Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic acid

doi:10.1007/s11783-015-0798-6

Front. Environ. Sci. Eng.

2016, Vol. 10

Issue (3) : 438-446 https://doi.org/10.1007/s11783-015-0798-6

RESEARCH ARTICLE

Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic acid

Minhui XU,Xiaogang GU,Shuguang LU(

),Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI

State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China

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Abstract

The thermally activated persulfate (PS) degradation of carbon tetrachloride (CT) in the presence of formic acid (FA) was investigated. The results indicated that CT degradation followed a zero order kinetic model, and CO2-· was responsible for the degradation of CT confirmed by radical scavenger tests. CT degradation rate increased with increasing PS or FA dosage, and the initial CT had no effect on CT degradation rate. However, the initial solution pH had effect on the degradation of CT, and the best CT degradation occurred at initial pH 6. Cl^- had a negative effect on CT degradation, and high concentration of Cl^- displayed much strong inhibition. Ten mmol·L^-1HCO3- promoted CT degradation, while 100 mmol·L^-1NO3- inhibited the degradation of CT, but SO42- promoted CT degradation in the presence of FA. The measured Cl^- concentration released into solution along with CT degradation was 75.8% of the total theoretical dechlorination yield, but no chlorinated intermediates were detected. The split of C-Cl was proposed as the possible reaction pathways in CT degradation. In conclusion, this study strongly demonstrated that the thermally activated PS system in the presence of FA is a promising technique in in situ chemical oxidation (ISCO) remediation for CT contaminated site.

Keywords persulfate carbon tetrachloride thermal activation formic acid carbon dioxide radical anion

Corresponding Author(s): Shuguang LU

Online First Date: 18 June 2015 Issue Date: 05 April 2016

Cite this article:

Minhui XU,Xiaogang GU,Shuguang LU, et al. 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.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-015-0798-6
https://academic.hep.com.cn/fese/EN/Y2016/V10/I3/438

Fig.1 CT degradation in the thermally activated PS system in the presence of FA (50°C, [CT]₀ = 10 μmol·L^-1, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

Fig.2 Effect of scavenger on CT degradation (50°C, [CT]₀ = 10 μmol·L^-1, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

Fig.3 Effect of dosages of PS and FA, and initial CT concentration on CT degradation. (a) PS (50°C, [CT]₀ = 10 μmol·L^-1, [FA] = 30 mmol·L^-1); (b) FA (50°C, [CT]₀ = 10 μmol·L^-1, [PS] = 20 mmol·L^-1); (c) CT (50°C, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

Fig.4 Effect of initial solution pH on CT degradation. (a) Cl^-; (b) H C O 3 - ; (c) N O 3 - ; (d) S O 4 2 - . (50°C, [CT]₀ = 10 μmol·L^-1, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

Tab.1 pH variation along with reaction at different initial solution pH conditions

Fig.5 Effect of solution matrix on CT degradation (50°C, [CT]₀ = 10 μmol·L^-1, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

Fig.6 Performance of CT degradation versus PS decomposition and Cl^- release. (50°C, [CT]₀ = 0.1 mmol·L^-1, [PS] = 20 mmol·L^-1, [FA] = 30 mmol·L^-1)

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