Journal
NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-31967-0
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Funding
- National Natural Science Foundation of China [22025204, 92034301, 21904127]
- Innovation Program of the Shanghai Municipal Education Commission [2021-01-07-00-02-E00119]
- Shanghai Science Technology [19070502700]
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Traditional approaches for transition-metal catalyzed oxidative cross-coupling reactions rely on sp(2)-hybridized starting materials. Here the authors report a novel heterogeneous Pd-catalyzed radical relay method for the conversion of a heteroarene C(sp(3))-H bond into ethers with high efficiency and selectivity.
Traditional approaches for transition-metal catalyzed oxidative cross-coupling reactions rely on sp(2)-hybridized starting materials, such as aryl halides, and more specifically, homogeneous catalysts. We report a heterogeneous Pd-catalyzed radical relay method for the conversion of a heteroarene C(sp(3))-H bond into ethers. Pd nanoparticles are supported on an ordered mesoporous composite which, when compared with microporous activated carbons, greatly increases the Pd d charge because of their strong interaction with N-doped anatase nanocrystals. Mechanistic studies provide evidence that electron-deficient Pd with Pd-O/N coordinations efficiently catalyzes the radical relay reaction to release diffusible methoxyl radicals, and highlight the difference between this surface reaction and C-H oxidation mediated by homogeneous catalysts that operate with cyclopalladated intermediates. The reactions proceed efficiently with a turn-over frequency of 84 h(-1) and high selectivity toward ethers of >99%. Negligible Pd leaching and activity loss are observed after 7 catalytic runs. Traditional approaches for transition-metal catalyzed oxidative cross-coupling reactions rely on sp(2)-hybridized starting materials. Here the authors report a heterogeneous Pd-catalyzed radical relay method for the conversion of a heteroarene C(sp(3))-H bond into ethers.
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