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Atomic-level regulation of POMOF homologous isomer for photocatalytic C-H bond oxidation
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DOI:10.1016/j.cclet.2026.113018.png)
Abstract
En 中文
How to break through the oxidation energy barrier of C(sp3)-H bonds with high dissociation energy and prevent excessive oxidation is a significant challenge. This study presents the atomic-level regulation of POMOF dimensions by inducing structural differentiation through hydroxide end-capping. Two homologous isomers, named as Co-W10 and OH-Co-W10 respectively, have formed three-dimensional (3D) and two-dimensional (2D) structures through varied metal coordination modes. The 2D structure of OH-Co-W10 demonstrates excellent electron delocalization and transfer channels over the 3D structure of Co-W10. OH-Co-W10 exhibits enhanced oxygen activation capacity compared to Co-W10. In the catalytic oxidation of toluene, OH-Co-W10 achieves an impressive conversion rate of 98.1 %, and the selectivity of benzaldehyde is as high as 97.3 % (6720.2 µmol/g), which is cleaner and more efficient than that of the latest photocatalysts and Co-W10 (4713.1 µmol/g). In this study, the hydroxide capping strategy is proposed for generation of homologous isomers, offering a new direction for catalytic oxidation of C(sp3)-H bonds by expounding differences in active sites through distinct structural features.
Journal
IF:
8.9
Papers:
1.2W
Citations:
3.8W
