Статья

Insights into Heteroatom-Doped Graphene for Catalytic Ozonation: Active Centers, Reactive Oxygen Species Evolution, and Catalytic Mechanism

Zilong SongBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaMengxuan WangBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaZheng WangBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaYufang WangBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaRuoyu LiBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaYuting ZhangBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaChao LiuBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaLiu YeBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, ChinaBingbing XuState Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, ChinaFei QiBeijing Key Laboratory for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China

2019en

ABI

Аннотация

To guide the design of novel graphene-based catalysts in catalytic ozonation for micropollutant degradation, the mechanism of catalytic ozonation with heteroatom-doped graphene was clarified. Reduced graphene oxide doped with nitrogen, phosphorus, boron, and sulfur atoms (N-, P-, B-, and S-rGO) were synthesized, and their catalytic ozonation performances were evaluated in the degradation of refractory organics and bromate elimination simultaneously. Doping with heteroatoms, except sulfur, significantly improved the catalytic ozonation activity of graphene. Introducing sulfur atoms destroyed the stability of graphene during ozonation, with the observed partial performance improvement caused by surface adsorption. Degradation pathways for selected refractory organics were proposed based on the intermediates identified using high-resolution Orbitrap mass spectroscopy and gas chromatographic–mass spectroscopy. Three and six new unopened intermediates were identified in benzotriazole and p-chlorobenzoic acid degradation, respectively. Roles of chemical functional groups, doped atoms, free electron, and delocalized π electron of heteroatom-doped graphene in catalytic ozonation were identified, and contributions of these active centers to the formation of reactive oxygen species (ROS), including hydroxyl radicals, superoxide radicals, singlet oxygen, and H2O2, were evaluated. A mechanism for catalytic ozonation by heteroatom-doped graphene was proposed for the first time.

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Идентификаторы

DOI: 10.1021/acs.est.9b01361

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