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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2020, Vol. 14 Issue (2) : 18     https://doi.org/10.1007/s11783-019-1197-1
RESEARCH ARTICLE
Enhanced carbon tetrachloride degradation by hydroxylamine in ferrous ion activated calcium peroxide in the presence of formic acid
Wenchao Jiang1,2, Ping Tang1, Zhen Liu2, Huan He2, Qian Sui1, Shuguang Lyu1()
1. State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China
2. Environmental Engineering and Science Program, Department of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221-0071, USA
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Abstract

• Complete CT degradation was achieved by employing HA to CP/Fe(II)/FA process.

• Quantitative detection of Fe(II) regeneration and HO• production was investigated.

• Benzoic acid outcompeted FA for the reaction with HO•.

• CO2 was the dominant reductive radical for CT removal.

• Effects of solution matrix on CT removal were conducted.

Hydroxyl radicals (HO•) show low reactivity with perchlorinated hydrocarbons, such as carbon tetrachloride (CT), in conventional Fenton reactions, therefore, the generation of reductive radicals has attracted increasing attention. This study investigated the enhancement of CT degradation by the synergistic effects of hydroxylamine (HA) and formic acid (FA) (initial [CT] = 0.13 mmol/L) in a Fe(II) activated calcium peroxide (CP) Fenton process. CT degradation increased from 56.6% to 99.9% with the addition of 0.78 mmol/L HA to the CP/Fe(II)/FA/CT process in a molar ratio of 12/6/12/1. The results also showed that the presence of HA enhanced the regeneration of Fe(II) from Fe(III), and the production of HO• increased one-fold when employing benzoic acid as the HO• probe. Additionally, FA slightly improves the production of HO•. A study of the mechanism confirmed that the carbon dioxide radical (CO2), a strong reductant generated by the reaction between FA and HO•, was the dominant radical responsible for CT degradation. Almost complete CT dechlorination was achieved in the process. The presence of humic acid and chloride ion slightly decreased CT removal, while high doses of bicarbonate and high pH inhibited CT degradation. This study helps us to better understand the synergistic roles of FA and HA for HO• and CO2 generation and the removal of perchlorinated hydrocarbons in modified Fenton systems.

Keywords Calcium peroxide      Hydroxylamine      Modified Fenton      Reactive oxygen species      Perchlorinated hydrocarbon     
Corresponding Author(s): Shuguang Lyu   
Issue Date: 17 December 2019
 Cite this article:   
Wenchao Jiang,Ping Tang,Zhen Liu, et al. Enhanced carbon tetrachloride degradation by hydroxylamine in ferrous ion activated calcium peroxide in the presence of formic acid[J]. Front. Environ. Sci. Eng., 2020, 14(2): 18.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-019-1197-1
http://journal.hep.com.cn/fese/EN/Y2020/V14/I2/18
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Wenchao Jiang
Ping Tang
Zhen Liu
Huan He
Qian Sui
Shuguang Lyu
CP (mmol/L) Fe(II) (mmol/L) FA (mmol/L) HA (mmol/L) Initial pH Final pH
1.56 0.78 0 0 5.27 6.82
1.56 0.78 1.56 0 3.65 5.76
1.56 0.78 0 0.78 4.69 6.25
1.56 0.78 1.56 0.39 3.52 5.65
1.56 0.78 1.56 0.78 3.50 5.69
1.56 0.78 1.56 1.56 3.44 5.62
1.56 0.78 1.56 2.34 3.37 5.56
1.56 0.78 0.78 0.78 4.26 6.35
1.56 0.78 3.12 0.78 3.28 5.62
1.56 0.78 7.80 0.78 3.01 5.36
1.56 0.78 15.6 0.78 2.76 4.96
Tab.1  pH variations under various experimental conditions ([CT]0 = 0.13 mmol/L)
Fig.1  Degradation of CT in various processes (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Experimental conditions Electron donor CT removal Ref.
[CT]0 = 100 mg/L; [persulfate] = 20 g/L; [NaOH] = 26 g/L; [MeOH] = 10 g/L O2 >99% (20 h) Dominguez et al. (2019)
[CT]0 = 0.5 mmol/L; [H2O2] = 590 mmol/L; [Iron(III)] = 1 mmol/L; O2; HO2 90% (120 min) Teel and Watts (2002)
[CT]0 = 1 mmol/L; [KO2] = 2 mol/L; [acetone] = 1 mol/L O2 80% (120 min) Smith et al. (2004)
50°C; [CT]0 = 0.01 mmol/L; [persulfate] = 20 mmol/L; [FA] = 30 mmol/L CO2 >99% (180 min) Xu et al. (2016)
UV; [CT]0 = 0.15 mmol/L; [persulfate] = 1.5 mmol/L; [FA] = 2.25 mmol/L CO2 >99% (25 min) Gu et al. (2017)
UVC; [CT]0 = 1.2–1.6 mmol/L; [H2O2] = 0.049 mol/L; [Methanol] = 0.011 mmol/L •CH2OH >99% (60 min) Gonzalez et al. (2007)
[CT]0 = 0.13 mmol/L; [CP] = 1.56 mmol/L; [Iron(II)] = 1.56 mmol/L; [FA] = 1.56 mmol/L CO2 88.9% (15 min) Jiang et al. (2018a)
[CT]0 = 0.13 mmol/L; [CP] = 1.56 mmol/L; [Iron(II)] = 1.56 mmol/L; [FA] = 1.56 mmol/L; [citric acid] = 1.56 mmol/L CO2 95.1% (20 min) Jiang et al. (2019)
Tab.2  CT degradation in some representative advanced oxidation processes
Fig.2  Effect of HA concentration on CT degradation in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.3  Effects of HA on (a) Fe(II) and (b) HO• concentrations in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [BA]0 = 10 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.4  Effect of FA on HO• concentration in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [BA]0 = 1.56 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = 1.56 mmol/L, 25°C).
Fig.5  Effects of different scavengers on CT degradation in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.6  Release of Cl from CT in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.7  CT removal under different initial pH (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.8  Effect of humic acid concentrations on CT degradation in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
Fig.9  Effects of (a) Cl, (b) NO3, (c) SO42 and (d) HCO3 on CT degradation in the CP/Fe(II)/FA/HA process (Conditions: [CT]0 = 0.13 mmol/L, [Fe(II)]0 = [HA]0 = 0.78 mmol/L, [CP]0 = [FA]0 = 1.56 mmol/L, 25°C).
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