Department of Civil and Environmental Engineering, Stanford University , Stanford, California 94305-4020, United States.
Environ Sci Technol. 2014 Oct 7;48(19):11161-9. doi: 10.1021/es5028184. Epub 2014 Sep 24.
The disposal and leaks of hydraulic fracturing wastewater (HFW) to the environment pose human health risks. Since HFW is typically characterized by elevated salinity, concerns have been raised whether the high bromide and iodide in HFW may promote the formation of disinfection byproducts (DBPs) and alter their speciation to more toxic brominated and iodinated analogues. This study evaluated the minimum volume percentage of two Marcellus Shale and one Fayetteville Shale HFWs diluted by fresh water collected from the Ohio and Allegheny Rivers that would generate and/or alter the formation and speciation of DBPs following chlorination, chloramination, and ozonation treatments of the blended solutions. During chlorination, dilutions as low as 0.01% HFW altered the speciation toward formation of brominated and iodinated trihalomethanes (THMs) and brominated haloacetonitriles (HANs), and dilutions as low as 0.03% increased the overall formation of both compound classes. The increase in bromide concentration associated with 0.01-0.03% contribution of Marcellus HFW (a range of 70-200 μg/L for HFW with bromide = 600 mg/L) mimics the increased bromide levels observed in western Pennsylvanian surface waters following the Marcellus Shale gas production boom. Chloramination reduced HAN and regulated THM formation; however, iodinated trihalomethane formation was observed at lower pH. For municipal wastewater-impacted river water, the presence of 0.1% HFW increased the formation of N-nitrosodimethylamine (NDMA) during chloramination, particularly for the high iodide (54 ppm) Fayetteville Shale HFW. Finally, ozonation of 0.01-0.03% HFW-impacted river water resulted in significant increases in bromate formation. The results suggest that total elimination of HFW discharge and/or installation of halide-specific removal techniques in centralized brine treatment facilities may be a better strategy to mitigate impacts on downstream drinking water treatment plants than altering disinfection strategies. The potential formation of multiple DBPs in drinking water utilities in areas of shale gas development requires comprehensive monitoring plans beyond the common regulated DBPs.
水力压裂废水(HFW)的处置和泄漏对环境构成了人类健康风险。由于 HFW 通常具有较高的盐度,因此人们担心 HFW 中的高溴化物和碘化物是否会促进消毒副产物(DBPs)的形成,并改变其形态以形成更具毒性的溴化和碘化类似物。本研究评估了从俄亥俄河和阿勒格尼河收集的淡水稀释的两口马塞勒斯页岩和一口费耶特维尔页岩 HFW 的最小体积百分比,这些 HFW 在混合溶液进行氯化、氯胺化和臭氧化处理后会生成和/或改变 DBPs 的形成和形态。在氯化过程中,低至 0.01%的 HFW 稀释度就改变了形态,形成了溴化和碘化三卤甲烷(THMs)和溴化卤乙腈(HANs),低至 0.03%的稀释度增加了这两类化合物的总体形成。与马塞勒斯 HFW 0.01-0.03%(马塞勒斯 HFW 中溴化物=600mg/L 时,溴化物浓度范围为 70-200μg/L)的浓度增加相关的溴化物浓度增加模拟了马塞勒斯页岩天然气开采热潮后宾夕法尼亚西部地表水观察到的溴化物水平增加。氯胺化减少了 HAN 和受管制 THM 的形成;然而,在较低 pH 值下观察到碘代三卤甲烷的形成。对于受城市废水影响的河水,存在 0.1%的 HFW 会增加氯胺化过程中 N-亚硝基二甲胺(NDMA)的形成,特别是对于高碘化物(54ppm)的费耶特维尔页岩 HFW。最后,0.01-0.03%HFW 受影响的河水的臭氧化导致溴酸盐形成显著增加。结果表明,与改变消毒策略相比,完全消除 HFW 排放和/或在集中盐水处理设施中安装卤化物专用去除技术可能是减轻对下游饮用水处理厂影响的更好策略。在页岩气开发地区的饮用水处理厂中,可能会形成多种 DBP,这需要制定综合监测计划,而不仅仅是常见的受监管的 DBP。