Origin of the improved reactivity of MoS2 single crystal by confining lattice Fe atom in peroxymonosulfate-based Fenton-like reaction

被引:82
作者
Sun, Yibing [1 ]
Li, Ruiping [2 ,3 ]
Song, Chunli [1 ]
Zhang, Hao [2 ,3 ]
Cheng, Yingchun [2 ,3 ]
Nie, Anmin [5 ]
Li, Hongchao [1 ]
Dionysiou, Dionysios D. [6 ]
Qian, Jieshu [1 ,4 ]
Pan, Bingcai [4 ]
机构
[1] Nanjing Univ Sci & Technol, Sch Environm & Biol Engn, Jiangsu Key Lab Chem Pollut Control & Resources R, Nanjing 210094, Peoples R China
[2] Nanjing Tech Univ, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Key Lab Flexible Elect, Nanjing 211816, Peoples R China
[3] Nanjing Tech Univ, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Inst Adv Mat, Nanjing 211816, Peoples R China
[4] Nanjing Univ, Res Ctr Environm Nanotechnol ReCENT, Sch Environm, State Key Lab Pollut Control & Resources Reuse, Nanjing 210023, Peoples R China
[5] Yanshan Univ, Ctr High Pressure Sci, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Hebei, Peoples R China
[6] Univ Cincinnati, Dept Chem & Environm Engn, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
关键词
Peroxymonosulfate; Fenton-like reaction; MoS2 single crystal; Confinement; Chemical vapor transport; FREE-RADICALS; ORGANIC CONTAMINANTS; HYDROXYL RADICALS; RATE CONSTANTS; DEGRADATION; ACTIVATION; OXIDATION; WATER; PERFORMANCE; GENERATION;
D O I
10.1016/j.apcatb.2021.120537
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
In this study, we describe a confinement of trace amount of Fe atoms (0.66 at. parts per thousand) in Mo lattice, via a chemical vapor transport growth of MoS2 single crystal. In the Fenton-like reaction for the degradation of atrazine, the Fe@MoS2 as catalyst to activate PMS could produce more reactive oxygen species and exhibit a rate constant (1.30 min(-1)) three times higher than that of pristine MoS2 (0.43 min(-1)). Theoretical simulation suggests that the diluted confinement of Fe atoms in Mo sites activates the inert basal plane of MoS2, creating new active sites of Mo both nearby the Fe site and afar, for the adsorption and decomposition of PMS. Our work provides a clear atomic mechanism of the improvement of the chemical reactivity of MoS2 single crystal in Fenton-like reaction via heteroatom confinement.
引用
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页数:10
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