废弃油气井泄漏到含水层的甲烷厌氧氧化

IF 5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS
Samuel W. Shaheen, Max K. Lloyd, Eric E. Roden, Susan L. Brantley
{"title":"废弃油气井泄漏到含水层的甲烷厌氧氧化","authors":"Samuel W. Shaheen, Max K. Lloyd, Eric E. Roden, Susan L. Brantley","doi":"10.1016/j.gca.2025.08.039","DOIUrl":null,"url":null,"abstract":"As oil and gas wells in sedimentary basins worldwide are increasingly abandoned, the legacy wells can remain as conduits for deeper fluids to reach shallow aquifers. To investigate impacts of mixing between the deep and shallow subsurface, we characterized the geochemistry of artesian flows and groundwater discharges associated with abandoned wellbores in the oldest commercially developed oil and gas basin (Appalachian Basin, U.S.A.). Across 18 sites, we observed evidence that basin brines and gases migrate upwards from oil- and gas-producing formations and mix with meteoric waters at shallow depths. All the observed groundwater chemistries were methane-rich and reducing, but some sites were also characterized by high concentrations of dissolved metals, which we hypothesized to derive from the anaerobic oxidation of methane near leaking wellbores. To explore this, we characterized microbial assemblages in groundwaters, conducted laboratory incubation experiments, and developed a reactive transport model integrating our results. We detected evidence for both brine contamination and anaerobic methanotrophic archaea in field samples. Our observations of these archaea in field samples, alongside observations from laboratory incubations of the consortia, provide evidence for active anaerobic oxidation of methane (AOM) in aquifers affected by gas and oil extraction. We also discovered that dissolved gas compositions and the microbial community assemblages are consistent with both methanogenesis and methanotrophy affecting fluids that migrate via abandoned wellbores. We observed complex patterns in the carbon isotopes of hydrocarbons, including divergent trends in the isotopic composition of methane and ethane. These patterns may derive from non-traditional isotopic effects of AOM at low energetic yields in freshwater environments, particularly where aquifer geochemistry or long fluid residence times produce low concentrations of electron acceptors. Simulating AOM coupled to iron- or sulfate-reduction within methane migration pathways using a reactive transport model, we show that metal-rich and metal-poor waters can be easily explained by a chemical divide driven by availability of electron acceptors (iron versus sulfur respectively) in the presence of AOM. Our results emphasize that legacy oil and gas operations not only leak natural gases that contaminate the atmosphere, but also release salts and reducing equivalents into groundwater that deleteriously affect water quality.","PeriodicalId":327,"journal":{"name":"Geochimica et Cosmochimica Acta","volume":"72 1","pages":""},"PeriodicalIF":5.0000,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Anaerobic oxidation of methane from abandoned oil and gas wells leaking into aquifers\",\"authors\":\"Samuel W. Shaheen, Max K. Lloyd, Eric E. Roden, Susan L. Brantley\",\"doi\":\"10.1016/j.gca.2025.08.039\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"As oil and gas wells in sedimentary basins worldwide are increasingly abandoned, the legacy wells can remain as conduits for deeper fluids to reach shallow aquifers. To investigate impacts of mixing between the deep and shallow subsurface, we characterized the geochemistry of artesian flows and groundwater discharges associated with abandoned wellbores in the oldest commercially developed oil and gas basin (Appalachian Basin, U.S.A.). Across 18 sites, we observed evidence that basin brines and gases migrate upwards from oil- and gas-producing formations and mix with meteoric waters at shallow depths. All the observed groundwater chemistries were methane-rich and reducing, but some sites were also characterized by high concentrations of dissolved metals, which we hypothesized to derive from the anaerobic oxidation of methane near leaking wellbores. To explore this, we characterized microbial assemblages in groundwaters, conducted laboratory incubation experiments, and developed a reactive transport model integrating our results. We detected evidence for both brine contamination and anaerobic methanotrophic archaea in field samples. Our observations of these archaea in field samples, alongside observations from laboratory incubations of the consortia, provide evidence for active anaerobic oxidation of methane (AOM) in aquifers affected by gas and oil extraction. We also discovered that dissolved gas compositions and the microbial community assemblages are consistent with both methanogenesis and methanotrophy affecting fluids that migrate via abandoned wellbores. We observed complex patterns in the carbon isotopes of hydrocarbons, including divergent trends in the isotopic composition of methane and ethane. These patterns may derive from non-traditional isotopic effects of AOM at low energetic yields in freshwater environments, particularly where aquifer geochemistry or long fluid residence times produce low concentrations of electron acceptors. Simulating AOM coupled to iron- or sulfate-reduction within methane migration pathways using a reactive transport model, we show that metal-rich and metal-poor waters can be easily explained by a chemical divide driven by availability of electron acceptors (iron versus sulfur respectively) in the presence of AOM. Our results emphasize that legacy oil and gas operations not only leak natural gases that contaminate the atmosphere, but also release salts and reducing equivalents into groundwater that deleteriously affect water quality.\",\"PeriodicalId\":327,\"journal\":{\"name\":\"Geochimica et Cosmochimica Acta\",\"volume\":\"72 1\",\"pages\":\"\"},\"PeriodicalIF\":5.0000,\"publicationDate\":\"2025-08-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Geochimica et Cosmochimica Acta\",\"FirstCategoryId\":\"89\",\"ListUrlMain\":\"https://doi.org/10.1016/j.gca.2025.08.039\",\"RegionNum\":1,\"RegionCategory\":\"地球科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"GEOCHEMISTRY & GEOPHYSICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Geochimica et Cosmochimica Acta","FirstCategoryId":"89","ListUrlMain":"https://doi.org/10.1016/j.gca.2025.08.039","RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"GEOCHEMISTRY & GEOPHYSICS","Score":null,"Total":0}
引用次数: 0

