Mechanism of carbon tetrachloride reduction in ferrous ion activated calcium peroxide system in the presence of methanol

Ping Tang; Wenchao Jiang; Shuguang Lyu; Mark L. Brusseau; Yunfei Xue; Zhaofu Qiu; Qian Sui

doi:10.1016/j.cej.2019.01.034

Mechanism of carbon tetrachloride reduction in ferrous ion activated calcium peroxide system in the presence of methanol

Ping Tang
, Wenchao Jiang
, Shuguang Lyu
, Mark L. Brusseau
, Yunfei Xue
, Zhaofu Qiu
, Qian Sui

Research output: Contribution to journal › Article › peer-review

43 Scopus citations

Abstract

This study investigated the reductive initiation for the depletion of highly oxidized/perhalogenated pollutants, specifically the degradation of carbon tetrachloride (CT) was induced by adding methanol (MeOH) into a ferrous ion (Fe(II)) activated calcium peroxide (CaO₂) system. The results indicated that CT could be completely degraded within 20 min at CaO₂/Fe(II)/MeOH/CT molar ratio of 30/40/10/1 in this system. Scavenging tests suggested that both superoxide radical anion (O₂^[rad]−) and carbon dioxide radical anion (CO₂^[rad]−) were predominant reactive species responsible for CT destruction. Hydroxymethyl radicals (^[rad]CH₂OH), an intermediate in the transformation of MeOH, could also initiate CT degradation by reducing C–Cl bond. GC/MS analysis identified CHCl₃, C₂Cl₄, and C₂Cl₆ as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation was proposed accordingly. In addition, the impact of solution matrix and initial solution pH were evaluated, and the results showed that Cl⁻, NO₃⁻, and HCO₃⁻ had adverse effects on CT degradation. Moreover, the alkaline condition was unfavorable to CT depletion. In conclusion, the results obtained in the actual groundwater tests encouragingly demonstrated that the CaO₂/Fe(II)/MeOH process is a highly promising technique for the remediation of CT-contaminated groundwater.

Original language	English (US)
Pages (from-to)	243-250
Number of pages	8
Journal	Chemical Engineering Journal
Volume	362
DOIs	https://doi.org/10.1016/j.cej.2019.01.034
State	Published - Apr 15 2019

Keywords

Calcium peroxide
Carbon tetrachloride
Groundwater remediation
Methanol
Reductive radicals

ASJC Scopus subject areas

Environmental Chemistry
General Chemistry
General Chemical Engineering
Industrial and Manufacturing Engineering

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10.1016/j.cej.2019.01.034

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@article{cc03c1086785430f8be9fb24a3c5fab6,

title = "Mechanism of carbon tetrachloride reduction in ferrous ion activated calcium peroxide system in the presence of methanol",

abstract = "This study investigated the reductive initiation for the depletion of highly oxidized/perhalogenated pollutants, specifically the degradation of carbon tetrachloride (CT) was induced by adding methanol (MeOH) into a ferrous ion (Fe(II)) activated calcium peroxide (CaO2) system. The results indicated that CT could be completely degraded within 20 min at CaO2/Fe(II)/MeOH/CT molar ratio of 30/40/10/1 in this system. Scavenging tests suggested that both superoxide radical anion (O2[rad]−) and carbon dioxide radical anion (CO2[rad]−) were predominant reactive species responsible for CT destruction. Hydroxymethyl radicals ([rad]CH2OH), an intermediate in the transformation of MeOH, could also initiate CT degradation by reducing C–Cl bond. GC/MS analysis identified CHCl3, C2Cl4, and C2Cl6 as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation was proposed accordingly. In addition, the impact of solution matrix and initial solution pH were evaluated, and the results showed that Cl−, NO3−, and HCO3− had adverse effects on CT degradation. Moreover, the alkaline condition was unfavorable to CT depletion. In conclusion, the results obtained in the actual groundwater tests encouragingly demonstrated that the CaO2/Fe(II)/MeOH process is a highly promising technique for the remediation of CT-contaminated groundwater.",

keywords = "Calcium peroxide, Carbon tetrachloride, Groundwater remediation, Methanol, Reductive radicals",

author = "Ping Tang and Wenchao Jiang and Shuguang Lyu and Brusseau, \{Mark L.\} and Yunfei Xue and Zhaofu Qiu and Qian Sui",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

year = "2019",

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doi = "10.1016/j.cej.2019.01.034",

language = "English (US)",

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T1 - Mechanism of carbon tetrachloride reduction in ferrous ion activated calcium peroxide system in the presence of methanol

AU - Tang, Ping

AU - Jiang, Wenchao

AU - Lyu, Shuguang

AU - Brusseau, Mark L.

AU - Xue, Yunfei

AU - Qiu, Zhaofu

AU - Sui, Qian

PY - 2019/4/15

Y1 - 2019/4/15

N2 - This study investigated the reductive initiation for the depletion of highly oxidized/perhalogenated pollutants, specifically the degradation of carbon tetrachloride (CT) was induced by adding methanol (MeOH) into a ferrous ion (Fe(II)) activated calcium peroxide (CaO2) system. The results indicated that CT could be completely degraded within 20 min at CaO2/Fe(II)/MeOH/CT molar ratio of 30/40/10/1 in this system. Scavenging tests suggested that both superoxide radical anion (O2[rad]−) and carbon dioxide radical anion (CO2[rad]−) were predominant reactive species responsible for CT destruction. Hydroxymethyl radicals ([rad]CH2OH), an intermediate in the transformation of MeOH, could also initiate CT degradation by reducing C–Cl bond. GC/MS analysis identified CHCl3, C2Cl4, and C2Cl6 as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation was proposed accordingly. In addition, the impact of solution matrix and initial solution pH were evaluated, and the results showed that Cl−, NO3−, and HCO3− had adverse effects on CT degradation. Moreover, the alkaline condition was unfavorable to CT depletion. In conclusion, the results obtained in the actual groundwater tests encouragingly demonstrated that the CaO2/Fe(II)/MeOH process is a highly promising technique for the remediation of CT-contaminated groundwater.

AB - This study investigated the reductive initiation for the depletion of highly oxidized/perhalogenated pollutants, specifically the degradation of carbon tetrachloride (CT) was induced by adding methanol (MeOH) into a ferrous ion (Fe(II)) activated calcium peroxide (CaO2) system. The results indicated that CT could be completely degraded within 20 min at CaO2/Fe(II)/MeOH/CT molar ratio of 30/40/10/1 in this system. Scavenging tests suggested that both superoxide radical anion (O2[rad]−) and carbon dioxide radical anion (CO2[rad]−) were predominant reactive species responsible for CT destruction. Hydroxymethyl radicals ([rad]CH2OH), an intermediate in the transformation of MeOH, could also initiate CT degradation by reducing C–Cl bond. GC/MS analysis identified CHCl3, C2Cl4, and C2Cl6 as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation was proposed accordingly. In addition, the impact of solution matrix and initial solution pH were evaluated, and the results showed that Cl−, NO3−, and HCO3− had adverse effects on CT degradation. Moreover, the alkaline condition was unfavorable to CT depletion. In conclusion, the results obtained in the actual groundwater tests encouragingly demonstrated that the CaO2/Fe(II)/MeOH process is a highly promising technique for the remediation of CT-contaminated groundwater.

KW - Calcium peroxide

KW - Carbon tetrachloride

KW - Groundwater remediation

KW - Methanol

KW - Reductive radicals

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JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

ER -

Mechanism of carbon tetrachloride reduction in ferrous ion activated calcium peroxide system in the presence of methanol

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