Role of oxygen vacancies and Mn sites in hierarchical Mn2O3/LaMnO3-delta perovskite composites for aqueous organic pollutants decontamination
文献类型：期刊论文
| 作者 | Wang, Yuxian1,2; Chen, Lulu1; Cao, Hongbin2; Chi, Zhaoxu1; Chen, Chunmao1; Duan, Xiaoguang3; Xie, Yongbing2; Qi, Fei4; Song, Weiyu1; Liu, Jian1 |
| 刊名 | APPLIED CATALYSIS B-ENVIRONMENTAL
 |
| 出版日期 | 2019-05-15 |
| 卷号 | 245页码:546-554 |
| ISSN号 | 0926-3373 |
| 关键词 | Perovskites Catalytic ozonation Oxygen vacancies Density functional theory Reactive oxygen species |
| DOI | 10.1016/j.apcatb.2019.01.025 |
| 英文摘要 | La-based perovskites are catalytically active owing to the oxygen vacancies, redox metal centers of B sites and surface hydroxyl groups. Nevertheless, the insights into these active centers on environmental catalysis are still insufficient. In this study, hierarchical mixed oxides perovskite microspheres were synthesized for catalytic ozonation over oxalic acid and benzotriazole. LaMn4O., with LaMnO3-delta as the dominant crystal phase, demonstrated superior catalytic activity to Mn2O3 and LaMnO3 synthesized from citric acid sol-gel method. Temperature-programmed desorption of NH3 (NH3-TPD) and pyridine-Fourier transform infrared spectroscopy (pyridine-FTIR) tests proved Lewis acid as the main acid type. Temperature-programmed reduction of H-2 (H-2-TPR), O-2-TPD and X-ray photoelectron spectroscopy (XPS) analysis indicated the presence of oxygen vacancies and mixed valences of Mn in the crystal structure facilitated the catalytic process. Moreover, the content of oxygen vacancy was calculated by iodometric titration method. With the aid of theoretical calculations, oxygen vacancies were found to exhibit a strong affinity toward ozone adsorption, where ozone molecules spontaneously dissociated into reactive oxygen species (ROS) such as O-2(center dot-) and O-1(2). The B site of Mn facilitated ozone decomposition by extending the O-O bond of ozone due to the electron transfer from Mn3+/Mn4+ redox cycle. In-situ EPR and quenching tests confirmed the contribution of O-2(center dot-) and O-1(2) in benzotriazole degradation along with (OH)-O-center dot. This study stepped further to unveil the ozone adsorption/decomposition and ROS generation on nanoscale perovskite-based composites. |
| WOS关键词 | ADVANCED OXIDATION PROCESS ; CATALYTIC OZONATION ; OXIDE CATALYSTS ; DEGRADATION ; OZONE ; PEROXYMONOSULFATE ; MECHANISM ; KINETICS ; BENZOTHIAZOLE ; BENZOTRIAZOLE |
| 资助项目 | National Natural Science Foundation of China[21606253] ; National Science Fund for Distinguished Young Scholars of China[51425405] ; Science Foundation of China University of Petroleum, Beijing[2462016YJRC013] ; Beijing Natural Science Foundation[8172043] ; Major Science and Technology Program for Water Pollution Control and Treatment[2017ZX07402003] ; Major Science and Technology Program for Water Pollution Control and Treatment[2017ZX07402001] |
| WOS研究方向 | Chemistry ; Engineering |
| 语种 | 英语 |
| 出版者 | ELSEVIER SCIENCE BV |
| WOS记录号 | WOS:000467661700055 |
| 资助机构 | National Natural Science Foundation of China ; National Science Fund for Distinguished Young Scholars of China ; Science Foundation of China University of Petroleum, Beijing ; Beijing Natural Science Foundation ; Major Science and Technology Program for Water Pollution Control and Treatment |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/28198]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Xie, Yongbing; Liu, Jian |
| 作者单位 | 1.China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China 2.Chinese Acad Sci, Inst Proc Engn, Div Environm Technol & Engn, Beijing 100190, Peoples R China 3.Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia 4.Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing Key Lab Source Control Technol Water Poll, Beijing 100083, Peoples R China |
| 推荐引用方式 GB/T 7714 | Wang, Yuxian,Chen, Lulu,Cao, Hongbin,et al. Role of oxygen vacancies and Mn sites in hierarchical Mn2O3/LaMnO3-delta perovskite composites for aqueous organic pollutants decontamination[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,245:546-554. |
| APA | Wang, Yuxian.,Chen, Lulu.,Cao, Hongbin.,Chi, Zhaoxu.,Chen, Chunmao.,...&Wang, Shaobin.(2019).Role of oxygen vacancies and Mn sites in hierarchical Mn2O3/LaMnO3-delta perovskite composites for aqueous organic pollutants decontamination.APPLIED CATALYSIS B-ENVIRONMENTAL,245,546-554. |
| MLA | Wang, Yuxian,et al."Role of oxygen vacancies and Mn sites in hierarchical Mn2O3/LaMnO3-delta perovskite composites for aqueous organic pollutants decontamination".APPLIED CATALYSIS B-ENVIRONMENTAL 245(2019):546-554. |
入库方式： OAI收割
来源：过程工程研究所
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