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Title: Effects of sulfate and magnesium on cement degradation under geologic CO2 sequestration conditions

Abstract

For safer geologic CO2 sequestration (GCS), it is important to understand CO2-brine-cement interactions, which affect wellbore integrity. However, potential effects of sulfate and magnesium ions on cement degradation under GCS conditions are not well understood. Class H Portland cement were reacted in brines containing 0.05 M sulfate and/or magnesium ions under both GCS (50 °C and 100 atm CO2) and control (50 °C and atmospheric pressure) conditions. Using optical microscopy and scanning electron microscope coupled with energy dispersive spectrometry and electron back scattered electron (SEM-EDS/BSE), slower cement carbonation rates were observed in the presence of sulfate under GCS conditions, because of gypsum precipitation on cement surfaces. Calcite rather than gypsum formed in both the inner layers of cement samples reacted under GCS conditions, and on cement surfaces reacted under atmospheric pressure conditions. Under GCS conditions, the dissolved CO2 lowered the pH of the solution surrounding cement surfaces, thus favoring the formation of gypsum over calcite on cement surfaces; while the high pH condition in pore solution inside cement favors the formation of calcite over gypsum. Finally, the presence of magnesium had no significant effect on cement degradation under GCS conditions, as brucite, magnesium carbonates and magnesium calcite did not form,more » due to the low pH at cement surface and the limited diffusion of Mg into cement inner layers.« less

Authors:
 [1];  [2];  [3];  [4];  [2]
  1. China University of Geosciences, Beijing (China)y; University of Houston, TX (United States)
  2. University of Houston, TX (United States)
  3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  4. China University of Geosciences, Beijing (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Science and Technology Innovation Fund of the China Univ. of Geosciences
OSTI Identifier:
1475007
Alternate Identifier(s):
OSTI ID: 1459454
Grant/Contract Number:  
AC02-05CH11231; 41272061; 41472232
Resource Type:
Accepted Manuscript
Journal Name:
International Journal of Greenhouse Gas Control
Additional Journal Information:
Journal Volume: 63; Journal ID: ISSN 1750-5836
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; geologic CO2 sequestration (GCS); cement degradation; sulfate; magnesium; gypsum; calcite

Citation Formats

Guo, Jilong, Cao, Bo, Steefel, Carl I., Chen, Jiawei, and Hu, Yandi. Effects of sulfate and magnesium on cement degradation under geologic CO2 sequestration conditions. United States: N. p., 2017. Web. doi:10.1016/j.ijggc.2017.04.017.
Guo, Jilong, Cao, Bo, Steefel, Carl I., Chen, Jiawei, & Hu, Yandi. Effects of sulfate and magnesium on cement degradation under geologic CO2 sequestration conditions. United States. https://doi.org/10.1016/j.ijggc.2017.04.017
Guo, Jilong, Cao, Bo, Steefel, Carl I., Chen, Jiawei, and Hu, Yandi. Thu . "Effects of sulfate and magnesium on cement degradation under geologic CO2 sequestration conditions". United States. https://doi.org/10.1016/j.ijggc.2017.04.017. https://www.osti.gov/servlets/purl/1475007.
@article{osti_1475007,
title = {Effects of sulfate and magnesium on cement degradation under geologic CO2 sequestration conditions},
author = {Guo, Jilong and Cao, Bo and Steefel, Carl I. and Chen, Jiawei and Hu, Yandi},
abstractNote = {For safer geologic CO2 sequestration (GCS), it is important to understand CO2-brine-cement interactions, which affect wellbore integrity. However, potential effects of sulfate and magnesium ions on cement degradation under GCS conditions are not well understood. Class H Portland cement were reacted in brines containing 0.05 M sulfate and/or magnesium ions under both GCS (50 °C and 100 atm CO2) and control (50 °C and atmospheric pressure) conditions. Using optical microscopy and scanning electron microscope coupled with energy dispersive spectrometry and electron back scattered electron (SEM-EDS/BSE), slower cement carbonation rates were observed in the presence of sulfate under GCS conditions, because of gypsum precipitation on cement surfaces. Calcite rather than gypsum formed in both the inner layers of cement samples reacted under GCS conditions, and on cement surfaces reacted under atmospheric pressure conditions. Under GCS conditions, the dissolved CO2 lowered the pH of the solution surrounding cement surfaces, thus favoring the formation of gypsum over calcite on cement surfaces; while the high pH condition in pore solution inside cement favors the formation of calcite over gypsum. Finally, the presence of magnesium had no significant effect on cement degradation under GCS conditions, as brucite, magnesium carbonates and magnesium calcite did not form, due to the low pH at cement surface and the limited diffusion of Mg into cement inner layers.},
doi = {10.1016/j.ijggc.2017.04.017},
journal = {International Journal of Greenhouse Gas Control},
number = ,
volume = 63,
place = {United States},
year = {Thu May 25 00:00:00 EDT 2017},
month = {Thu May 25 00:00:00 EDT 2017}
}

