Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts

ACS Applied Optical Materials Pub Date : 2025-04-16 DOI:10.1021/acsaom.5c0001910.1021/acsaom.5c00019

Allison St. John, Hannah Flayhart, Shuting Xiang, Qian Qian, N. Aaron Deskins, Anatoly I. Frenkel, Jonathan Rochford* and Gonghu Li*,

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Abstract

Graphitic carbon nitride (C₃N₄) has been widely explored as a photoactive support for single-atom catalysts (SACs). In this study, three different π-rich aromatic dianhydrides are employed to introduce molecularly quantized trap states into the conduction band of C₃N₄ to facilitate efficient charge separation, and to promote an enhanced photocatalytic CO₂ reduction response. These modified C₃N₄ materials have been characterized structurally and spectroscopically for use as a support for Co-based SACs. In photocatalytic CO₂ reduction studies, the Co SAC on naphthalene dianhydride-doped C₃N₄ exhibited the highest activity and selectivity toward CO production among the Co SACs tested in this work. The observed improvement in photocatalytic CO₂-to-CO conversion activity correlates with trends in photoinduced charge separation, as revealed by photoluminescence spectroscopy.

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二酐改性石墨氮化碳作为钴单原子光催化剂的载体

石墨化氮化碳（C3N4）作为单原子催化剂（SACs）的光活性载体已被广泛探索。本研究采用三种不同的富π芳香二酐，在C3N4的导带中引入分子量子化的阱态，以促进有效的电荷分离，并增强光催化CO2还原反应。这些改性的C3N4材料已经在结构和光谱上进行了表征，可以作为钴基SACs的载体。在光催化CO2还原研究中，二氢萘掺杂C3N4上的Co SAC在本工作测试的Co SAC中表现出最高的Co生成活性和选择性。光致发光光谱显示，光催化CO2-to-CO转化活性的提高与光诱导电荷分离的趋势有关。

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来源期刊

ACS Applied Optical Materials 材料科学-光学材料-

CiteScore

1.10

自引率

0.00%

发文量

期刊介绍： ACS Applied Optical Materials is an international and interdisciplinary forum to publish original experimental and theoretical including simulation and modeling research in optical materials complementing the ACS Applied Materials portfolio. With a focus on innovative applications ACS Applied Optical Materials also complements and expands the scope of existing ACS publications that focus on fundamental aspects of the interaction between light and matter in materials science including ACS Photonics Macromolecules Journal of Physical Chemistry C ACS Nano and Nano Letters.The scope of ACS Applied Optical Materials includes high quality research of an applied nature that integrates knowledge in materials science chemistry physics optical science and engineering.