掺杂剂
等结构
光催化
可见光谱
带隙
金属有机骨架
兴奋剂
杂原子
材料科学
配体(生物化学)
连接器
光化学
溶剂热合成
催化作用
分解水
化学
组合化学
无机化学
晶体结构
有机化学
光电子学
受体
吸附
操作系统
生物化学
计算机科学
戒指(化学)
作者
Xiaoxuan Su,Tongfei Xu,Rongbin Ye,Changfa Guo,Saikh Mohammad Wabaidur,De–Li Chen,Sikandar Aftab,Yijun Zhong,Yong Hu
标识
DOI:10.1016/j.jcis.2023.05.041
摘要
Metal organic frameworks (MOFs) with high porosity and highly tunable physical/chemical properties can serve as heterogeneous catalysts for CO2 photoreduction, but the application is hindered by the large band gap (Eg) and insufficient ligand-to-metal charge transfer (LMCT). In this study, a simple one-pot solvothermal strategy is proposed to prepare an amino-functionalized MOF (aU(Zr/In)) featuring an amino-functionalizing ligand linker and In-doped Zr-oxo clusters, which enables efficient CO2 reduction driven with visible light. The amino functionalization leads to a significant reduction of Eg as well as a charge redistribution of the framework, allowing the absorption of visible light and the efficient separation of photogenerated carriers. Furthermore, the incorporation of In not only promotes the LMCT process by creating oxygen vacancies in Zr-oxo clusters, but also greatly lowers the energy barrier of the intermediates for CO2-to-CO conversion. With the synergistic effects of the amino groups and the In dopants, the optimized aU(Zr/In) exhibits a CO production rate of 37.58 ± 1.06 μmol g-1 h−1, outperforming the isostructural University of Oslo-66- and Material of Institute Lavoisier-125-based photocatalysts. Our work demonstrates the potential of modifying MOFs with ligands and heteroatom dopants in metal-oxo clusters for solar energy conversion.
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