EVO(乳化油)-Mg(OH)_2双功能缓释剂强化修复三氯乙烯污染地下水
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摘要
氯代烃污染地下水在外加有机质(电子供体)进行强化还原脱氯时,存在有机质消耗快、pH持续降低等影响脱氯效率的问题。利用乳化油(EVO)与胶体氢氧化镁复配的方法,制备了一种兼具电子供体缓释性和OH-缓释性的双功能缓释剂EVO-Mg(OH)_2;成功制备了不同EVO∶Mg(OH)_2配比的EVO-Mg(OH)_2试剂,并对其稳定性、分散性及粒径分布进行了研究;向模拟砂柱中注入不同体积的EVO-Mg(OH)_2,考察试剂的迁移性能以及试剂注入对三氯乙烯(TCE)迁移的影响;开展了EVO-Mg(OH)_2强化TCE还原脱氯摇瓶实验,考察了该试剂对脱氯效果的影响。结果表明:不同EVO∶Mg(OH)_2配比的试剂稳定性及分散性良好,粒径无明显差异;EVO-Mg(OH)_2可以有效地在多孔介质中迁移并实现部分滞留;注入量对EVO-Mg(OH)_2的迁移性有一定的影响;EVO-Mg(OH)_2可以促进TCE溶解和迁移从而减小EVO-Mg(OH)_2和TCE之间的传质阻力;EVO-Mg(OH)_2能够实现电子供体及OH-的双重缓释,有效促进脱氯微生物的生长,提高TCE的降解速率(k=0.128 d-1),同时抑制pH的降低(pH=7.5)。
Reductive dechlorination can be enhanced by the addition of organic substrate(as electron donor) to the chlorinated organic compound contaminated groundwater. However, the dechlorination efficiency can be limited by the rapid consumption of substrates and continuous decline in pH. In this study, the emulsified vegetable oil(EVO) combined with colloidal Mg(OH)_2 was used to prepare a bifunctional sustained-release agent of EVO-Mg(OH)_2, which could slowly release electrons and OH-. And the EVO-Mg(OH)_2 agents with different EVO∶Mg(OH)_2 ratios were successfully prepared and their stability, dispersibility and particle size distribution were studied. Then different volumes of EVO-Mg(OH)_2 were injected into simulated sand columns to evaluate the migration properties of EVO-Mg(OH)_2, and the influence of EVO-Mg(OH)_2 injection on the migration of TCE.Flask experiments on enhanced TCE reduction were conducted to investigate the TCE dechlorination efficiency in the presence of EVO-Mg(OH)_2. The results showed that the EVO-Mg(OH)_2 with different EVO∶Mg(OH)_2 ratios had a good stability and dispersibility with no significant difference in particle size. EVO-Mg(OH)_2 could effectively migrate and partially retain in the porous media. The injection volumes had an obvious effect on the migration of EVO-Mg(OH)_2. In addition, the injection of EVO-Mg(OH)_2 significantly enhanced the dissolution and migration of TCE, and reduce the mass transfer resistance between EVO-Mg(OH)_2 and TCE. The addition of EVO-Mg(OH)_2 could achieve double sustained release of electron donor and OH-, and effectively facilitate the growth of dechlorinating bacteria to increase the dechlorination rate of TCE(k=0.128 d-1), and inhibit the decline of pH(pH=7.5).
Reductive dechlorination can be enhanced by the addition of organic substrate(as electron donor) to the chlorinated organic compound contaminated groundwater. However, the dechlorination efficiency can be limited by the rapid consumption of substrates and continuous decline in pH. In this study, the emulsified vegetable oil(EVO) combined with colloidal Mg(OH)_2 was used to prepare a bifunctional sustained-release agent of EVO-Mg(OH)_2, which could slowly release electrons and OH-. And the EVO-Mg(OH)_2 agents with different EVO∶Mg(OH)_2 ratios were successfully prepared and their stability, dispersibility and particle size distribution were studied. Then different volumes of EVO-Mg(OH)_2 were injected into simulated sand columns to evaluate the migration properties of EVO-Mg(OH)_2, and the influence of EVO-Mg(OH)_2 injection on the migration of TCE.Flask experiments on enhanced TCE reduction were conducted to investigate the TCE dechlorination efficiency in the presence of EVO-Mg(OH)_2. The results showed that the EVO-Mg(OH)_2 with different EVO∶Mg(OH)_2 ratios had a good stability and dispersibility with no significant difference in particle size. EVO-Mg(OH)_2 could effectively migrate and partially retain in the porous media. The injection volumes had an obvious effect on the migration of EVO-Mg(OH)_2. In addition, the injection of EVO-Mg(OH)_2 significantly enhanced the dissolution and migration of TCE, and reduce the mass transfer resistance between EVO-Mg(OH)_2 and TCE. The addition of EVO-Mg(OH)_2 could achieve double sustained release of electron donor and OH-, and effectively facilitate the growth of dechlorinating bacteria to increase the dechlorination rate of TCE(k=0.128 d-1), and inhibit the decline of pH(pH=7.5).
