文章基本信息

标题：Elevated levels of diesel range organic compounds in groundwater near Marcellus gas operations are derived from surface activities
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作者：Brian D. Drollette ; Kathrin Hoelzer ; Nathaniel R. Warner 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2015
卷号：112
期号：43
页码：13184-13189
DOI：10.1073/pnas.1511474112
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：SignificanceOrganic compounds found in drinking water aquifers above the Marcellus Shale and other shale plays could reflect natural geologic transport processes or contamination from anthropogenic activities, including enhanced natural gas production. Using analyses of organic compounds coupled with inorganic geochemical fingerprinting, estimates of groundwater residence time, and geospatial analyses of shale gas wells and disclosed safety violations, we determined that the dominant source of organic compounds to shallow aquifers was consistent with surface spills of disclosed chemical additives. There was no evidence of association with deeper brines or long-range migration of these compounds to the shallow aquifers. Encouragingly, drinking water sources affected by disclosed surface spills could be targeted for treatment and monitoring to protect public health. Hundreds of organic chemicals are used during natural gas extraction via high-volume hydraulic fracturing (HVHF). However, it is unclear whether these chemicals, injected into deep shale horizons, reach shallow groundwater aquifers and affect local water quality, either from those deep HVHF injection sites or from the surface or shallow subsurface. Here, we report detectable levels of organic compounds in shallow groundwater samples from private residential wells overlying the Marcellus Shale in northeastern Pennsylvania. Analyses of purgeable and extractable organic compounds from 64 groundwater samples revealed trace levels of volatile organic compounds, well below the Environmental Protection Agency's maximum contaminant levels, and low levels of both gasoline range (0-8 ppb) and diesel range organic compounds (DRO; 0-157 ppb). A compound-specific analysis revealed the presence of bis(2-ethylhexyl) phthalate, which is a disclosed HVHF additive, that was notably absent in a representative geogenic water sample and field blanks. Pairing these analyses with (i) inorganic chemical fingerprinting of deep saline groundwater, (ii) characteristic noble gas isotopes, and (iii) spatial relationships between active shale gas extraction wells and wells with disclosed environmental health and safety violations, we differentiate between a chemical signature associated with naturally occurring saline groundwater and one associated with alternative anthropogenic routes from the surface (e.g., accidental spills or leaks). The data support a transport mechanism of DRO to groundwater via accidental release of fracturing fluid chemicals derived from the surface rather than subsurface flow of these fluids from the underlying shale formation.
关键词：natural gas extraction ; high-volume hydraulic fracturing ; groundwater ; hydrophobic organic contaminants ; transport mechanisms