Li Han, Song Qinjun, Wan Sijie, Tung Ching-Wei, Liu Chengyuan, Pan Yang, Luo GuoQiang, Chen Hao Ming, Cao Shaowen, Yu Jiaguo, Zhang LianMeng
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, P. R. China.
Department of Materials Engineering, Ming Chi University of Technology, New Taipei City, 24301, Taiwan.
Small. 2023 Aug;19(34):e2301711. doi: 10.1002/smll.202301711. Epub 2023 Apr 24.
Solar-driven CO conversion into valuable fuels is a promising strategy to alleviate the energy and environmental issues. However, inefficient charge separation and transfer greatly limits the photocatalytic CO reduction efficiency. Herein, single-atom Pt anchored on 3D hierarchical TiO -Ti C with atomic-scale interface engineering is successfully synthesized through an in situ transformation and photoreduction method. The in situ growth of TiO on Ti C nanosheets can not only provide interfacial driving force for the charge transport, but also create an atomic-level charge transfer channel for directional electron migration. Moreover, the single-atom Pt anchored on TiO or Ti C can effectively capture the photogenerated electrons through the atomic interfacial PtO bond with shortened charge migration distance, and simultaneously serve as active sites for CO adsorption and activation. Benefiting from the synergistic effect of the atomic interface engineering of single-atom Pt and interfacial TiOTi, the optimized photocatalyst exhibits excellent CO -to-CO conversion activity of 20.5 µmol g h with a selectivity of 96%, which is five times that of commercial TiO (P25). This work sheds new light on designing ideal atomic-scale interface and single-atom catalysts for efficient solar fuel conversation.
太阳能驱动的一氧化碳转化为有价值的燃料是缓解能源和环境问题的一种有前景的策略。然而,低效的电荷分离和转移极大地限制了光催化一氧化碳还原效率。在此,通过原位转化和光还原方法成功合成了锚定在具有原子尺度界面工程的三维分级TiO -Ti C上的单原子铂。TiO在Ti C纳米片上的原位生长不仅可以为电荷传输提供界面驱动力,还可以为定向电子迁移创建原子级电荷转移通道。此外,锚定在TiO或Ti C上的单原子铂可以通过缩短电荷迁移距离的原子界面PtO键有效地捕获光生电子,同时作为一氧化碳吸附和活化的活性位点。受益于单原子铂的原子界面工程与界面TiOTi的协同效应,优化后的光催化剂表现出优异的一氧化碳到一氧化碳转化活性,为20.5 µmol g h,选择性为96%,是商用TiO(P25)的五倍。这项工作为设计用于高效太阳能燃料转化的理想原子尺度界面和单原子催化剂提供了新的思路。