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<p>The functionalization of C–H bonds is a core challenge in synthetic chemistry, which is limited by the development of heterogeneous catalysts that possess high oxidation ability, selectivity, and stability. This paper reports a new two-dimensional interpenetrating metal-organic framework based on decatungstate (POMOFs), namely Cu<sub>3</sub>-BPE-W<sub>10</sub>, BPE=1,2-bis(4-pyridyl)ethylene. The single crystal structure analysis indicates that the formed chains can act as an electronic transmission channel, facilitating the transfer of photogenerated charges and being conducive to proton-coupled electron transfer under different substrates. Under visible light irradiation, Cu<sub>3</sub>-BPE-W<sub>10</sub> can achieve highly selective oxidation of the C(sp<sup>3</sup>)–H bond in diphenylmethane (DPM) to diphenylketone (BP) (with a conversion rate of 99.9% and selectivity of 100%). The outstanding photocatalytic performance can be ascribed to the synergistic effect of the individual parts in Cu<sub>3</sub>-BPE-W<sub>10</sub>, in which the W<sub>10</sub> cluster acts as the photosensitive unit dominating the initial activation of the C–H bond, the trinuclear copper chains promote the activation of TBHP, and collaboratively reduce the energy barrier for C–H bond cleavage. This work achieves the precise combination of the photocatalytic redox ability of W<sub>10</sub> and the multi-nuclear copper center through structural design, providing a new strategy for the design of efficient heterogeneous C–H bond photocatalysts.</p>

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Triple-core copper(II) chain-constructed W10-MOFs for efficient photocatalytic activation of benzyl C–H bonds

  • 期刊论文

  • 发表日期：

    2026年7月24日

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  • Yanjie Lv,
  • Xinyu Zhao,
  • Jing Sun,
  • Wenxi Zhang,
  • Yuzhe Tang,
  • Xiao Li,
  • Zhongmin Su

摘要

The functionalization of C–H bonds is a core challenge in synthetic chemistry, which is limited by the development of heterogeneous catalysts that possess high oxidation ability, selectivity, and stability. This paper reports a new two-dimensional interpenetrating metal-organic framework based on decatungstate (POMOFs), namely Cu3-BPE-W10, BPE=1,2-bis(4-pyridyl)ethylene. The single crystal structure analysis indicates that the formed chains can act as an electronic transmission channel, facilitating the transfer of photogenerated charges and being conducive to proton-coupled electron transfer under different substrates. Under visible light irradiation, Cu3-BPE-W10 can achieve highly selective oxidation of the C(sp3)–H bond in diphenylmethane (DPM) to diphenylketone (BP) (with a conversion rate of 99.9% and selectivity of 100%). The outstanding photocatalytic performance can be ascribed to the synergistic effect of the individual parts in Cu3-BPE-W10, in which the W10 cluster acts as the photosensitive unit dominating the initial activation of the C–H bond, the trinuclear copper chains promote the activation of TBHP, and collaboratively reduce the energy barrier for C–H bond cleavage. This work achieves the precise combination of the photocatalytic redox ability of W10 and the multi-nuclear copper center through structural design, providing a new strategy for the design of efficient heterogeneous C–H bond photocatalysts.