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

Jiawei Li, Liuqing He, Qiong Liu, Yanwei Ren () and Huanfeng Jiang ()
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Jiawei Li: South China University of Technology
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

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-28474-7

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