Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

doi:10.1007/s11783-013-0544-x

Front Envir Sci Eng

2014, Vol. 8

Issue (2) : 188-194 https://doi.org/10.1007/s11783-013-0544-x

RESEARCH ARTICLE

Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

Qishi LUO(

)

State Environmental Protection Engineering Center for Urban Soil Contamination Control and Remediation, Shanghai Academy of Environmental Science, Shanghai 200233, China

Download: PDF(283 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

The oxidation of aqueous monochlorobenzene (MCB) solutions using thermally- activated persulfate has been investigated. The influence of reaction temperature on the kinetics of MCB oxidation was examined, and the Arrenhius Equation rate constants at 20°C, 30°C, 40°C, 50°C, and 60°C for MCB oxidation performance were calculated as 0, 0.001, 0.002, 0.015, 0.057 min^-1, which indicates that elevated temperature accelerated the rate. The most efficient molar ratio of persulfate/MCB for MCB oxidation was determined to be 200 to 1 and an increase in the rate constants suggests that the oxidation process proceeded more rapidly with increasing persulfate/MCB molar ratios. In addition, the reactivity of persulfate in contaminated water is partly influenced by the presence of background ions such as Cl^-, HCO3-, SO42-, and NO3-. Importantly, a scavenging effect in rate constant was observed for both Cl^- and CO32- but not for other ions. The effective thermally activated persulfate oxidation of MCB in groundwater from a real contaminated site was achieved using both elevated reaction temperature and increased persulfate/MCB molar ratio.

Keywords persulfate monochlorobenzene advanced oxidation process

Corresponding Author(s): LUO Qishi,Email:luoqs@saes.sh.cn

Issue Date: 01 April 2014

Cite this article:

Qishi LUO. Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate[J]. Front Envir Sci Eng, 2014, 8(2): 188-194.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-013-0544-x
https://academic.hep.com.cn/fese/EN/Y2014/V8/I2/188

Tab.1 Characterisitics of groundwater at the contaminated site

Fig.1 Oxidation of MCB at various temperatures (initial MCB concentration= 100 mg·L, PS/MCB molar ratio= 100/1)

Fig.2 This shows the effect of initial MCB concentration on oxidation performance with temperature at 50°C and PS/MCB molar ratio= 100/1)

Fig.3 This shows the effect of various PS/MCB molar ratios on oxidation performance at 50°C with initial MCB concentration= 100 mg·L

Fig.4 Effect of cations and anions on MCB oxidation performance (temperature= 50°C, initial MCB concentration= 100 mg·L, PS/MCB molar ratio= 60/1): (a) Cl, (b) CO

Fig.5 In situ MCB-contaminated groundwater treatment using thermally excited persulfate: (a) with various temperature ; (b) with various PS/MCB molar ratios

