Evidence for biodegradation and volatilisation of dissolved petroleum hydrocarbons during in situ air sparging in large laboratory columns

Laboratory column experiments run for up to 13 days compared air sparging of groundwater contaminated by dissolved petroleum hydrocarbons in sterile and non-sterile aquifer sediments as well as uncontaminated sediments and groundwater. Loss of dissolved BTEX compounds in the contaminated columns was very rapid, occurring through volatilisation. The majority of the dissolved total organic carbon (TOC) persisted for much longer periods however. A direct comparison between losses from sterile and non-sterile columns suggested a negligible contribution of biodegradation to the removal of TOC. This was difficult to confirm through examination of O₂ utilisation because oxidation of a small amount of reduced sulphur in the aquifer materials was the dominant sink for O₂. Despite this, it was possible to conclude that less than 22% of the removal of TOC was through biodegradation during the first three days of air sparging.     

A strategy for aromatic hydrocarbon bioremediation under anaerobic conditions and the impacts of ethanol: a microcosm study

Increased use of ethanol-blended gasoline (gasohol) and its potential release into the subsurface have spurred interest in studying the biodegradation of and interactions between ethanol and gasoline components such as benzene, toluene, ethylbenzene and xylene isomers (BTEX) in groundwater plumes. The preferred substrate status and the high biological oxygen demand (BOD) posed by ethanol and its biodegradation products suggests that anaerobic electron acceptors (EAs) will be required to support in situ bioremediation of BTEX. To develop a strategy for aromatic hydrocarbon bioremediation and to understand the impacts of ethanol on BTEX biodegradation under strictly anaerobic conditions, a microcosm experiment was conducted using pristine aquifer sand and groundwater obtained from Canadian Forces Base Borden, Canada. The initial electron accepter pool included nitrate, sulfate and/or ferric iron. The microcosms typically contained 400 g of sediment, 600 approximately 800 ml of groundwater, and with differing EAs added, and were run under anaerobic conditions. Ethanol was added to some at concentrations of 500 and 5000 mg/L. Trends for biodegradation of aromatic hydrocarbons for the Borden aquifer material were first developed in the absence of ethanol, The results showed that indigenous microorganisms could degrade all aromatic hydrocarbons (BTEX and trimethylbenzene isomers-TMB) under nitrate- and ferric iron-combined conditions, but not under sulfate-reducing conditions. Toluene, ethylbenzene and m/p-xylene were biodegraded under denitrifying conditions. However, the persistence of benzene indicated that enhancing denitrification alone was insufficient. Both benzene and o-xylene biodegraded significantly under iron-reducing conditions, but only after denitrification had removed other aromatics. For the trimethylbenzene isomers, 1,3,5-TMB biodegradation was found under denitrifying and then iron-reducing conditions. Biodegradation of 1,2,3-TMB or 1,2,4-TMB was slower under iron-reducing conditions. This study suggests that addition of excess ferric iron combined with limited nitrate has promise for in situ bioremediation of BTEX and TMB in the Borden aquifer and possibly for other sites contaminated by hydrocarbons. This study is the first to report 1,2,3-TMB biodegradation under strictly anaerobic condition. With the addition of 500 mg/L ethanol but without EA addition, ethanol and its main intermediate, acetate, were quickly biodegraded within 41 d with methane as a major product. Ethanol initially present at 5000 mg/L without EA addition declined slowly with the persistence of unidentified volatile fatty acids, likely propionate and butyrate, but less methane. In contrast, all ethanol disappeared with repeated additions of either nitrate or ferric iron, but acetate and unidentified intermediates persisted under iron-enhanced conditions. With the addition of 500 mg/L ethanol and nitrate, only minor toluene biodegradation was observed under denitrifying conditions and only after ethanol and acetate were utilized. The higher ethanol concentration (5000 mg/L) essentially shut down BTEX biodegradation likely due to high EA demand provided by ethanol and its intermediates. The negative findings for anaerobic BTEX biodegradation in the presence of ethanol and/or its biodegradation products are in contrast to recent research reported by Da Silva et al. [Da Silva, M.L.B., Ruiz-Aguilar, G.M.L., Alvarez, P.J.J., 2005. Enhanced anaerobic biodegradation of BTEX-ethanol mixtures in aquifer columns amended with sulfate, chelated ferric iron or nitrate. Biodegradation. 16, 105-114]. Our results suggest that the apparent conservation of high residual labile carbon as biodegradation products such as acetate makes natural attenuation of aromatics less effective, and makes subsequent addition of EAs to promote in situ BTEX biodegradation problematic.     

