The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis

被引:686
作者
Ren, Wei [1 ,2 ]
Nie, Gang [1 ,2 ]
Zhou, Peng [2 ,3 ]
Zhang, Hui [1 ]
Duan, Xiaoguang [2 ]
Wang, Shaobin [2 ]
机构
[1] Wuhan Univ, Dept Environm Sci & Engn, Wuhan 430079, Peoples R China
[2] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
[3] Sichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
关键词
WALLED CARBON NANOTUBES; REDUCED GRAPHENE OXIDE; ORGANIC POLLUTANTS; CATALYTIC-OXIDATION; GRAPHITIZED NANODIAMONDS; HETEROGENEOUS CATALYSTS; PEROXYMONOSULFATE PMS; ENHANCED ACTIVATION; NONRADICAL REACTION; SINGLET OXYGEN;
D O I
10.1021/acs.est.0c01161
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Persulfates activation by carbon nanotubes (CNT) has been evidenced as nonradical systems for oxidation of organic pollutants. Peroxymonosulfate (PMS) and peroxydisulfate (PDS) possess discrepant atomic structures and redox potentials, while the nature of their distinct behaviors in carbocatalytic activation has not been investigated. Herein, we illustrated that the roles of nitrogen species in CNT-based persulfate systems are intrinsically different. In PMS activation mediated by nitrogen-doped CNT (N-CNT), surface chemical modification (N-doping) can profoundly promote the adsorption quantity of PMS, consequently elevate potential of derived nonradical N-CNT-PMS* complexes, and boost organic oxidation efficiency via an electron-transfer regime. In contrast, PDS adsorption was not enhanced upon incorporating N into CNT due to the limited equilibrium adsorption quantity of PDS, leading to a relatively lower oxidative potential of PDS/N-CNT system and a mediocre degradation rate. However, with equivalent persulfate adsorption on N-CNT at a low quantity, PDS/N-CNT exhibited a stronger oxidizing capacity than PMS/N-CNT because of the intrinsic higher redox potential of PDS than PMS. The oxidation rates of the two systems were in great linearity with the potentials of carbon-persulfate* complexes, suggesting N-CNT activation of PMS and PDS shared the similar electron-transfer oxidation mechanism. Therefore, this study provides new insights into the intrinsic roles of heteroatom doping in nanocarbons for persulfates activation and unveils the principles for a rational design of reaction-oriented carbocatalysts for persulfate-based advanced oxidation processes.
引用
收藏
页码:6438 / 6447
页数:10
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