Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal
Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance. Herein, the underlying nature of N promotional effects on peroxymonosulfate (PMS) activation for phenol removal is understood by combining kinetics analysis with multiple techniques. A s...
| Main Authors: | , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
KeAi Communications Co., Ltd.
2020-10-01
|
| Series: | Green Energy & Environment |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2468025720300558 |
| _version_ | 1818616362133618688 |
|---|---|
| author | Mingjie Zhang Chen Han Wenyao Chen Wei Luo Yueqiang Cao Gang Qian Xinggui Zhou Xiaoguang Duan Shaobin Wang Xuezhi Duan |
| author_facet | Mingjie Zhang Chen Han Wenyao Chen Wei Luo Yueqiang Cao Gang Qian Xinggui Zhou Xiaoguang Duan Shaobin Wang Xuezhi Duan |
| author_sort | Mingjie Zhang |
| collection | DOAJ |
| description | Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance. Herein, the underlying nature of N promotional effects on peroxymonosulfate (PMS) activation for phenol removal is understood by combining kinetics analysis with multiple techniques. A strategy using mixed acid oxidation of carbon nanotube (CNT) followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp2-hybridized carbon and defective degree, endowing with a chance to discriminate the dominant N-containing active sites. The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites. The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism. The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis. |
| first_indexed | 2024-12-16T16:48:35Z |
| format | Article |
| id | doaj.art-36311c3077f1415ab405ef18c20f7072 |
| institution | Directory Open Access Journal |
| issn | 2468-0257 |
| language | English |
| last_indexed | 2024-12-16T16:48:35Z |
| publishDate | 2020-10-01 |
| publisher | KeAi Communications Co., Ltd. |
| record_format | Article |
| series | Green Energy & Environment |
| spelling | doaj.art-36311c3077f1415ab405ef18c20f70722022-12-21T22:24:06ZengKeAi Communications Co., Ltd.Green Energy & Environment2468-02572020-10-0154444452Active sites and reaction mechanism for N-doped carbocatalysis of phenol removalMingjie Zhang0Chen Han1Wenyao Chen2Wei Luo3Yueqiang Cao4Gang Qian5Xinggui Zhou6Xiaoguang Duan7Shaobin Wang8Xuezhi Duan9State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China; WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, Western Australia 6845, AustraliaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China; Corresponding author.Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance. Herein, the underlying nature of N promotional effects on peroxymonosulfate (PMS) activation for phenol removal is understood by combining kinetics analysis with multiple techniques. A strategy using mixed acid oxidation of carbon nanotube (CNT) followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp2-hybridized carbon and defective degree, endowing with a chance to discriminate the dominant N-containing active sites. The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites. The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism. The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.http://www.sciencedirect.com/science/article/pii/S2468025720300558Phenol removalCarbocatalysisMulti-sites kinetics analysisGraphitic N-Containing sitesSurface-bound reactive species |
| spellingShingle | Mingjie Zhang Chen Han Wenyao Chen Wei Luo Yueqiang Cao Gang Qian Xinggui Zhou Xiaoguang Duan Shaobin Wang Xuezhi Duan Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal Green Energy & Environment Phenol removal Carbocatalysis Multi-sites kinetics analysis Graphitic N-Containing sites Surface-bound reactive species |
| title | Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal |
| title_full | Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal |
| title_fullStr | Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal |
| title_full_unstemmed | Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal |
| title_short | Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal |
| title_sort | active sites and reaction mechanism for n doped carbocatalysis of phenol removal |
| topic | Phenol removal Carbocatalysis Multi-sites kinetics analysis Graphitic N-Containing sites Surface-bound reactive species |
| url | http://www.sciencedirect.com/science/article/pii/S2468025720300558 |
| work_keys_str_mv | AT mingjiezhang activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT chenhan activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT wenyaochen activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT weiluo activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT yueqiangcao activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT gangqian activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT xingguizhou activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT xiaoguangduan activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT shaobinwang activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval AT xuezhiduan activesitesandreactionmechanismforndopedcarbocatalysisofphenolremoval |