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C(sp3)–H Bond Activation by Perovskite Solar Photocatalyst Cell AITranslate

Haowei Huang; Haifeng Yuan; Jiwu Zhao; Guillermo SolísFernández; Chen Zhou; Jin Won Seo; Jelle Hendrix; Elke Debroye; Julian A. Steele; Johan Hofkens; Jinlin Long; Maarten B. J. Roeffaers;
Department of Microbial and Molecular Systems, Centre for Surface Chemistry and Catalysis (COK);Department of Chemistry, Faculty of Sciences; Fuzhou University;Department of Chemistry, Faculty of Sciences;Department of Materials Engineering, KU Leuven;Department of Materials Engineering, KU Leuven;Department of Chemistry, Faculty of Sciences;Department of Chemistry, Faculty of Sciences;Department of Microbial and Molecular Systems, Centre for Surface Chemistry and Catalysis (COK);Department of Chemistry, Faculty of Sciences; Fuzhou University;Department of Microbial and Molecular Systems, Centre for Surface Chemistry and Catalysis (COK)
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Abstract AITranslate

Inspired by efficient perovskite solar cells, we developed a three-component hybrid perovskite-based solar photocatalyst cell, NiOx/FAPbBr3/TiO2, for C(sp3)–H bond activation with high selectivity (∼90%) and high conversion rates (3800 μmol g–1 h–1) under ambient conditions. Time-resolved spectroscopy on our photocatalytic cell reveals efficient exciton dissociation and charge separation, where TiO2 and NiOx serve as the electron- and hole-transporting layers, respectively. The photogenerated charge carriers injected into TiO2 and NiOx drive the challenging C–H activation reaction via the synergetic effects of their band alignment relative to FAPbBr3. The reaction pathway is investigated by controlling the free-radical formation, and we find that C–H activation is mainly triggered by hole oxidation. Besides aromatic alkanes, also the C(sp3)–H bond in cycloalkanes can be oxidized selectively. This work demonstrates a generic strategy for engineering high-performance photocatalysts based on the perovskite solar cell concept.

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DOI：https://doi.org/10.1021/acsenergylett.8b01698

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Citation Information:

Inspired by efficient perovskite solar cells, we developed a three-component hybrid perovskite-based solar photocatalyst cell, NiOx/FAPbBr3/TiO2, for C(sp3)–H bond activation with high selectivity (∼90%) and high conversion rates (3800 μmol g–1 h–1) under ambient conditions. Time-resolved spectroscopy on our photocatalytic cell reveals efficient exciton dissociation and charge separation, where TiO2 and NiOx serve as the electron- and hole-transporting layers, respectively. The photogenerated charge carriers injected into TiO2 and NiOx drive the challenging C–H activation reaction via the synergetic effects of their band alignment relative to FAPbBr3. The reaction pathway is investigated by controlling the free-radical formation, and we find that C–H activation is mainly triggered by hole oxidation. Besides aromatic alkanes, also the C(sp3)–H bond in cycloalkanes can be oxidized selectively. This work demonstrates a generic strategy for engineering high-performance photocatalysts based on the perovskite solar cell concept.

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GB/T 7714-2015 [1] Haowei Huang, Haifeng Yuan, Jiwu Zhao, et al. ACS Energy Letters, 2019(4). DOI:10.1021/acsenergylett.8b01698.
MLA [1] Haowei Huang, et al., ACS Energy Letters, no. 4, 2019, https://doi.org/10.1021/acsenergylett.8b01698.
APA [1] Haowei Huang, Haifeng Yuan, Jiwu Zhao, Guillermo SolísFernández, Chen Zhou, Jin Won Seo, Jelle Hendrix, Elke Debroye, Julian A. Steele, Johan Hofkens, Jinlin Long, & Maarten B. J. Roeffaers. (2019). ACS Energy Letters(4). https://doi.org/10.1021/acsenergylett.8b01698
IEEE [1] Haowei Huang, Haifeng Yuan, Jiwu Zhao, Guillermo SolísFernández, Chen Zhou, Jin Won Seo, Jelle Hendrix, Elke Debroye, Julian A. Steele, Johan Hofkens, Jinlin Long, and Maarten B. J. Roeffaers, ACS Energy Letters, no. 4, 2019, doi: 10.1021/acsenergylett.8b01698.