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

• DOI: 10.1021/acs.est.9b01361
• Publication Date: 2019-04-18T11:24:26Z
• Authors: Zilong Song; Mengxuan Wang; Zheng Wang; Yufang Wang; Ruoyu Li; Yuting Zhang; Chao Liu; Ye Liu; Bingbing Xu; Fei Qi
• Keywords: Heteroatom

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