化学
光催化
还原(数学)
电子
金属
金属有机骨架
光化学
无机化学
物理化学
有机化学
催化作用
物理
几何学
数学
吸附
量子力学
作者
Zhaohui Zhang,Qiang Xü,Weiran Li,Yunhai Zhu,Jun‐Sheng Qin,Yingkui Yang,Heng Rao,Long Chen
摘要
Metal-organic frameworks (MOFs) are distinguished by their structural diversity, tunable electronic properties, and exceptional performance in various applications. Notably, the electron-donating ability of ligands significantly enhances the ligand-to-metal charge transfer (LMCT) processes within these frameworks, thereby promoting efficient charge migration. Herein, we developed two electron-rich macrocyclic ligands derived from phenothiazine- and phenoxazine-functionalized calix[3]arenes, alongside their corresponding cobalt-coordinated MOFs. Remarkably, the MOF designated as Co-C[3]PTZ-MOF─constructed using the more electron-donating calix[3]phenothiazine ligand (C[3]PTZ-COOH)─exhibited superior photoresponse and enhanced charge-transport characteristics. This optimized material achieved an exceptional CO2 photoreduction initial efficiency of 17,800 μmol g-1 h-1 with 81% CO selectivity. The outstanding photocatalytic performance originates from the strong electron-donating nature of the calix[3]arene-based ligands, which facilitated efficient LMCT processes. This study provides valuable insights for designing high-performance photocatalysts through rational engineering of macrocyclic ligands.
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