Fig.6 Proposed MCB decomposition pathway

Fig.7 Change of TOC over time

1	Xu Z, Deng S, Yang Y, Zhang T, Cao Q, Huang J, Yu G. Catalytic destruction of pentachlorobenzene in simulated flue gas by a V₂O₅-WO₃/TiO₂ catalyst. Chemosphere , 2012, 87(9): 1032-1038 doi: 10.1016/j.chemosphere.2012.01.004 pmid:22280981
2	Song Y, Wang F, Bian Y, Zhang Y, Jiang X. Chlorobenzenes and organochlorinated pesticides in vegetable soils from an industrial site, China. Journal of Environmental Sciences-China , 2012, 24(3): 362-368 doi: 10.1016/S1001-0742(11)60720-1 pmid:22655347
3	Lee C L, Lee H Y, Tseng K H, Hong P K, Jou C J G.Enhanced dechlorination of chlorobenzene by microwave-induced zero-valent iron: particle effects and activation energy. Environmental Chemistry Letters , 2011, 9(3): 355-359 doi: 10.1007/s10311-010-0286-y
4	Lee C L, Jou C J G, Huang H G. Degradation of chlorobenzene in water using nanoscale Cu coupled with microwave irradiation. Journal of Environmental Engineering , 2010, 136(4): 412-416 doi: 10.1061/(ASCE)EE.1943-7870.0000163
5	Wang K H, Hsieh Y H, Chou M Y, Chang C Y. Photocalytic degradation of 2-chloro and 2-nitrophenol by titanium dioxide suspensions in aqueous solution. Applied Catalysis B: Environmental , 1999, 21(1): 1-8 doi: 10.1016/S0926-3373(98)00116-7
6	Pagano M, Volpe A, Lopez A, Mascolo G, Ciannarella R. Degradation of chlorobenzene by Fenton-like processes using zero-valent iron in the presence of Fe³⁺ and Cu²⁺. Environmental Technology , 2011, 32(1-2): 155-165 doi: 10.1080/09593330.2010.490855 pmid:21473278
7	Hollige C, Schraa G, Stams A J M, Zehnder A J B. Enrichment and properties of an anaerobic mixed culture reductively dechlorinating 1,2,3-trichlorobenzene to 1,3-dichlorobenzene. Applied and Environmental Microbiology , 1992, 58(5): 1636-1644 pmid:1622233
8	Chen X, Christopher A, Jones J P, Bell S G, Guo Q, Xu F, Rao Z, Wong L L. Crystal structure of the F87W/Y96F/V247L mutant of cytochrome P-450cam with 1,3,5-trichlorobenzene bound and further protein engineering for the oxidation of pentachlorobenzene and hexachlorobenzene. The Journal of Biological Chemistry , 2002, 277(40): 37519-37526 doi: 10.1074/jbc.M203762200 pmid:12114516
9	Tsitonaki A, Petri B, Crimi M, Mosb?k H, Siegrist R, Bjerg P. In situ oxidation of contaminated soil and ground water using persulfate. Critical Reviews in Environmental Science and Technology , 2010, 40(1): 55-91 doi: 10.1080/10643380802039303
10	Watts R J, Teel A L. Chemistry of modified Fenton’s reagent (catalysed H₂O₂ propagations-CHP) for in situ soil and ground water remediation. Journal of Environmental Engineering , 2005, 131(4): 612-622 doi: 10.1061/(ASCE)0733-9372(2005)131:4(612)
11	Huang K C, Couttenye R A, Hoag G E. Kinetics of heat-assisted persulfate oxidation of methyl tert-butyl ether (MTBE). Chemosphere , 2002, 49(4): 413-420 doi: 10.1016/S0045-6535(02)00330-2 pmid:12365838
12	Huang K C, Zhao Z, Hoag G E, Dahmani A, Block P A. Degradation of volatile organic compounds with thermally activated persulfate oxidation. Chemosphere , 2005, 61(4): 551-560 doi: 10.1016/j.chemosphere.2005.02.032 pmid:16202809
13	Liang C J, Bruell C J, Marley M C, Sperry K L. Thermally activated persulfate oxidation of trichloroethylene (TCE) and 1,1,1-trichloroethane (TCA) in aqueous systems and soil slurries. Soil and Sediment Contamination , 2003, 12(2): 207-228 doi: 10.1080/713610970
14	Liang C, Wang Z S, Bruell C J. Influence of pH on persulfate oxidation of TCE at ambient temperatures. Chemosphere , 2007, 66(1): 106-113 doi: 10.1016/j.chemosphere.2006.05.026 pmid:16814844
15	Waldemer R H, Tratnyek P G, Johnson R L, Nurmi J T. Oxidation of chlorinated ethenes by heat-activated persulfate: kinetics and products. Environmental Science & Technology , 2007, 41(3): 1010-1015 doi: 10.1021/es062237m pmid:17328217
16	Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants. Environmental Science & Technology , 2004, 38(13): 3705-3712 doi: 10.1021/es035121o pmid:15296324
17	Anipsitakis G P, Dionysiou D D. Transition metal/UV-based advanced oxidation technologies for water decontamination. Applied Catalysis , 2004, 54(3): 155-163 doi: 10.1016/j.apcatb.2004.05.025
18	Liang C, Bruell C J, Marley M C, Sperry K L. Persulfate oxidation for in situ remediation of TCE. I. Activated by ferrous ion with and without a persulfate-thiosulfate redox couple. Chemosphere , 2004, 55(9): 1213-1223 doi: 10.1016/j.chemosphere.2004.01.029 pmid:15081762
19	Liang C, Bruell C J, Marley M C, Sperry K L. Persulfate oxidation for in situ remediation of TCE. II. Activated by chelated ferrous ion. Chemosphere , 2004, 55(9): 1225-1233 doi: 10.1016/j.chemosphere.2004.01.030 pmid:15081763
20	Rastogi A, Al-Abed S R, Dionysiou D D. Sulfate radical-based ferrous peroxymonosulfate oxidative system for PCBs degradation in aqueous and sediment systems. Applied Catalysis B: Environmental , 2009, 85(3-4): 171-179 doi: 10.1016/j.apcatb.2008.07.010
21	Rastogi A, Al-Abed S R, Dionysiou D D. Effect of inorganic, synthetic and naturally occurring chelating agents on Fe(II) mediated advanced oxidation of chlorophenols. Water Research , 2009, 43(3): 684-694 doi: 10.1016/j.watres.2008.10.045 pmid:19038413
22	Kolthoff I M, Medalia A I, Raaen H P. The reaction between ferrous iron and peroxides. IV. Reaction with potassium persulfate. Journal of American Chemical Society , 1951, 73(4): 1733-1739 doi: 10.1021/ja01148a089
23	House D A. Kinetics and mechanism of oxidation by peroxydisulfate. Chemical Reviews , 1962, 62(3): 185-203 doi: 10.1021/cr60217a001
24	Gu X, Lu S, Li L, Qiu Z, Sui Q, Lin K, Luo Q. Oxidation of 1,1,1-trichloroethane stimulated by thermally activated persulfate. Industrial & Engineering Chemistry , 2011, 50(19): 11029-11036 doi: 10.1021/ie201059x
25	Liang C J, Huang C F, Chen Y J. Potential for activated persulfate degradation of BTEX contamination. Water Research , 2008, 42(15): 4091-4100 doi: 10.1016/j.watres.2008.06.022 pmid:18718627
26	Huie R E, Clifton C L, Neta P. Electron transfer reaction and equilibria of the carbonate and sulphate radical anions. IRadiation Physics and Chemistry , 1991, 38(5): 477-481

