，该催化剂表现出相当高的催化性能，甲醇生产率为627.66 μmol g⁻¹ h⁻¹，选择性约为90%，表观量子效率为12.23%。机理研究表明，甲醇的高选择性可归因于CO中间体的能量有利氢化生成CHO。在Cu@BiOBr上的不利吸附可防止甲醇被光生空穴氧化。这项工作突出了单原子光催化剂在化学转化和能量存储反应中的巨大潜力。
