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Title: In situ transformation of ethoxylate and glycol surfactants by shale-colonizing microorganisms during hydraulic fracturing

Abstract

In the last decade, extensive application of hydraulic fracturing technologies to unconventional low-permeability hydrocarbon-rich formations has significantly increased natural gas production in the United States and abroad. The injection of surface-sourced fluids to generate fractures in the deep subsurface introduces microbial cells and substrates to low-permeability rock. A subset of injected organic additives has been investigated for their ability to support biological growth in shale microbial community members; however, to date, little is known on how complex xenobiotic organic compounds undergo biotransformations in this deep rock ecosystem. Here, high-resolution chemical, metagenomic, and proteomic analyses reveal that widely-used surfactants are degraded by the shale-associated taxa Halanaerobium, both in situ and under laboratory conditions. These halotolerant bacteria exhibit surfactant substrate specificities, preferring polymeric propoxylated glycols (PPGs) and longer alkyl polyethoxylates (AEOs) over polyethylene glycols (PEGs) and shorter AEOs. Enzymatic transformation occurs through repeated terminal-end polyglycol chain shortening during co-metabolic growth through the methylglyoxal bypass. Furthermore, this work provides the first evidence that shale microorganisms can transform xenobiotic surfactants in fracture fluid formulations, likely affecting the efficiency of hydrocarbon recovery, and demonstrating an important association between injected substrates and microbial growth in an engineered subsurface ecosystem.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [4]; ORCiD logo [4];  [1]; ORCiD logo [5]; ORCiD logo [5];  [5];  [1];  [1]; ORCiD logo [5]; ORCiD logo [5];  [2];  [5];  [4];  [3]
+ Show Author Affiliations
  1. The Ohio State Univ., Columbus, OH (United States)
  2. Duke Univ., Durham, NC (United States)
  3. Univ. of New Hampshire, Durham, NH (United States)
  4. Colorado State Univ., Fort Collins, CO (United States)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1572967
Report Number(s):
PNNL-SA-141428
Journal ID: ISSN 1751-7362
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
The ISME Journal
Additional Journal Information:
Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 1751-7362
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Evans, Morgan V., Getzinger, Gordon, Luek, Jenna L., Hanson, Andrea J., McLaughlin, Molly C., Blotevogel, Jens, Welch, Susan A., Nicora, Carrie D., Purvine, Samuel O., Xu, Chengdong, Cole, David R., Darrah, Thomas H., Hoyt, David W., Metz, Thomas O., Ferguson, P. Lee, Lipton, Mary S., Wilkins, Michael J., and Mouser, Paula J. In situ transformation of ethoxylate and glycol surfactants by shale-colonizing microorganisms during hydraulic fracturing. United States: N. p., 2019. Web. doi:10.1038/s41396-019-0466-0.
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Evans, Morgan V., Getzinger, Gordon, Luek, Jenna L., Hanson, Andrea J., McLaughlin, Molly C., Blotevogel, Jens, Welch, Susan A., Nicora, Carrie D., Purvine, Samuel O., Xu, Chengdong, Cole, David R., Darrah, Thomas H., Hoyt, David W., Metz, Thomas O., Ferguson, P. Lee, Lipton, Mary S., Wilkins, Michael J., & Mouser, Paula J. In situ transformation of ethoxylate and glycol surfactants by shale-colonizing microorganisms during hydraulic fracturing. United States. https://doi.org/10.1038/s41396-019-0466-0
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Evans, Morgan V., Getzinger, Gordon, Luek, Jenna L., Hanson, Andrea J., McLaughlin, Molly C., Blotevogel, Jens, Welch, Susan A., Nicora, Carrie D., Purvine, Samuel O., Xu, Chengdong, Cole, David R., Darrah, Thomas H., Hoyt, David W., Metz, Thomas O., Ferguson, P. Lee, Lipton, Mary S., Wilkins, Michael J., and Mouser, Paula J. Wed . "In situ transformation of ethoxylate and glycol surfactants by shale-colonizing microorganisms during hydraulic fracturing". United States. https://doi.org/10.1038/s41396-019-0466-0. https://www.osti.gov/servlets/purl/1572967.
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@article{osti_1572967,
title = {In situ transformation of ethoxylate and glycol surfactants by shale-colonizing microorganisms during hydraulic fracturing},
author = {Evans, Morgan V. and Getzinger, Gordon and Luek, Jenna L. and Hanson, Andrea J. and McLaughlin, Molly C. and Blotevogel, Jens and Welch, Susan A. and Nicora, Carrie D. and Purvine, Samuel O. and Xu, Chengdong and Cole, David R. and Darrah, Thomas H. and Hoyt, David W. and Metz, Thomas O. and Ferguson, P. Lee and Lipton, Mary S. and Wilkins, Michael J. and Mouser, Paula J.},
abstractNote = {In the last decade, extensive application of hydraulic fracturing technologies to unconventional low-permeability hydrocarbon-rich formations has significantly increased natural gas production in the United States and abroad. The injection of surface-sourced fluids to generate fractures in the deep subsurface introduces microbial cells and substrates to low-permeability rock. A subset of injected organic additives has been investigated for their ability to support biological growth in shale microbial community members; however, to date, little is known on how complex xenobiotic organic compounds undergo biotransformations in this deep rock ecosystem. Here, high-resolution chemical, metagenomic, and proteomic analyses reveal that widely-used surfactants are degraded by the shale-associated taxa Halanaerobium, both in situ and under laboratory conditions. These halotolerant bacteria exhibit surfactant substrate specificities, preferring polymeric propoxylated glycols (PPGs) and longer alkyl polyethoxylates (AEOs) over polyethylene glycols (PEGs) and shorter AEOs. Enzymatic transformation occurs through repeated terminal-end polyglycol chain shortening during co-metabolic growth through the methylglyoxal bypass. Furthermore, this work provides the first evidence that shale microorganisms can transform xenobiotic surfactants in fracture fluid formulations, likely affecting the efficiency of hydrocarbon recovery, and demonstrating an important association between injected substrates and microbial growth in an engineered subsurface ecosystem.},
doi = {10.1038/s41396-019-0466-0},
journal = {The ISME Journal},
number = 11,
volume = 13,
place = {United States},
year = {Wed Jun 26 00:00:00 EDT 2019},
month = {Wed Jun 26 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41396-019-0466-0
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Citation Metrics:
Cited by: 12 works
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Figures / Tables:

Fig. 1 Fig. 1: a Structures of polyglycol compounds observed in this UticaPoint Pleasant natural-gas well. b Produced fluid temporal change in total AEO species for linear nC6, branched C6, and C8 AEOs where C0 is the sum of all ethoxylates of a particular alkyl species at Day 86. Error bars correspondmore » to the standard deviation of the average change experienced by the sum of all ethoxylates for a given alkyl chain. c Branched C6 AEO temporal trends relative to Day 86, with each bar representing a different C6 ethoxylate. d First-order rate constants (bars, left y-axis) and half-lives (circles, right y-axis) for PEGs, C4, nC6, C6, and C8 AEOs. Colors correspond to legend given in b, e. e Produced fluid temporal change in total AEO for C4 AEOs and PEGs where C0 is the sum of all ethoxylates of a particular alkyl species at Day 86. Error is the same as described in b« less
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    Works referencing / citing this record:

    Identification of Persistent Sulfidogenic Bacteria in Shale Gas Produced Waters
    conference, January 2020

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