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The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations

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Abstract

Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H–N···Ce and the C–S···Ce interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O2 activation and reduction occur at coordinatively unsaturated Ce3+ sites to form ·O2–. This is accelerated by the Ce3+/Ce4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level.

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摘要

MOFs的缺陷工程在光催化领域引起了广泛的关注。该工作制备了一系列不同含量的配体缺陷的UiO-66(Ce) MOFs，用于在可见光下光催化选择性氧化苄胺(BA)和茴香硫醚(TA)。配体缺陷的引入促进了高Ce3+含量的不饱和Ce位点的形成，并且产生更多的氧空位。原位FTIR结果表明，BA和TA分子分别通过H-N···Ce和C-S···Ce相互作用在配位不饱和Ce位点上被吸附活化。模拟原位EPR数据表明，O2的活化和还原发生在配位不饱和Ce3+位点，形成·O2-自由基。通过光生电子协同的Ce3+/Ce4+氧化还原循环进一步促进其形成。光生空穴参与了活化的BA和TA的去质子化过程。最佳的催化剂展现了98.4%的BA转化率和95.5%的TA转化率。最后，在分子水平上提出了分子活化的机制。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 22272026 and 22272028) and the 111 Project (No. D16008). Jinhong Bi thanks the Youth Talent Support Program of Fujian Province (No. 00387077).

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  1. State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou, 350116, China

    Cheng Liu, Ying-Zhang Shi, Qi Chen, Bing-Hua Ye, Jin-Hong Bi, Jimmy C. Yu & Ling Wu

  2. Department of Environmental Science and Engineering, Fuzhou University, Fuzhou, 350108, China

    Jin-Hong Bi

  3. Department of Chemistry, The Chinese University of Hong Kong, Hong Kong, 999077, China

    Jimmy C. Yu

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Liu, C., Shi, YZ., Chen, Q. et al. The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02693-x

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