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Benzophenone-Based Polymers and Covalent Organic Framework for Photocatalytic Molecular Oxygen Activation
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DOI：10.1021/acsami.5c03943.png)
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Abstract
En 中文
Photosensitization by photoactive materials requires well-designed molecular engineering to enable continuous photochemical processes. However, developing a heavy-atom-free (HAF) strategy to enhance the photoactivity of photosensitizers remains a significant challenge. In this study, we introduce a novel strategy to enhance photosensitization by incorporating benzophenone-rich components into 3D polymers (BQP1 and BQP2) and the 2D covalent organic framework (BQ-TMT COF). This incorporation accelerates both charge carrier separation and intersystem crossing, thereby significantly improving photo-to-chemical energy conversion and electron transfer reactions. Notably, the crystalline BQ-TMT COF enables efficient photocatalytic molecular O2 activation, producing both 1O2 and O2 - with high efficiency and recyclability. It demonstrates selective photocatalytic oxidation in 1O2-mediated sulfide transformations. Moreover, the material performs well in O2 --mediated oxidation, including the hydroxylation of boronic acids and oxidation of amines to imines. The BQ-TMT COF-based photoelectrode generates a photocurrent of approximately 20.7 mu Acm-2 at 0.4 V vs RHE and achieves a high photocatalytic hydrogen production rate. Our study demonstrates a HAF heterogeneous photosensitizer with efficient photoactive small molecule activation through molecular engineering.
Keywords:
covalent organic frameworks
benzophenone
photocatalysis
heavy-atom-free
small moleculeactivation
Journal
IF:
8.2
Papers:
6.1W
Citations:
38.7W