Oxidation of trichloroethylene by the hydroxyl radicals produced from oxygenation of reduced nontronite

被引:96
作者
Liu, Xixiang [1 ]
Yuan, Songhu [1 ]
Tong, Man [1 ]
Liu, Deng [1 ]
机构
[1] China Univ Geosci, State Key Lab Biogeol & Environm Geol, 388 Lumo Rd, Wuhan 430074, Peoples R China
关键词
Iron-bearing silicate minerals; Oxygenation; Hydroxyl radicals; Chlorinated hydrocarbons; Oxidative transformation; ABIOTIC REDUCTIVE DECHLORINATION; BEARING SOIL MINERALS; CHLORINATED ETHYLENES; CIS-DICHLOROETHYLENE; CARBON-TETRACHLORIDE; FE(II) OXIDATION; CLAY-MINERALS; IRON; FE; TRANSFORMATION;
D O I
10.1016/j.watres.2017.02.012
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Reduction by Fe(II)-bearing silicate minerals has been proposed as an important mechanism for the attenuation of chlorinated hydrocarbons (CHCs) in anoxic subsurfaces. The redox condition of subsurface often changes from anoxic to oxic due to natural processes and human activities, but little is known about the transformation of CHCs induced by Fe(II)-bearing silicate minerals under oxic conditions. This study reveals that trichloroethylene (TCE) can be efficiently oxidized during the oxygenation of reduced nontronite at pH 7.5, whereas the reduction was negligible under anoxic conditions. The maximum oxidation of TCE (initially 1 mg/L) attained 89.6% for 3 h oxygenation of 2 g/L nontronite with 50% reduction extent. TCE oxidation is attributed to the strongly oxidizing hydroxyl radicals (*OH) produced by the oxygenation of Fe(II) in nontronite. Fe(II) on the edges is preferentially oxygenated for "OH production, and the interior Fe(II) serves as an electron pool to regenerate the Fe(II) on the edges. Oxidation of TCE could be sustainable through chemically or biologically reducing the oxidized silicate minerals. Our findings present a new mechanism for the transformation of CHCs and other redox-active substances in the redox-fluctuation environments. (C) 2017 Elsevier Ltd. All rights reserved.
引用
收藏
页码:72 / 79
页数:8
相关论文
共 54 条
[1]   Improvements to the quantitative assay of nonrefractory minerals for Fe(II) and total Fe using 1,10-phenanthroline [J].
Amonette, JE ;
Templeton, JC .
CLAYS AND CLAY MINERALS, 1998, 46 (01) :51-62
[2]   Dechlorination of carbon tetrachloride by Fe(II) associated with goethite [J].
Amonette, JE ;
Workman, DJ ;
Kennedy, DW ;
Fruchter, JS ;
Gorby, YA .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (21) :4606-4613
[3]   Characterization of a redox-modified clay mineral with respect to its suitability as a barrier in radioactive waste confinement [J].
Anastacio, Alexandre S. ;
Aouad, Amina ;
Sellin, Patrik ;
Fabris, Jose Domingos ;
Bergaya, Faiza ;
Stucki, Joseph W. .
APPLIED CLAY SCIENCE, 2008, 39 (3-4) :172-179
[4]   Cycling of trace metals (Mn, Fe, Mo, U, V, Cr) in deep pore waters of intertidal flat sediments [J].
Beck, Melanie ;
Dellwig, Laf ;
Schnetger, Bernhard ;
Brumsack, Hans-Juergen .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2008, 72 (12) :2822-2840
[5]   Reduction and immobilization of hexavalent chromium by microbially reduced Fe-bearing clay minerals [J].
Bishop, Michael E. ;
Glasser, Paul ;
Dong, Hailiang ;
Arey, Bruce ;
Kovarik, Libor .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2014, 133 :186-203
[6]   Bioreduction of Fe-bearing clay minerals and their reactivity toward pertechnetate (Tc-99) [J].
Bishop, Michael E. ;
Dong, Hailiang ;
Kukkadapu, Ravi K. ;
Liu, Chongxuan ;
Edelmann, Richard E. .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2011, 75 (18) :5229-5246
[7]   Dechlorinating chloroacetanilide herbicides by dithionite-treated aquifer sediment and surface soil [J].
Boparai, HK ;
Shea, PJ ;
Comfort, SD ;
Snow, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (09) :3043-3049
[8]   Reductive dechlorination of tetrachloroethylene and trichloroethylene catalyzed by vitamin B-12 in homogeneous and heterogeneous systems [J].
Burris, DR ;
Delcomyn, CA ;
Smith, MH ;
Roberts, AL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1996, 30 (10) :3047-3052
[9]   Kinetics of the transformation of trichloroethylene and tetrachloroethylene by iron sulfide [J].
Butler, EC ;
Hayes, KF .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (12) :2021-2027
[10]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886