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Title: Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO 2 Flooding

Mineral reactions during CO 2 sequestration will change the pore-size distribution and pore surface characteristics, complicating permeability and storage security predictions. In this study, we report a small/wide angle scattering study of wellbore cement that has been exposed to carbon dioxide for three decades. We have constructed detailed contour maps that describe local porosity distributions and the mineralogy of the sample and relate these quantities to the carbon dioxide reaction front on the cement. We find that the initial bimodal distribution of pores in the cement, 1–2 and 10–20 nm, is affected differently during the course of carbonation reactions. Initial dissolution of cement phases occurs in the 10–20 nm pores and leads to the development of new pore spaces that are eventually sealed by CaCO 3 precipitation, leading to a loss of gel and capillary nanopores, smoother pore surfaces, and reduced porosity. This suggests that during extensive carbonation of wellbore cement, the cement becomes less permeable because of carbonate mineral precipitation within the pore space. Additionally, the loss of gel and capillary nanoporosities will reduce the reactivity of cement with CO 2 due to reactive surface area loss. Finally, this work demonstrates the importance of understanding not only changes inmore » total porosity but also how the distribution of porosity evolves with reaction that affects permeability.« less
Authors:
ORCiD logo [1] ;  [1] ; ORCiD logo [2] ;  [1] ;  [1] ;  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Report Number(s):
LA-UR-17-27502
Journal ID: ISSN 0013-936X; KC0307010; ERKCC67
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; FE-371-14-FY16; AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 51; Journal Issue: 1; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Fossil Energy (FE)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; Earth Sciences; Energy Sciences
OSTI Identifier:
1338566
Alternate Identifier(s):
OSTI ID: 1373414; OSTI ID: 1407900

Cheshire, Michael C., Stack, Andrew G., Carey, J. William, Anovitz, Lawrence M., Prisk, Timothy R., and Ilavsky, Jan. Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO2 Flooding. United States: N. p., Web. doi:10.1021/acs.est.6b03290.
Cheshire, Michael C., Stack, Andrew G., Carey, J. William, Anovitz, Lawrence M., Prisk, Timothy R., & Ilavsky, Jan. Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO2 Flooding. United States. doi:10.1021/acs.est.6b03290.
Cheshire, Michael C., Stack, Andrew G., Carey, J. William, Anovitz, Lawrence M., Prisk, Timothy R., and Ilavsky, Jan. 2016. "Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO2 Flooding". United States. doi:10.1021/acs.est.6b03290. https://www.osti.gov/servlets/purl/1338566.
@article{osti_1338566,
title = {Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO2 Flooding},
author = {Cheshire, Michael C. and Stack, Andrew G. and Carey, J. William and Anovitz, Lawrence M. and Prisk, Timothy R. and Ilavsky, Jan},
abstractNote = {Mineral reactions during CO2 sequestration will change the pore-size distribution and pore surface characteristics, complicating permeability and storage security predictions. In this study, we report a small/wide angle scattering study of wellbore cement that has been exposed to carbon dioxide for three decades. We have constructed detailed contour maps that describe local porosity distributions and the mineralogy of the sample and relate these quantities to the carbon dioxide reaction front on the cement. We find that the initial bimodal distribution of pores in the cement, 1–2 and 10–20 nm, is affected differently during the course of carbonation reactions. Initial dissolution of cement phases occurs in the 10–20 nm pores and leads to the development of new pore spaces that are eventually sealed by CaCO3 precipitation, leading to a loss of gel and capillary nanopores, smoother pore surfaces, and reduced porosity. This suggests that during extensive carbonation of wellbore cement, the cement becomes less permeable because of carbonate mineral precipitation within the pore space. Additionally, the loss of gel and capillary nanoporosities will reduce the reactivity of cement with CO2 due to reactive surface area loss. Finally, this work demonstrates the importance of understanding not only changes in total porosity but also how the distribution of porosity evolves with reaction that affects permeability.},
doi = {10.1021/acs.est.6b03290},
journal = {Environmental Science and Technology},
number = 1,
volume = 51,
place = {United States},
year = {2016},
month = {12}
}