Serious BTEX pollution in rural area of the North China Plain during winter season

Atmospheric BTEX compounds(benzene, toluene, ethylbenzene and xylenes) in a rural site of the North China Plain(NCP) were preliminarily investigated in winter, and the outdoor concentrations(25.8–236.0 μg/m3) were found to be much higher than those reported in urban regions. The pollution of BTEX inside a farmer's house was even more serious, with combined concentrations of 254.5–1552.9 μg/m3. Based on the ratio of benzene to toluene(1.17 ± 0.34) measured, the serious BTEX pollution in the rural site was mainly ascribed to domestic coal combustion for heating during the winter season. With the enhancement of farmers' incomes in recent years, coal consumption by farmers in the NCP is rapidly increasing to keep their houses warm, and hence the serious air pollution in rural areas of the NCP during winter, including BTEX, should be paid great attention.     

基于TMVOC的地下水位波动带苯系物迁移转化模拟

为探究水位波动情况下苯系物的迁移转化规律,提高石油污染场地地下水污染治理精度,以西北某傍河石化场地为研究对象,基于TMVOC模型对特征污染物苯系物开展泄漏模拟,通过情景模拟比较水位波动对苯系物迁移转化的影响,并从污染分布、相间转化等方面,解析地下水位稳定和波动状态下苯系物迁移转化过程差异.结果表明:①TMVOC模型较好地模拟了水位波动状态下苯系物迁移转化过程.②相较于水位稳定状态下,水位波动作用下苯系物污染深度增加0.5 m,污染面积增加25%,总质量增加12 kg.③水位稳定和波动状态下苯系物"气-液-NAPL（Non-Aqueous Phase Liquids）相"占比分别为0.17%、2.03%、97.8%和0.04%、3.69%、96.27%.④NAPL相苯系物饱和度分布与苯系物质量分布呈正相关,水位波动造成NAPL相初始饱和度降低,且初始水位面以下NAPL相饱和度升高.⑤对于苯而言,水位波动状态下非饱和带中苯在液相中的质量是水位稳定状态下的1.11倍,饱和带为10.15倍.研究显示,水位波动显著地影响了苯系物的迁移转化过程,促进了苯系物的溶解,并使更多的苯系物残留在地下介质中.      

Comprehensive Environmental Investigation at Former Industrial/Petroleum Underground Storage Tank Sites in Long Beach,CA: A Forensic Perspective

Two industrial sites were investigated based on years of available hydrogeologic information and monitoring data for soil and groundwater. Collected data were forensically evaluated using age-dating and fingerprinting methods. The previous business uses of the project sites were as a gas station, laundry/dry-cleaning service, and car wash with petroleum underground storage tanks (USTs). As a result, these sites were exposed to a number of toxic contaminants at relatively high concentrations. Source control was necessary for successful remediation and the ultimate removal of the remaining compounds from these industrial sites. Although contaminated soil around the source was excavated during the remedial action and the high concentrations of contaminants were reduced, typical groundwater contaminants such as petroleum hydrocarbons as gasoline (TPH-G), benzene, toluene, ethylbenzene, xylenes (BTEX), and oxygenates including methyl tert-butyl ether (MTBE), diisopropyl ether (DIPE), ethyl tert-butyl ether (ETBE), tert-amyl methyl ether (TAME), and tert-butyl alcohol (TBA) were persistently found at the studied sites around the source points. The plume and concentration of contaminants had changed their shapes and strength for all monitoring periods. Thus, additional source control seems to be a requirement for the complete removal of source contamination, which must be ascertained with groundwater and soil monitoring on a regular time base. For the study sites, monitored natural attenuation was relatively feasible for the long-term plan; however, it did not offer a perfect remediation solution for an ultimate goal because of residual toxic compounds that might have affected the surrounding residential areas at higher concentrations than their health limits. Therefore, as a remediation strategy, the combination of clean-up technology and natural attenuation with monitoring activities are more highly recommended than either clean-up or natural attenuation used separately.     

