Oxidation of 1,1,1-Trichloroethane Stimulated by Thermally Activated Persulfate

被引:142
|
作者
Gu, Xiaogang [1 ]
Lu, Shuguang [1 ]
Li, Lin [1 ]
Qiu, Zhaofu [1 ]
Sui, Qian [1 ]
Lin, Kuangfei [1 ]
Luo, Qishi [2 ]
机构
[1] E China Univ Sci & Technol, Shanghai Key Lab Funct Mat Chem, State Environm Protect Key Lab Environm Risk Asse, Shanghai 200237, Peoples R China
[2] Shanghai Acad Environm Sci, Shanghai 200233, Peoples R China
基金
中国国家自然科学基金;
关键词
CHLORINATED ETHENES; SODIUM PERSULFATE; NITRIC-OXIDE; DEGRADATION; SULFATE; KINETICS; HEAT; TRICHLOROETHYLENE; PEROXYMONOSULFATE; RADICALS;
D O I
10.1021/ie201059x
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
In this study, thermally activated persulfate (PS) to stimulate the oxidation of 1,1,1-trichloroethane (TCA) in groundwater remediation was investigated. The effects of various factors including temperature; initial TCA concentration; PS/TCA molar ratio; solution pH; and common constituents in groundwater such as Cl-, HCO3-, SO42-, and NO3- anions and humic acid (HA) were evaluated. The experimental results showed that TCA can be completely oxidized in 2 h at 50 degrees C with a PS/TCA molar ratio of 100/1, indicating the effectiveness of thermally activated PS oxidation for TCA removal. TCA oxidation was fitted with a pseudo-first-order kinetic model, and the rate constant was found to increase with increasing temperature and PS/TCA molar ratio, but to decrease with increasing initial TCA concentration. In addition, acidic conditions were favorable to TCA removal and elevating, the initial solution pH value (from pH 3 to 11) decreased the TCA degradation rate. Anions Cl- and HCO3- had negative effects on TCA removal, whereas the effects of both SO42- and NO3- were negligible. With 5-10 mg L-1 of HA in solution, an inhibitive effect was observed, indicating that dissolved organic matter consumed some of the oxidant. However, the anticipated effective thermally activated PS oxidation of TCA in groundwater from a real contaminated site was not achieved because of the complex solution matrix. On the other hand, the TCA degradation mechanism derived from GC/MS analytical results confirmed formic acid, dichloromethane, and trichloromethane as the primary intermediates, and therefore, two TCA decomposition pathways were proposed. In conclusion, thermally activated PS oxidation is a highly promising technique for TCA-contaminated groundwater remediation, but more complex constituents in in situ groundwater should be carefully considered for its practical application.
引用
收藏
页码:11029 / 11036
页数:8
相关论文
共 50 条
  • [1] Thermally activated persulfate oxidation of trichloroethylene (TCE) and 1,1,1-trichloroethane (TCA) in aqueous systems and soil slurries
    Liang, CJ
    Bruell, CJ
    Marley, MC
    Sperry, KL
    SOIL & SEDIMENT CONTAMINATION, 2003, 12 (02): : 207 - 228
  • [2] Role of Reactive Oxygen Species for 1,1,1-Trichloroethane Degradation in a Thermally Activated Persulfate System
    Xu, Minhui
    Gu, Xiaogang
    Lu, Shuguang
    Qiu, Zhaofu
    Sui, Qian
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2014, 53 (03) : 1056 - 1063
  • [3] KINETICS AND MECHANISM FOR THE OXIDATION OF 1,1,1-TRICHLOROETHANE
    NELSON, L
    SHANAHAN, I
    SIDEBOTTOM, HW
    TREACY, J
    NIELSEN, OJ
    INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1990, 22 (06) : 577 - 590
  • [4] 1,1,1-TRICHLOROETHANE
    不详
    AMERICAN INDUSTRIAL HYGIENE ASSOCIATION JOURNAL, 1964, 25 (06): : 585 - &
  • [5] 1,1,1-TRICHLOROETHANE
    BRETHERICK, L
    CHEMICAL & ENGINEERING NEWS, 1988, 66 (50) : 2 - 2
  • [6] Removal of 1,1,1-trichloroethane from aqueous solution by a sono-activated persulfate process
    Li, Bingzhi
    Li, Lin
    Lin, Kuangfei
    Zhang, Wei
    Lu, Shuguang
    Luo, Qishi
    ULTRASONICS SONOCHEMISTRY, 2013, 20 (03) : 855 - 863
  • [7] PHOSGENE FORMATION FROM 1,1,1-TRICHLOROETHANE OXIDATION
    THOMSON, MJ
    HIGGINS, BS
    LUCAS, D
    KOSHLAND, CP
    SAWYER, RF
    COMBUSTION AND FLAME, 1994, 98 (04) : 350 - 360
  • [8] 1,1,1-TRICHLOROETHANE AND THE LIVER
    GUZELIAN, PS
    ARCHIVES OF INTERNAL MEDICINE, 1991, 151 (11) : 2321 - 2322
  • [9] PHOTOOXIDATION OF 1,1,1-TRICHLOROETHANE
    SHANAHAN, I
    SIDEBOTTOM, HW
    PROCEEDINGS OF THE ROYAL IRISH ACADEMY SECTION B-BIOLOGICAL GEOLOGICAL AND CHEMICAL SCIENCE, 1989, 89 (6-52) : 363 - 367
  • [10] THE PYROLYSIS OF 1,1,1-TRICHLOROETHANE
    BARTON, DHR
    ONYON, PF
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1950, 72 (02) : 988 - 995