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A Supported Bismuth Halide Perovskite Photocatalyst for Selective Aliphatic and Aromatic C–H Bond Activation

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Dai,  Yitao
Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Poidevin,  Corentin
Research Group Auer, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Ochoa-Hernández,  Cristina
Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Auer,  Alexander A.
Research Group Auer, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Tüysüz,  Harun
Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Citation

Dai, Y., Poidevin, C., Ochoa-Hernández, C., Auer, A. A., & Tüysüz, H. (2020). A Supported Bismuth Halide Perovskite Photocatalyst for Selective Aliphatic and Aromatic C–H Bond Activation. Angewandte Chemie, International Edition, 59(14), 5788-5796. doi:10.1002/anie.201915034.


Cite as: https://hdl.handle.net/21.11116/0000-0005-EEE3-F
Abstract
Direct selective oxidation of hydrocarbons to oxygenates by O2 is challenging. Catalysts are limited by the low activity and narrow application scope, and the main focus is on active C−H bonds at benzylic positions. In this work, stable, lead‐free, Cs3Bi2Br9 halide perovskites are integrated within the pore channels of mesoporous SBA‐15 silica and demonstrate their photocatalytic potentials for C−H bond activation. The composite photocatalysts can effectively oxidize hydrocarbons (C5 to C16 including aromatic and aliphatic alkanes) with a conversion rate up to 32900 μmol gcat−1 h−1 and excellent selectivity (>99 %) towards aldehydes and ketones under visible‐light irradiation. Isotopic labeling, in situ spectroscopic studies, and DFT calculations reveal that well‐dispersed small perovskite nanoparticles (2–5 nm) possess enhanced electron–hole separation and a close contact with hydrocarbons that facilitates C(sp3)−H bond activation by photoinduced charges.