Activation of peroxymonosulfate by Fe0@Fe3O4 core-shell nanowires for sulfate radical generation: Electron transfer and transformation products

被引:42
作者
Feng, Yong [1 ,2 ,3 ]
Zhong, Jie [1 ,2 ,3 ]
Zhang, Liyuan [4 ]
Fan, Yiang [4 ]
Yang, Zequn [4 ]
Shih, Kaimin [4 ]
Li, Hailong [5 ]
Wu, Deli [6 ]
Yan, Bo [1 ,2 ,3 ]
机构
[1] South China Normal Univ, SCNU Environm Res Inst, Guangdong Prov Key Lab Chem Pollut & Environm Saf, Guangzhou 510006, Peoples R China
[2] South China Normal Univ, MOE Key Lab Theoret Chem Environm, Guangzhou 510006, Peoples R China
[3] South China Normal Univ, Sch Environm, Guangzhou 510006, Peoples R China
[4] Univ Hong Kong, Dept Civil Engn, Pokfulam, Hong Kong, Peoples R China
[5] Cent South Univ, Sch Energy Sci & Engn, Changsha 410083, Peoples R China
[6] Tongji Univ, State Key Lab Pollut Control & Resources Reuse, Sch Environm Sci & Engn, Shanghai 200092, Peoples R China
关键词
Zero-valent iron; Fe-0@Fe3O4; Core-shell nanowires; Atrazine; Peroxymonosulfate; ZERO-VALENT IRON; RATE CONSTANTS; ADVANCED OXIDATION; ZEROVALENT IRON; DEGRADATION; PERSULFATE; OXIDANTS; REMOVAL; 1,4-DIOXANE; NZVI;
D O I
10.1016/j.seppur.2020.116942
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Nanoscale zero-valent iron (nZVI) is highly promising for oxidative removal of micropollutants by initiating advanced oxidation processes, but its vulnerability to deactivation due to the surface oxidation is challenging. In this study, we propose Fe-0@Fe3O4 core-shell nanowires (CSNWs) as a novel activator to generate radicals for atrazine, a representative micropollutant, degradation via the activation of peroxymonosulfate (PMS). Fe-0@Fe3O4 CSNWs with a shell thickness of around 5 nm were synthesized using a facile chemical reduction approach and were comprehensively characterized using a series of surface sensitive techniques. The results showed that the Fe-0@Fe3O4 CSNW had great reactivity for atrazine degradation via the activation of PMS; near complete degradation of atrazine was achieved after reaction for only 2 min. Under identical conditions, the pseudo-first order rate constant with Fe-0@Fe3O4 was more than 36 times greater than that with nano Fe3O4. The surface activation of PMS contributed only a small proportion to the overall degradation. Instead, the iron released from Fe-0@Fe3O4 CSNWs primarily activated PMS to generate SO4 center dot- that degraded atrazine. The Fe-0@Fe3O4 CSNWs were stable and no deactivation was observed after exposing Fe-0@Fe(3)O(4 )CSNWs to air for 3 months. The results from this study demonstrate a stable nZVI for oxidative removal of organic contaminants.
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页数:8
相关论文
共 56 条
[1]   Core-Shell Structure Dependent Reactivity of Fe@Fe2O3 Nanowires on Aerobic Degradation of 4-Chlorophenol [J].
Ai, Zhihui ;
Gao, Zhiting ;
Zhang, Lizhi ;
He, Weiwei ;
Yin, Jun Jie .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5344-5352
[2]   Emerging opportunities for nanotechnology to enhance water security [J].
Alvarez, Pedro J. J. ;
Chan, Candace K. ;
Elimelech, Menachem ;
Halas, Naomi J. ;
Villagan, Dino .
NATURE NANOTECHNOLOGY, 2018, 13 (08) :634-641
[3]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[4]  
Armstrong D.A., 2014, BIOINORG REACT MECH, V9, P59, DOI DOI 10.1515/IRM-2013-0005
[5]   THE KINETICS AND MECHANISM OF THE DECOMPOSITION OF CAROS ACID .1. [J].
BALL, DL ;
EDWARDS, JO .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1956, 78 (06) :1125-1129
[6]   4-Chlorophenol degradation using ultrasound/peroxymonosulfate/nanoscale zero valent iron: Reusability, identification of degradation intermediates and potential application for real wastewater [J].
Barzegar, Gelavizh ;
Jorfi, Sahand ;
Zarezade, Vahid ;
Khatebasreh, Masoumeh ;
Mehdipour, Fayyaz ;
Ghanbari, Farshid .
CHEMOSPHERE, 2018, 201 :370-379
[7]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[8]   Reaction of SO4.- with Fe2+, Mn2+ and Cu2+ in aqueous solution [J].
Buxton, GV ;
Malone, TN ;
Salmon, GA .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (16) :2893-2897
[9]   Novel magnetic MnO2/MnFe2O4 nanocomposite as a heterogeneous catalyst for activation of peroxymonosulfate (PMS) toward oxidation of organic pollutants [J].
Chen, Gong ;
Zhang, Xinyi ;
Gao, Yingjie ;
Zhu, Guixian ;
Cheng, Qingfeng ;
Cheng, Xiuwen .
SEPARATION AND PURIFICATION TECHNOLOGY, 2019, 213 :456-464
[10]   RATE CONSTANTS FOR HYDROGEN ABSTRACTION REACTIONS OF THE SULFATE RADICAL, SO4- - ALCOHOLS [J].
CLIFTON, CL ;
HUIE, RE .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1989, 21 (08) :677-687