摘要

随着世界范围内沉积盆地的油气井越来越多地被废弃,遗留井可以作为深层流体进入浅层含水层的管道。为了研究深层和浅层地下混合的影响,我们对美国最古老的商业开发油气盆地(Appalachian basin, U.S.A.)废弃井的自流和地下水排放的地球化学特征进行了描述。在18个地点,我们观察到盆地盐水和气体从油气生产层向上运移的证据,并与浅层的大气水混合。所有观测到的地下水化学成分都是富含甲烷的,而且是还原的,但一些地点也有高浓度的溶解金属,我们假设这是由于泄漏井附近甲烷的厌氧氧化造成的。为了探索这一点,我们对地下水中的微生物组合进行了表征,进行了实验室培养实验,并结合我们的结果建立了一个反应性输运模型。我们在野外样品中发现了盐水污染和厌氧甲烷营养古细菌的证据。我们在野外样品中对这些古菌的观察,以及对该联合体实验室孵育的观察,为受天然气和石油开采影响的含水层中甲烷(AOM)的活性厌氧氧化提供了证据。我们还发现,溶解气体组成和微生物群落组合与产甲烷和产甲烷作用相一致,影响通过废弃井运移的流体。我们观察到碳氢化合物碳同位素的复杂模式,包括甲烷和乙烷同位素组成的不同趋势。这些模式可能源于淡水环境中低能量产出的AOM的非传统同位素效应,特别是在含水层地球化学或长流体停留时间产生低浓度电子受体的情况下。使用反应输运模型模拟甲烷迁移路径中与铁或硫酸盐还原耦合的AOM,我们表明,在AOM存在的情况下,由电子受体(分别为铁和硫)的可用性驱动的化学划分可以很容易地解释富金属和贫金属的水。我们的研究结果强调,传统的油气作业不仅会泄漏污染大气的天然气,还会将盐和还原物释放到地下水中,从而对水质产生有害影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Anaerobic oxidation of methane from abandoned oil and gas wells leaking into aquifers
As oil and gas wells in sedimentary basins worldwide are increasingly abandoned, the legacy wells can remain as conduits for deeper fluids to reach shallow aquifers. To investigate impacts of mixing between the deep and shallow subsurface, we characterized the geochemistry of artesian flows and groundwater discharges associated with abandoned wellbores in the oldest commercially developed oil and gas basin (Appalachian Basin, U.S.A.). Across 18 sites, we observed evidence that basin brines and gases migrate upwards from oil- and gas-producing formations and mix with meteoric waters at shallow depths. All the observed groundwater chemistries were methane-rich and reducing, but some sites were also characterized by high concentrations of dissolved metals, which we hypothesized to derive from the anaerobic oxidation of methane near leaking wellbores. To explore this, we characterized microbial assemblages in groundwaters, conducted laboratory incubation experiments, and developed a reactive transport model integrating our results. We detected evidence for both brine contamination and anaerobic methanotrophic archaea in field samples. Our observations of these archaea in field samples, alongside observations from laboratory incubations of the consortia, provide evidence for active anaerobic oxidation of methane (AOM) in aquifers affected by gas and oil extraction. We also discovered that dissolved gas compositions and the microbial community assemblages are consistent with both methanogenesis and methanotrophy affecting fluids that migrate via abandoned wellbores. We observed complex patterns in the carbon isotopes of hydrocarbons, including divergent trends in the isotopic composition of methane and ethane. These patterns may derive from non-traditional isotopic effects of AOM at low energetic yields in freshwater environments, particularly where aquifer geochemistry or long fluid residence times produce low concentrations of electron acceptors. Simulating AOM coupled to iron- or sulfate-reduction within methane migration pathways using a reactive transport model, we show that metal-rich and metal-poor waters can be easily explained by a chemical divide driven by availability of electron acceptors (iron versus sulfur respectively) in the presence of AOM. Our results emphasize that legacy oil and gas operations not only leak natural gases that contaminate the atmosphere, but also release salts and reducing equivalents into groundwater that deleteriously affect water quality.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Geochimica et Cosmochimica Acta
Geochimica et Cosmochimica Acta 地学-地球化学与地球物理
CiteScore
9.60
自引率
14.00%
发文量
437
审稿时长
6 months
期刊介绍: Geochimica et Cosmochimica Acta publishes research papers in a wide range of subjects in terrestrial geochemistry, meteoritics, and planetary geochemistry. The scope of the journal includes: 1). Physical chemistry of gases, aqueous solutions, glasses, and crystalline solids 2). Igneous and metamorphic petrology 3). Chemical processes in the atmosphere, hydrosphere, biosphere, and lithosphere of the Earth 4). Organic geochemistry 5). Isotope geochemistry 6). Meteoritics and meteorite impacts 7). Lunar science; and 8). Planetary geochemistry.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信