EFFECTS OF ETHANOL ON REMOVAL OF BTEX FROM GASOLINE BY PERSULFATE IN LIMESTONE AQUEOUS MEDIA
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摘要: 随着乙醇汽油的推广应用,其污染岩溶地下水的环境问题受到越来越多的关注。汽油组分苯、甲苯、乙苯和二甲苯(BTEX)可以被过硫酸盐(PS)化学氧化作用有效去除。然而,乙醇的存在是否影响PS去除BTEX尚缺乏深入研究。利用石灰岩颗粒为介质,以汽油组分BTEX(总浓度为20 mg/L)和乙醇(浓度分别为500,5000 mg/L)为污染物,通过微元体(Microcosm)实验模拟污染的岩溶地下水环境,研究PS分别去除BTEX和乙醇,以及同时去除BTEX和乙醇的效果,讨论了乙醇对PS去除BTEX的影响。结果表明:前28 d,PS可以去除91%的BTEX,准一级动力学常数为0.006~0.349 d-1,其中苯最难去除,其次为甲苯。乙醇能够被PS有效去除,准一级动力学常数为0.003~0.054 d-1,去除速率小于BTEX;乙醇与BTEX共存时能够抑制BTEX的去除,但不会影响BTEX去除的优先性。PS浓度增大,有利于去除乙醇和BTEX,但会抑制微生物活性,促使pH值下降,并导致CaSO4沉淀。该试验结果可为乙醇汽油污染岩溶地下水的原位化学氧化研究提供科学参考。Abstract: With the increasing application of ethanol gasoline, the contaminated karst groundwater by its release has been concerned. Benzene, toluene, ethylbenzene, and xylene (referred to as BTEX) in gasoline can be effectively removed by in situ chemical oxidation using persulfate (PS). However, it’s still not clear whether the presence of ethanol affects the removal of BTEX by PS. In this paper, limestone particles, acting as the aqueous media, and gasoline BTEX (20 mg/L) combined with ethanol (500 mg/L or 5000 mg/L), acting as the pollutants, were used to form microcosms and simulate a contaminated karst groundwater environment. BTEX and ethanol removal effects by PS chemical oxidation were studied respectively, as well as their removal effects in coexistence. The results showed that 91% of BTEX was removed by PS in the first 28 days, with the first-order rate constants ranging from 0.006 to 0.349 d-1. Benzene was the most difficult to remove, followed by toluene. Ethanol was removed by PS with the pseudo-first-order rate constants ranging from 0.003 to 0.054 d-1, which was less than that of BTEX. The presence of ethanol could decrease the removal rate of BTEX, but couldn’t affect the removal priority of BTEX. The increase of PS concentration was beneficial to the removal of ethanol and BTEX, nevertheless, which could inhibit microbial activity, make the pH value drop more, and cause calcium sulfate precipitation. This work provides scientific data for in situ chemical oxidation of karst groundwater contaminated by ethanol gasoline.
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Key words:
- aromatics /
- persulfate /
- in-situ chemical oxidation /
- ethanol gasoline /
- karst groundwater
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[1] 刘长礼, 王秀艳, 赵悦文, 等. 一种岩溶地下水污染风险的源径标值评价方法[J]. 地球学报, 2021, 42(3):363-372. [2] 高旭波, 王万洲, 侯保俊, 等. 中国北方岩溶地下水污染分析[J]. 中国岩溶, 2020, 39(3):287-298. [3] 陈奂良, 王金晓, 林广奇, 等.岩溶地下水污染预警:以山东省刘征水源地为例[J]. 安全与环境工程, 2021, 28(3):130-136. [4] GIELNIK A, PECHAUD Y, HUGUENOT D, et al. Effect of digestate application on microbial respiration and bacterial communities' diversity during bioremediation of weathered petroleum hydrocarbons contaminated soils[J]. Science of the Total Environment, 2019, 670:271-281. [5] LU L, YAZDI H, JIN S, et al. Enhanced bioremediation of hydrocarbon-contaminated soil using pilot-scale bioelectrochemical systems[J]. Journal of Hazardous Materials, 2014, 274:8-15. [6] XUE Y F, GU X G, LU S S, et al. The destruction of benzene by calcium peroxide activated with Fe(Ⅱ) in water[J]. Chemical Engineering Journal, 2016, 302:187-193. [7] 中国能源编辑部. 《关于扩大生物燃料乙醇生产和推广使用车用乙醇汽油的实施方案》印发[J]. 中国能源, 2017, 39(9):1. [8] SOUZA D T, BENETTI C N, SAUER E, et al. Decontamination of pure and ethanol/gasoline-contaminated soil by fenton-like process[J]. Water, Air, & Soil Pollution, 2018, 229(4):105. [9] RAMA F, RAMOS D T, MULLER J B, et al. Flow field dynamics and high ethanol content in gasohol blends enhance BTEX migration and biodegradation in groundwater[J]. Journal of Contamnant Hydrology, 2019, 222:17-30. [10] WANG H, CHEN Y D, MENG W, et al. Preferential removal of benzene, toluene, ethylbenzene, and xylene (BTEX) by persulfate in ethanol-containing aquifer materials[J]. Environmental Science and Pollution Research, 2022, 29(12):17617-17625. [11] 李传维, 迟克宇, 杨乐巍, 等. 碱活化过硫酸盐在某氯代烃污染场地地下水修复中的应用[J]. 