Reducing the excition binding energy of covalent-organic frameworks via spatial-confined NiCo-NC as internal nanoreactors for photocatalytic hydrogen evolution

文献类型： 外文期刊

第一作者： Pan, Ailing

作者： Pan, Ailing;Che, Yuanyuan;Du, Hong;Sun, Xiaohui;Wang, Yu;Du, Hong

作者机构：

关键词： Nanoreactor; Hydrogen bond; Hydrogen evolution; Excitation binding energy; Spatial-confined

期刊名称：JOURNAL OF COLLOID AND INTERFACE SCIENCE （ 影响因子：9.7； 五年影响因子：8.9 ）

ISSN： 0021-9797

年卷期： 2025 年 697 卷

页码：

收录情况： SCI

摘要： COFs (covalent-organic frameworks) are regarded as ideal photocatalyst for hydrogen-evolution, due to their structural controllability, but they possess poor electrical conductivity and high exciton binding energy, which limits their photocatalytic activity. Here, the NiCo-ZIF-67 derived NiCo-nitrogen-doped carbon (NiCo-NC) with superior conductivity and high light-absorption capacity was spatially confined in the channels of TP-BD COF (TP: 2, 4, 6-triformylphloroglucino; BD: 4, 4 '-biphenylenediamin) by constructing hydrogen bonds to form NiCo-NC@TP-BD COF core@shell heterojunctions and NiCo-NC acts as internal highly active nanoreactor, which could accelerate the photocatalytic efficiency. Specifically, the optimal catalyst NiCo-NC@TP-BD-0.6 (NT-0.6) exhibits the maximum H2 evolution rate of 78.97mmol g-1 h-1 without Pt cocatalyst, which is approximately 395 times higher than that of bare TP-BD COF. Systematic investigations imply that the NiCo-NC as a high active nanoreactor was stably encapsulated in the pore of TP-BD by hydrogen bonds and formed a close interfacial contact, which is revealed by Fourier-transform infrared spectroscopy (FT-IR) and proton nuclear magnetic resonance (1H NMR). Meanwhile, the charge transfer and Hydrogen Evolution Reaction (HER) are revealed by the density functional theory (DFT) calculation. This work offers a promising strategy to reduce the high excitation binding energy of COFs-based catalysts in photocatalytic H2 evolution.

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