引文
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[11] PHILIPS J, MAES N, SPRINGAEL D, et al. Acidification due to microbial dechlorination near a trichloroethene DNAPL is overcome with pH buffer or formate as electron donor:Experimental demonstration in diffusion-cells[J]. Journal of Contami?nant Hydrology, 2013, 147(2):25-33.
[12] HIORTDAHL K M, BORDEN R C. Enhanced reductive dechlorination of tetrachloroethene dense nonaqueous phase liquid with EVO and Mg(OH)2[J]. Environmental Science&Technology, 2014, 48(1):624-631.
[13] PISHTSHEV A, KARAZHANOV S Z, KLOPOV M. Materials properties of magnesium and calcium hydroxides from firstprinciples calculations[J]. Computational Materials Science, 2014, 95(1/2/3/4):693-705.
[14] KAMEDA T, TAKEUCHI H, YOSHIOKA T. Preparation of organic acid anion-modified magnesium hydroxides by coprecipi?tation:A novel material for the uptake of heavy metal ions from aqueous solutions[J]. Journal of Physics&Chemistry of Sol?ids, 2009, 70(7):1104-1108.
[15] DONG J, YU J, BAO Q. Simulated reactive zone with emulsified vegetable oil for the long-term remediation of Cr(VI)-contam?inated aquifer:Dynamic evolution of geological parameters and groundwater microbial community[J]. Environmental Science and Pollution Research, 2018, 25(34):34392-34402.
[16]沈丽,王益民,李淑民.复合生物柴油乳化油的制备及其稳定性研究[J].科学技术与工程, 2008, 8(13):3601-3602.
[17] AULENTA F, MAJONE M, TANDOI V. Enhanced anaerobic bioremediation of chlorinated solvents:environmental factors influencing microbial activity and their relevance under field conditions[J]. Journal of Chemical Technology&Biotechnology,2010, 81(9):1463-1474.
[18] GABITTO J, TSOURIS C. Surface transport processes in charged porous media[J]. Colloid Interface Science, 2017, 498:91-104.
[19] MCCARTY P L, CHU M Y, KITANIDIS P K. Electron donor and pH relationships for biologically enhanced dissolution of chlorinated solvent DNAPL in groundwater[J]. European Journal of Soil Biology, 2007, 43(5/6):276-282.
[20] DONG J, LI B, BAO Q. In situ reactive zone with modified Mg(OH)2for remediation of heavy metal polluted groundwater:Im?mobilization and interaction of Cr(III), Pb(II)and Cd(II)[J]. Journal of Contaminant Hydrology, 2017, 199:50-57.
[21] LI B, WEN C, DONG J. Study on the stability, transport behavior and OH-release properties of colloidal Mg(OH)2[J]. Col?loids&Surfaces A:Physicochemical&Engineering Aspects, 2018, 549(1):105-111.
[22]陈星欣,苏世灼,张清林.多孔介质中反复注入颗粒迁移特性试验[J].水利水电科技进展, 2017, 37(5):64-68.
[23]刘雪松,蔡五田,李胜涛.土壤与地下水中DNAPL的污染机理与调查技术[J].油气田环境保护, 2011, 21(6):37-39.
[2] AHMAD A, GU X, LI L, et al. Efficient degradation of trichloroethylene in water using persulfate activated by reduced gra?phene oxide-iron nanocomposite[J]. Environmental Science&Pollution Research International, 2015, 22(22):17876-17885.
[3] WANG S K. In situ chemical oxidation of TCE-contaminated groundwater using slow permanganate-releasing material[J].Tetrahedron Letters, 2011, 16(27):2249-2252.
[4] HUG L A, BEIKO R G, ROWE A R, et al. Comparative metagenomics of three Dehalococcoides-containing enrichment cul?tures:The role of the non-dechlorinating community[J]. BMC Genomics, 2012, 13(1):327.
