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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]
  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 Lab. (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.
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. doi:10.1038/s41396-019-0466-0.
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. doi:10.1038/s41396-019-0466-0.
@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 = {2019},
month = {6}
}

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