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石墨相氮化碳嵌入石墨烯材料对双酚 A 的光催化作用:石墨烯的作用和超氧自由基和单线态氧的介导作用。

Graphitic carbon nitride embedded with graphene materials towards photocatalysis of bisphenol A: The role of graphene and mediation of superoxide and singlet oxygen.

机构信息

Department of Environmental Engineering, National Cheng Kung University, Tainan City, 70101, Taiwan.

Department of Environmental Engineering, National Cheng Kung University, Tainan City, 70101, Taiwan.

出版信息

Chemosphere. 2021 Sep;278:130334. doi: 10.1016/j.chemosphere.2021.130334. Epub 2021 Mar 19.

Abstract

Composite photocatalysts comprising graphitic carbon nitride (g-CN) and graphene materials were synthesized and evaluated in the photocatalysis of bisphenol A (BPA) with a focus on elucidating the reaction mechanism. Embedding reduced graphene oxide (rGO) to g-CN significantly accelerated the photocatalysis rate of BPA by three folds under visible light irradiation at neutral pH. We showed that rGO synthesized in intimate contact with g-CN increased the surface areas and electrical conductivity of the g-CN composites and promoted the electron-hole pair separation. The BPA photodegradation mechanism involved selective oxidants as superoxide (O) and singlet oxygen (O) that were formed through one-electron reduction of O and the unique oxidation of O by photogenerated hole (h), respectively. The synthesized photocatalyst exhibited superior visible light photoreactivity to that of N-doped P25 TiO, good photo-stability and reuse potential, and was operative in complex wastewater. rGO embedded g-CN achieved good photomineralization of BPA at 80% in 4 h compared to 40% of bare g-CN. This study sheds light on the photocatalysis mechanism of BPA with a metal-free, promising rGO/g-CN photocatalyst.

摘要

包含石墨相氮化碳(g-CN)和石墨烯材料的复合光催化剂被合成并用于双酚 A(BPA)的光催化作用评估,重点在于阐明反应机制。在中性 pH 可见光照射下,将还原氧化石墨烯(rGO)嵌入 g-CN 中可使 BPA 的光催化速率显著提高三倍。我们表明,与 g-CN 紧密接触合成的 rGO 增加了 g-CN 复合材料的表面积和电导率,并促进了电子-空穴对的分离。BPA 光降解机制涉及选择性氧化剂,如超氧自由基(O)和单线态氧(O),它们分别通过 O 的单电子还原和光生空穴(h)对 O 的独特氧化形成。所合成的光催化剂表现出优于 N 掺杂 P25 TiO 的可见光光反应活性、良好的光稳定性和再利用潜力,并可在复杂废水中使用。与裸露的 g-CN 相比,rGO 嵌入 g-CN 在 4 h 内可实现 BPA 的良好光矿化作用,达到 80%,而裸露的 g-CN 仅为 40%。本研究为无金属、有前途的 rGO/g-CN 光催化剂的 BPA 光催化机制提供了启示。

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