| Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution | |
| Wang, Jing1,2; Xie, Yongbing1; Yu, Guangfei1; Yin, Lichang3; Xiao, Jiadong4; Wang, Yuxian5; Lv, Weiguang1,2; Sun, Zhi1; Kim, Jae-Hong6; Cao, Hongbin1 | |
| Corresponding Author | Cao, Hongbin(hbcao@ipe.ac.cn) |
| 2022-11-29 | |
| Source Publication | ENVIRONMENTAL SCIENCE & TECHNOLOGY
 |
| ISSN | 0013-936X |
| Pages | 10 |
| Abstract | Hydroxyl radical-dominated oxidation in catalytic ozonation is, in particular, important in water treatment scenarios for removing organic contaminants, but the mechanism about ozone-based radical oxidation processes is still unclear. Here, we prepared a series of transitional metal (Co, Mn, Ni) single-atom catalysts (SACs) anchored on graphitic carbon nitride to accelerate ozone decomposition and produce highly reactive center dot OH for oxidative destruction of a water pollutant, oxalic acid (OA). We experimentally observed that, depending on the metal type, OA oxidation occurred dominantly either in the bulk phase, which was the case for the Mn catalyst, or via a combination of the bulk phase and surface reaction, which was the case for the Co catalyst. We further performed density functional theory simulations and in situ X-ray absorption spectroscopy to propose that the ozone activation pathway differs depending on the oxygen binding energy of metal, primarily due to differential adsorption of O3 onto metal sites and differential coordination configuration of a key intermediate species, *OO, which is collectively responsible for the observed differences in oxidation mechanisms and kinetics. |
| Keyword | single-atom catalysts hydroxyl radical transitional metals surface oxidation solution oxidation catalytic ozonation |
| Funding Organization | National Natural Science Foundation of China ; State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization |
| DOI | 10.1021/acs.est.2c06836 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | National Natural Science Foundation of China[51934006] ; State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization[2021P4FZG04A] |
| WOS Research Area | Engineering ; Environmental Sciences & Ecology |
| WOS Subject | Engineering, Environmental ; Environmental Sciences |
| WOS ID | WOS:000891808200001 |
| Publisher | AMER CHEMICAL SOC |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/176923 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Cao, Hongbin |
| Affiliation | 1.Chinese Acad Sci, Inst Proc Engn, Chem & Chem Engn Data Ctr, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Shinshu Univ, Res Initiat Supramat, Interdisciplinary Cluster Cutting Edge Res, Nagano 3808553, Japan 5.China Univ Petr, State Key Lab Heavy Oil Proc, State Key Lab Petr Pollut Control, Beijing 102249, Peoples R China 6.Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06511 USA |
| Recommended Citation GB/T 7714 | Wang, Jing,Xie, Yongbing,Yu, Guangfei,et al. Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2022:10. |
| APA | Wang, Jing.,Xie, Yongbing.,Yu, Guangfei.,Yin, Lichang.,Xiao, Jiadong.,...&Cao, Hongbin.(2022).Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution.ENVIRONMENTAL SCIENCE & TECHNOLOGY,10. |
| MLA | Wang, Jing,et al."Manipulating Selectivity of Hydroxyl Radical Generation by Single- Atom Catalysts in Catalytic Ozonation: Surface or Solution".ENVIRONMENTAL SCIENCE & TECHNOLOGY (2022):10. |
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