Occurrence of both hydroxyl radical and surface oxidation pathways in N-doped layered nanocarbons for aqueous catalytic ozonation
文献类型：期刊论文
| 作者 | Wang, Yuxian1,3; Chen, Lulu3; Chen, Chunmao2; Xi, Jiaxin3; Cao, Hongbin1; Duan, Xiaoguang4; Xie, Yongbing1; Song, Weiyu3; Wang, Shaobin4 |
| 刊名 | APPLIED CATALYSIS B-ENVIRONMENTAL
 |
| 出版日期 | 2019-10-05 |
| 卷号 | 254页码:283-291 |
| ISSN号 | 0926-3373 |
| 关键词 | Metal-free catalysis Catalytic ozonation Nitrogen doping Surface oxidation Density functional theory (DFT) |
| DOI | 10.1016/j.apcatb.2019.05.008 |
| 英文摘要 | Metal-free catalysts such as N-doped nanocarbons are sustainable alternatives to metal-based catalysts for the degradation of persistent organic pollutants (POPs), but cost-efficient methods are required for their large-scale synthesis. In this study, a facile and scalable strategy was established for synthesizing layered N-doped nanocarbons via the pyrolysis of beta-cyclodextrin (beta-CD) and melamine in a N-2 atmosphere. Compared with undoped pyrolyzed beta-CD, N-doping led to a 30.3-fold enhancement in the pseudo-first-order rate constant for catalytic ozonation of oxalic acid (OA), and complete degradation of 50 mg/L OA was achieved in 45 min. Apart from the specific surface area boosting from 78.9 to 16.2 m(2)/g after N doping, the OA degradation results and material characterization also suggested that quaternary N was the main active site, which was further validated by density functional theory (DFT) simulations. DFT simulations also suggested that C atoms with high charge densities adjacent to N dopants exhibited considerable potential for the catalytic dissociation of ozone. Electron paramagnetic resonance (EPR), radical quenching, and in situ Raman studies indicated occurrence of surface oxidation pathway apart from the radical-based one. Ozone on the catalyst surface was decomposed into surface-adsorbed atomic oxygen (*O-ad) and free peroxide (*O-2 (free)). Both *O-ad and (OH)-O-center dot, which was further evolved on the surface or in bulk solution, contributed to OA destruction. These insights into the catalytic ozonation mechanism on N-doped nanocarbons will advance their practical application to the catalytic degradation of organic pollutants. |
| WOS关键词 | REDUCED GRAPHENE OXIDE ; METAL-FREE CATALYST ; OZONE DECOMPOSITION ; REACTIVE RADICALS ; CARBON NANOTUBES ; ACTIVATED CARBON ; DEGRADATION ; WATER ; PEROXYMONOSULFATE ; REDUCTION |
| 资助项目 | National Science Fund for Distinguished Young Scholars of China[51425405] ; National Natural Science Foundation of China[21606253] ; Science Foundation of China University of Petroleum, Beijing[2462016YJRC013] ; Beijing Natural Science Foundation[8172043] ; Independent Project of the State Key Laboratory of Petroleum Pollution Control, CNPC Research Institute of Safety and Environmental Technology[2017004] |
| WOS研究方向 | Chemistry ; Engineering |
| 语种 | 英语 |
| 出版者 | ELSEVIER SCIENCE BV |
| WOS记录号 | WOS:000472697500028 |
| 资助机构 | National Science Fund for Distinguished Young Scholars of China ; National Natural Science Foundation of China ; Science Foundation of China University of Petroleum, Beijing ; Beijing Natural Science Foundation ; Independent Project of the State Key Laboratory of Petroleum Pollution Control, CNPC Research Institute of Safety and Environmental Technology |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/30042]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Xie, Yongbing; Song, Weiyu |
| 作者单位 | 1.Chinese Acad Sci, Inst Proc Engn, Div Environm Technol & Engn, Beijing 100190, Peoples R China 2.China Univ Petr, State Key Lab Petr Pollut Control, Beijing 102200, Peoples R China 3.China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China 4.Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia |
| 推荐引用方式 GB/T 7714 | Wang, Yuxian,Chen, Lulu,Chen, Chunmao,et al. Occurrence of both hydroxyl radical and surface oxidation pathways in N-doped layered nanocarbons for aqueous catalytic ozonation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,254:283-291. |
| APA | Wang, Yuxian.,Chen, Lulu.,Chen, Chunmao.,Xi, Jiaxin.,Cao, Hongbin.,...&Wang, Shaobin.(2019).Occurrence of both hydroxyl radical and surface oxidation pathways in N-doped layered nanocarbons for aqueous catalytic ozonation.APPLIED CATALYSIS B-ENVIRONMENTAL,254,283-291. |
| MLA | Wang, Yuxian,et al."Occurrence of both hydroxyl radical and surface oxidation pathways in N-doped layered nanocarbons for aqueous catalytic ozonation".APPLIED CATALYSIS B-ENVIRONMENTAL 254(2019):283-291. |
入库方式： OAI收割
来源：过程工程研究所
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