[1]	Majid Mustafa, Huijiao Wang, Richard H. Lindberg, Jerker Fick, Yujue Wang, Mats Tysklind. Identification of resistant pharmaceuticals in ozonation using QSAR modeling and their fate in electro-peroxone process[J]. Front. Environ. Sci. Eng., 2021, 15(5): 106-.
[2]	Zhifei Ma, Huali Cao, Fengchun Lv, Yu Yang, Chen Chen, Tianxue Yang, Haixin Zheng, Daishe Wu. Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive black 5[J]. Front. Environ. Sci. Eng., 2021, 15(5): 98-.
[3]	Yang Li, Yixin Zhang, Guangshen Xia, Juhong Zhan, Gang Yu, Yujue Wang. Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized water treatment[J]. Front. Environ. Sci. Eng., 2021, 15(1): 1-.
[4]	Yapeng Song, Hui Gong, Jianbing Wang, Fengmin Chang, Kaijun Wang. Enhanced triallyl isocyanurate (TAIC) degradation through application of an O₃/UV process: Performance optimization and degradation pathways[J]. Front. Environ. Sci. Eng., 2020, 14(4): 64-.
[5]	Virender K. Sharma, Xin Yu, Thomas J. McDonald, Chetan Jinadatha, Dionysios D. Dionysiou, Mingbao Feng. Elimination of antibiotic resistance genes and control of horizontal transfer risk by UV-based treatment of drinking water: A mini review[J]. Front. Environ. Sci. Eng., 2019, 13(3): 37-.
[6]	Siyi Lu, Naiyu Wang, Can Wang. Oxidation and biotoxicity assessment of microcystin-LR using different AOPs based on UV, O₃ and H₂O₂[J]. Front. Environ. Sci. Eng., 2018, 12(3): 12-.
[7]	Pan Gao, Yuan Song, Shaoning Wang, Claude Descorme, Shaoxia Yang. Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst in the catalytic wet air oxidation (CWAO) of cationic red GTL under mild reaction conditions[J]. Front. Environ. Sci. Eng., 2018, 12(1): 8-.
[8]	Xiaoxia Ou, Jianfang Yan, Fengjie Zhang, Chunhua Zhang. Accelerated degradation of orange G over a wide pH range in the presence of FeVO₄[J]. Front. Environ. Sci. Eng., 2018, 12(1): 7-.
[9]	Minhui XU,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI. Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic acid[J]. Front. Environ. Sci. Eng., 2016, 10(3): 438-446.
[10]	Wenzhen LI, Yu DING, Qian SUI, Shuguang LU, Zhaofu QIU, Kuangfei LIN. Identification and ecotoxicity assessment of intermediates generated during the degradation of clofibric acid by advanced oxidation processes[J]. Front Envir Sci Eng, 2012, 6(4): 445-454.
[11]	Yuchi LEE, Shanglien LO, Jeff KUO, Chinghong HSIEH. Decomposition of perfluorooctanoic acid by microwave-activated persulfate: Effects of temperature, pH, and chloride ions[J]. Front Envir Sci Eng, 2012, 6(1): 17-25.

Viewed

Full text

Abstract

Cited

Shared

Discussed