环境工程学报, 2021, 15(6):1916-1926. [12] DING Y B, WANG X R, FU L B, et al. Nonradicals induced degradation of organic pollutants by peroxydisulfate (PDS) and peroxymonosulfate (PMS):recent advances and perspective[J]. Science of the Total Environment, 2021, 756:142794. [13] WACȽAWEK S, LUTZE H V, GRVBEL K, et al. Chemistry of persulfates in water and wastewater treatment:a review[J]. Chemical Engineering Journal, 2017, 330:44-62. [14] 韩爽, 肖鹏飞. 过硫酸盐活化技术在四环素类抗生素降解中的应用进展[J]. 环境化学, 2021, 40(9):2873-2883. [15] MCGREGOR R, VAKILI F. The in situ treatment of BTEX, MTBE, and TBA in saline groundwater[J]. Remediation Journal, 2019, 29(4):107-116. [16] WANG H, CHEN Y D, HE L W, et al. Feasibility of nitrate reduction combined with persulfate oxidation in the remediation of groundwater contaminated by gasoline[J]. Hydrogeology Journal, 2021, 30(1):151-161. [17] KAKOSOVÁ E, HRABÁK P, ČERNÍK M, et al. Effect of various chemical oxidation agents on soil microbial communities[J]. Chemical Engineering Journal, 2017, 314:257-265. [18] 韦延梅, 陈余道, 吴圣华, 等. 乙醇对过硫酸盐氧化地下水中苯系物的影响[J]. 水文地质工程地质, 2019, 46(6):142-148. [19] 韦俊宏, 蒋亚萍, 陈余道, 等. 过硫酸盐氧化去除地下水中乙醇的研究[J]. 环境污染与防治, 2020, 42(8):953-958. [20] YANG H, ZHUANG S, HU Q, et al. Competitive reactions of hydroxyl and sulfate radicals with sulfonamides in Fe2+/S2O82- system:reaction kinetics, degradation mechanism and acute toxicity[J]. Chemical Engineering Journal, 2018, 339:32-41. [21] SATAPANAJARU T, CHOKEJAROENRAT C, SAKULTHAEW C, et al. Remediation and restoration of petroleum hydrocarbon containing alcohol-contaminated soil by persulfate oxidation activated with soil minerals[J]. Water, Air, & Soil Pollution, 2017, 228(9):345. [22] CHEN K F, CHANG Y C, CHIOU W T. Remediation of diesel-contaminated soil using in situ chemical oxidation (ISCO) and the effects of common oxidants on the indigenous microbial community:a comparison study[J]. Journal of Chemical Technology & Biotechnology, 2016, 91(6):1877-1888. [23] 孟伟, 蒋亚萍, 陈余道, 等. 几种含水介质中过硫酸钠去除苯系物/乙醇的效果和影响[J]. 环境化学, 2019, 38(10):2187-2194. [24] LIANG C J, HUANG C F, MOHANTY N, et al. A rapid spectrophotometric determination of persulfate anion in ISCO[J]. Chemosphere, 2008, 73(9):1540-1543. [25] 陈余道, 宋晓薇, 蒋亚萍, 等. 岩溶地下河系统石灰石对BTEX的吸附动力学和热力学[J]. 地学前缘, 2014, 21(4):180-185. [26] XIA Y, CHENG Y P, LI L Y, et al. A microcosm study on persulfate oxidation combined with enhanced bioremediation to remove dissolved BTEX in gasoline-contaminated groundwater[J]. Biodegradation, 2020, 31(3):213-222. [27] FANG G D, DIONYSIOU D D, ZHOU D M, et al. Transformation of polychlorinated biphenyls by persulfate at ambient temperature[J]. Chemosphere, 2013, 90(5):1573-1580. [28] FENG Y, WU D L, DENG Y, et al. Sulfate radical-mediated degradation of sulfadiazine by CuFeO2 rhombohedral crystal-catalyzed peroxymonosulfate:synergistic effects and mechanisms[J]. Environmental Science & Technology, 2016, 50(6):3119-3127. [29] DING Y B, TANG H B, ZHANG S H, et al. Efficient degradation of carbamazepine by easily recyclable microscaled CuFeO2 mediated heterogeneous activation of peroxymonosulfate[J]. Journal of Hazardous Materials, 2016, 317:686-694. [30] LEI Y, ZHANG H, WANG J W, et al. Rapid and continuous oxidation of organic contaminants with ascorbic acid and a modified ferric/persulfate system[J]. Chemical Engineering Journal, 2015, 270:73-79. [31] LIANG C J, HUANG C F, CHEN Y J. Potential for activated persulfate degradation of BTEX contamination[J]. Water Research, 2008, 42(15):4091-4100. [32] ANDRADE L N, ARAUJO S F, MATOS A T, et al. Performance of different oxidants in the presence of oxisol:remediation of groundwater contaminated by gasoline/ethanol blend[J]. Chemical Engineering Journal, 2017, 308:428-437. [33] ZHU C Y, ZHU F X, DIONYSIOU D D, et al. Contribution of alcohol radicals to contaminant degradation in quenching studies of persulfate activation process[J]. Water Research, 2018, 139:66-73. [34] 蒋亚萍, 黄骏宇, 孙自森, 等. 用砂桶装置和米酒去除地下水硝酸盐的影响因素[J]. 桂林理工大学学报, 2017, 37(4):671-675. [35] YEUNG C W, van STEMPVOORT D R, SPOELSTRA J, et al. Bacterial community evidence for anaerobic degradation of petroleum hydrocarbons in cold climate groundwater[J]. Cold Regions Science and Technology, 2013, 86:55-68. [36] 江晓铭, 蒋亚萍, 陈余道, 等. 过硫酸盐在岩溶管道地下水中的稳定性及其对苯系物的去除效果[J]. 环境工程学报, 2021, 15(4):1395-1402.
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