天津城区夏冬季典型污染过程中BTEX变化特征及其健康风险评估

利用GC955在线气相色谱仪分别于2019年7月和2020年1月在天津市区开展苯系物(BTEX,包括苯、甲苯、乙苯、间/对-二甲苯和邻-二甲苯)实时在线观测,对典型污染过程中BTEX的浓度水平、组成及演化机制进行了研究,并运用特征物种比值法对BTEX的来源进行了定性分析,最后运用US EPA的人体暴露分析评价方法对BTEX健康风险进行评估.结果表明,臭氧和霾污染过程中BTEX体积分数平均值分别为1.32×10^-9和4.83×10^-9,其中苯的体积分数占比最大,其次是甲苯、乙苯和二甲苯占比最小.2020年1月BTEX体积分数很大程度上受到西南方向短距离传输的影响,而在2019年7月BTEX浓度受到本地排放的影响.BTEX浓度水平在2019年7月受到温度和相对湿度的共同影响,而在2020年1月当温度较低时BTEX浓度对相对湿度的变化更敏感.天津市区BTEX在霾污染过程中受生物质燃烧/化石燃料燃烧/燃煤排放的影响较大,而在臭氧污染过程中除了受到燃烧排放源影响,交通源排放在很大程度上也有影响.臭氧污染和霾污染过程中BTEX的HI分别为0.072和0....     

顶空气相色谱法测定土壤中BTEX

本文采用顶空气相色谱法从土壤样品中分离挥发性有机物。应用该技术,苯、甲苯、乙基苯及二甲苯异构体（ＢＴＥＸ）均得到有效分离。该方法有较好的精密度（变异系数６５％,回收率８９～１０３％）和低的检出限（对于苯为０５ｎｇ／ｇ）。土壤样品中加入水或加热,可提高方法的灵敏度。     

BTEX在河流渗滤系统中的降解行为实验模拟研究

河流渗滤是一种自然净化过程,污染河水通过该过程在河流沉积层中发生各种物理、化学和生物作用,使得污染物浓度降低,河水水质得到净化,从而达到增加地下水开采量的目的。本项研究通过淋滤实验,利用自行设计的土柱实验装置和人工配制的淋滤液,模拟了BTEX污染河水在下渗通过河流渗滤系统的过程中发生的降解行为。实验历时48 d,获得了该过程中BTEX各组分和电子受体的质量浓度变化历时曲线,得出的结论包括：污染河水中的BTEX在通过河流渗滤系统时将发生两种环境行为—吸附和降解。其中,吸附作用对于BTEX的净化效果较为有限,当吸附达到饱和之后,在存在电子受体的情况下,BTEX能够发生厌氧微生物降解,降解作用能够更有效的去除BTEX污染物。其中去除效率最高的是间二甲苯,在以NO3-为电子受体的情况下平均去除率为85.5%,在以SO42-为电子受体的情况下平均去除率为82.4%,其次是乙苯、甲苯,去除率最差的是苯,在两种电子受体的系统中平均去除率分别为68.5%和63.5%。由于吸附作用的影响,微生物降解相对于BTEX浓度变化存在一个滞后期,BTEX各组分的土壤-水吸附分配系数Kd越大,总的降解效率也就越低。通过河流渗滤系统这一自然净化过程,可以有效地去除浓度较高的BTEX混合污染,各组分平均去除效率都超过了60%,最高去除率均超过了80%。对于持续不断入渗的污染河水,当土壤吸附达到饱和、微生物活性受到抑制,去除效率会大大降低,从而使BTEX穿透河流沉积层进入含水层,对地下水产生危害。     

BTEX pollution caused by motorcycles in the megacity of HoChiMinh

Monitoring of benzene, toluene and xylenes (BTEX) was conducted along with traffic counts at 17 roadside sites in urban areas of HoChiMinh. Toluene was the most abundant substance, followed by p,m-xylenes, benzene, o-xylene and ethylbenzene. The maximum observed hour-average benzene concentration was 254 μg/m3 . Motorcycles contributed to 91% of the traffic fleet. High correlations among BTEX species, between BTEX concentrations and the volume of on-road motorcycles, and between inter-species ratios in air and in gasoline indicate the motorcycle-exhaust origin of BTEX species. Daily concentrations of benzene, toluene, ethylbenzene, p,m-xylenes and o-xylene were 56, 121, 21, 64 and 23 μg/m 3 , respectively. p,m-xylenes possess the highest ozone formation potential among the BTEX family.     

广州大坦沙污水处理厂挥发有机物的去除及其向空气中的排放

对广州大坦沙污水处理厂各工艺阶段污水中挥发性有机物(VOCs)的测试表明,进水中主要有害VOCs为苯系物和卤代烃;进水和出水比较,苯 甲苯、乙苯、二甲苯(合称BTEX) 的去除率接近100%,污水中几种主要卤代烃的去除效率范围为79%—89%.VOCs主要的去除作用发生在生物反应池,特别是厌氧阶段,本研究还对污水处理厂几种典型挥发有机物排放到周围空气中的量进行了理论估计,计算表明卤代烃进入空气中的比例高于BTEX.