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Visible light-driven efficient palladium catalyst turnover in oxidative transformations within confined frameworks

Author

Listed:
  • Jiawei Li

    (South China University of Technology
    Central South University)

  • Liuqing He

    (Central South University)

  • Qiong Liu

    (Guangdong Academy of Sciences (China National Analytical Center, Guangzhou))

  • Yanwei Ren

    (South China University of Technology)

  • Huanfeng Jiang

    (South China University of Technology)

Abstract

Palladium catalyst turnover by reoxidation of a low-valent Pd species dominates the proceeding of an efficient oxidative transformation, but the state-of-the-art catalysis approaches still have great challenges from the perspectives of high efficiency, atom-economy and environmental-friendliness. Herein, we report a new strategy for addressing Pd reoxidation problem by the fabrication of spatially proximate IrIII photocatalyst and PdII catalyst into metal-organic framework (MOF), affording MOFs based Pd/photoredox catalysts UiO-67-Ir-PdX2 (X = OAc, TFA), which are systematically evaluated using three representative Pd-catalyzed oxidation reactions. Owing to the stabilization of single-site Pd and Ir catalysts by MOFs framework as well as the proximity of them favoring fast electron transfer, UiO-67-Ir-PdX2, under visible light, exhibits up to 25 times of Pd catalyst turnover number than the existing catalysis systems. Mechanism investigations theoretically corroborate the capability of MOFs based Pd/photoredox catalysis to regulate the competitive processes of Pd0 aggregation and reoxidation in Pd-catalyzed oxidation reactions.

Suggested Citation

  • Jiawei Li & Liuqing He & Qiong Liu & Yanwei Ren & Huanfeng Jiang, 2022. "Visible light-driven efficient palladium catalyst turnover in oxidative transformations within confined frameworks," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28474-7
    DOI: 10.1038/s41467-022-28474-7
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    References listed on IDEAS

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    1. Craig P. Johnston & Russell T. Smith & Simon Allmendinger & David W. C. MacMillan, 2016. "Metallaphotoredox-catalysed sp3–sp3 cross-coupling of carboxylic acids with alkyl halides," Nature, Nature, vol. 536(7616), pages 322-325, August.
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