[5]李海军.三氯乙烯污染地下水厌氧生物修复研究[D].长春:吉林大学, 2016.
[6] PANT P, PANT S. A review:Advances in microbial remediation of trichloroethylene(TCE)[J]. Journal of Environmental Sci?ence, 2010, 22(1):116-126.
[7] AZIZIAN M F, MARSHALL I P G, BEHRENS S, et al. Comparison of lactate, formate, and propionate as hydrogen donors for the reductive dehalogenation of trichloroethene in a continuous-flow column[J]. Journal of Contaminant Hydrology, 2010,113(1):77-92.
[8] LIANG S H, KUO Y C, CHEN S H, et al. Development of a slow polycolloid-releasing substrate(SPRS)biobarrier to remedi?ate TCE-contaminated aquifers[J]. Journal of Hazardous Materials, 2013, 254-255(1):107-115.
[9] LUTES C C, LILES D S, SUTHERSAN S S, et al. Comment on“Comparison between donor substrates for biologically en?hanced tetrachloroethene DNAPL dissolution”[J]. Environmental Science&Technology, 2003, 36(15):3400-3404.
[10] HARKNESS M, FISHER A. Use of emulsified vegetable oil to support bioremediation of TCE DNAPL in soil columns[J].Journal of Contaminant Hydrology, 2013, 151(5):16-33.
[11] PHILIPS J, MAES N, SPRINGAEL D, et al. Acidification due to microbial dechlorination near a trichloroethene DNAPL is overcome with pH buffer or formate as electron donor:Experimental demonstration in diffusion-cells[J]. Journal of Contami?nant Hydrology, 2013, 147(2):25-33.
[12] HIORTDAHL K M, BORDEN R C. Enhanced reductive dechlorination of tetrachloroethene dense nonaqueous phase liquid with EVO and Mg(OH)2[J]. Environmental Science&Technology, 2014, 48(1):624-631.
[13] PISHTSHEV A, KARAZHANOV S Z, KLOPOV M. Materials properties of magnesium and calcium hydroxides from firstprinciples calculations[J]. Computational Materials Science, 2014, 95(1/2/3/4):693-705.
[14] KAMEDA T, TAKEUCHI H, YOSHIOKA T. Preparation of organic acid anion-modified magnesium hydroxides by coprecipi?tation:A novel material for the uptake of heavy metal ions from aqueous solutions[J]. Journal of Physics&Chemistry of Sol?ids, 2009, 70(7):1104-1108.
[15] DONG J, YU J, BAO Q. Simulated reactive zone with emulsified vegetable oil for the long-term remediation of Cr(VI)-contam?inated aquifer:Dynamic evolution of geological parameters and groundwater microbial community[J]. Environmental Science and Pollution Research, 2018, 25(34):34392-34402.
[16]沈丽,王益民,李淑民.复合生物柴油乳化油的制备及其稳定性研究[J].科学技术与工程, 2008, 8(13):3601-3602.
[17] AULENTA F, MAJONE M, TANDOI V. Enhanced anaerobic bioremediation of chlorinated solvents:environmental factors influencing microbial activity and their relevance under field conditions[J]. Journal of Chemical Technology&Biotechnology,2010, 81(9):1463-1474.
[18] GABITTO J, TSOURIS C. Surface transport processes in charged porous media[J]. Colloid Interface Science, 2017, 498:91-104.
[19] MCCARTY P L, CHU M Y, KITANIDIS P K. Electron donor and pH relationships for biologically enhanced dissolution of chlorinated solvent DNAPL in groundwater[J]. European Journal of Soil Biology, 2007, 43(5/6):276-282.
[20] DONG J, LI B, BAO Q. In situ reactive zone with modified Mg(OH)2for remediation of heavy metal polluted groundwater:Im?mobilization and interaction of Cr(III), Pb(II)and Cd(II)[J]. Journal of Contaminant Hydrology, 2017, 199:50-57.
[21] LI B, WEN C, DONG J. Study on the stability, transport behavior and OH-release properties of colloidal Mg(OH)2[J]. Col?loids&Surfaces A:Physicochemical&Engineering Aspects, 2018, 549(1):105-111.
[22]陈星欣,苏世灼,张清林.多孔介质中反复注入颗粒迁移特性试验[J].水利水电科技进展, 2017, 37(5):64-68.
[23]刘雪松,蔡五田,李胜涛.土壤与地下水中DNAPL的污染机理与调查技术[J].油气田环境保护, 2011, 21(6):37-39.