Mechanism of ozone adsorption and activation on B-, N-, P-, and Si-doped graphene: A DFT study
文献类型：期刊论文
| 作者 | Yu, Guangfei1,2,3; Xie, Yongbing1; Ge, Qingfeng3; Dai, Qin1,2; Xu, Jun4; Cao, Hongbin1 |
| 刊名 | CHEMICAL ENGINEERING JOURNAL
 |
| 出版日期 | 2022-02-15 |
| 卷号 | 430页码:11 |
| 关键词 | DFT Catalytic ozonation Activation mechanism Heteroatom-doped graphene QSAR |
| ISSN号 | 1385-8947 |
| DOI | 10.1016/j.cej.2021.133114 |
| 英文摘要 | The detailed evolution mechanism of O-3 into Reactive oxygen species (ROS) is of paramount importance but remains elusive in catalytic ozonation. Herein, we report a density functional theory study to comprehensively reveal the specific evolution processes of O-3 into ROS on the B-, N-, P-, and Si-doped graphene, including the adsorption, decomposition and ROS generation. In contrast to some previous reports that O-3 would directly decompose into effective ROS on catalysts, our results indicate that after O-3 adsorption, the decomposition products are ground state O-2 and the adsorbed oxygen species (O-ads). The O-ads is more likely to act as a crucial intermediate for generating other ROS instead of directly attacking the organics. The type of the ROS and generation efficiency vary with the doped heteroatoms, and the heteroatoms of B, P and Si, or the neighboring C of N, would serve as active sites for O-3 adsorption and decomposition. The N-and P-doped graphene are predicted to have the superior performance in ROS generation and catalytic stability. Finally, twenty representative descriptors were adopted to build the quantitative structure-activity relationship (QSAR) with the activation energy barrier of O-3 decomposition. The result indicates that condensed dual descriptor (CDD) could be useful for preliminarily selecting the modified graphene catalysts, since it shows a very good linear relation with the activation energy barrier. This contribution provides an alternative way to gain fundamental insights into the mechanism of catalytic ozonation at the molecular level, and could be helpful for designing more-efficient catalysts in environmental remediation. |
| WOS关键词 | EFFICIENT CATALYTIC OZONATION ; FENTON-LIKE CATALYST ; OXYGEN REDUCTION ; OXIDATION ; CO ; GRAPHITE ; INITIATION ; RADICALS ; DEFECTS ; MN |
| 资助项目 | Tianjin Municipal Sci-ence and Technology Bureau[18YFYSZ00170] ; Major Science and Technology Program for Water Pollution Control and Treatment[2017ZX07402001] ; Major Science and Technology Program for Water Pollution Control and Treatment[2017ZX07402004] |
| WOS研究方向 | Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:000740950400004 |
| 出版者 | ELSEVIER SCIENCE SA |
| 资助机构 | Tianjin Municipal Sci-ence and Technology Bureau ; Major Science and Technology Program for Water Pollution Control and Treatment |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/51617]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Ge, Qingfeng; Cao, Hongbin |
| 作者单位 | 1.Chinese Acad Sci, Beijing Engn Res Ctr Proc Pollut Control, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Southern Illinois Univ, Dept Chem & Biochem, Carbondale, IL 62901 USA 4.South China Univ Technol, State Key Lab Pulp & Paper Engn, Guangzhou 510640, Peoples R China |
| 推荐引用方式 GB/T 7714 | Yu, Guangfei,Xie, Yongbing,Ge, Qingfeng,et al. Mechanism of ozone adsorption and activation on B-, N-, P-, and Si-doped graphene: A DFT study[J]. CHEMICAL ENGINEERING JOURNAL,2022,430:11. |
| APA | Yu, Guangfei,Xie, Yongbing,Ge, Qingfeng,Dai, Qin,Xu, Jun,&Cao, Hongbin.(2022).Mechanism of ozone adsorption and activation on B-, N-, P-, and Si-doped graphene: A DFT study.CHEMICAL ENGINEERING JOURNAL,430,11. |
| MLA | Yu, Guangfei,et al."Mechanism of ozone adsorption and activation on B-, N-, P-, and Si-doped graphene: A DFT study".CHEMICAL ENGINEERING JOURNAL 430(2022):11. |
入库方式： OAI收割
来源：过程工程研究所
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