Fine-Tuning Radical/Nonradical Pathways on Graphene by Porous Engineering and Doping Strategies

被引:104
作者
Li, Xintong [1 ,2 ]
Wang, Jun [1 ]
Duan, Xiaoguang [3 ]
Li, Yang [1 ]
Fan, Xiaobin [1 ]
Zhang, Guoliang [1 ]
Zhang, Fengbao [1 ]
Peng, Wenchao [1 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300350, Peoples R China
[2] City Univ Hong Kong, Dept Chem, Kowloon, Hong Kong 999077, Peoples R China
[3] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
基金
中国国家自然科学基金;
关键词
doped graphene; porous engineering; peroxymonosulfate; radical oxidation; pathway tuning; OXYGEN REDUCTION REACTION; CO-DOPED GRAPHENE; CATALYTIC-OXIDATION; PHOTOCATALYTIC DEGRADATION; CARBON NANOTUBES; PEROXYMONOSULFATE ACTIVATION; HETEROGENEOUS ACTIVATION; EFFICIENT DEGRADATION; PHENOL DEGRADATION; ROBUST CATALYST;
D O I
10.1021/acscatal.0c05089
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nitrogen and sulfur co-doped graphene (N,S-G) is activated using ZnCl2, KOH, and CO2 to develop different defects and functionalities. The modified carbo-catalysts are used to activate peroxymonosulfate (PMS) for phenol degradation. Compared with nitrogen-doped graphene (N-G), N,S-G exhibits better catalytic activity, and KOH activation further enhances the oxidation efficiency. Radical quenching experiments, electrochemical characterization, and electron paramagnetic resonance characterization reveal that N-G activates PMS via a nonradical pathway. The involvement of a secondary sulfur dopant will transform the reaction pathway into radical-dominated oxidation (SO(4)(-)and OH). KOH activation further promotes the generation of the two radical species and further involves superoxide ion radicals (O-2(-)), thus achieving deeper mineralization of the organic pollutants. Different from the nonradical species confined on the catalyst surface, radical oxidation (including the singlet oxygen (O-1(2)) transformed from O-2(-)) occurs in bulk solution and protects the carbo-catalyst from corrosion, herein securing better structural integrity and stability of carbo-catalysts. Based on the structure-activity features, we designed a high-performance scalable carbo-catalyst of KOH-activated and N,S-codoped graphene (N,S-G-rGO-KOH) using a facile strategy, which is promising for practical applications.
引用
收藏
页码:4848 / 4861
页数:14
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