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Works referenced in this record:

Influence of sulfate solution concentration on the formation of gypsum in sulfate resistance test specimen
journal, February 2006


Magnesium sulfate attack on portland cement paste-I. Microstructural analysis
journal, January 1992


Analysis and performance of oil well cement with 30 years of CO2 exposure from the SACROC Unit, West Texas, USA
journal, April 2007

  • Carey, J. William; Wigand, Marcus; Chipera, Steve J.
  • International Journal of Greenhouse Gas Control, Vol. 1, Issue 1
  • DOI: 10.1016/S1750-5836(06)00004-1

Geochemistry of Wellbore Integrity in CO2 Sequestration: Portland Cement-Steel-Brine-CO2 Interactions
journal, January 2013


Wellbore integrity analysis of a natural CO2 producer
journal, March 2010

  • Crow, Walter; Carey, J. William; Gasda, Sarah
  • International Journal of Greenhouse Gas Control, Vol. 4, Issue 2
  • DOI: 10.1016/j.ijggc.2009.10.010

Fe(III) Hydroxide Nucleation and Growth on Quartz in the Presence of Cu(II), Pb(II), and Cr(III): Metal Hydrolysis and Adsorption
journal, December 2014

  • Dai, Chong; Hu, Yandi
  • Environmental Science & Technology, Vol. 49, Issue 1
  • DOI: 10.1021/es504140k

Homogeneous and Heterogeneous (Fe x , Cr 1– x )(OH) 3 Precipitation: Implications for Cr Sequestration
journal, January 2016

  • Dai, Chong; Zuo, Xiaobing; Cao, Bo
  • Environmental Science & Technology, Vol. 50, Issue 4
  • DOI: 10.1021/acs.est.5b04319

Geochemical aspects of CO2 sequestration in deep saline aquifers: A review
journal, September 2015


Degradation of oilwell cement due to exposure to carbonated brine
journal, May 2010


An estimate of the time to degrade the cement sheath in a well exposed to carbonated brine
journal, February 2009


Structure and morphology of synthetic magnesium calcite
journal, January 1998

  • Falini, Giuseppe; Fermani, Simona; Gazzano, Massimo
  • Journal of Materials Chemistry, Vol. 8, Issue 4
  • DOI: 10.1039/a707893e

Experimental investigations of the effects of acid gas (H2S / CO2 ) exposure under geological sequestration conditions
journal, January 2011


Biotite–Brine Interactions under Acidic Hydrothermal Conditions: Fibrous Illite, Goethite, and Kaolinite Formation and Biotite Surface Cracking
journal, July 2011

  • Hu, Yandi; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 45, Issue 14
  • DOI: 10.1021/es200489y

Na + , Ca 2+ , and Mg 2+ in Brines Affect Supercritical CO 2 –Brine–Biotite Interactions: Ion Exchange, Biotite Dissolution, and Illite Precipitation
journal, May 2012

  • Hu, Yandi; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es301273g

Neutralization of sulfuric acid solutions by calcite dissolution and the application to anoxic limestone drain design
journal, February 2008


Mineralogical Changes of a Well Cement in Various H 2 S-CO 2 (-Brine) Fluids at High Pressure and Temperature
journal, January 2008

  • Jacquemet, Nicolas; Pironon, Jacques; Saint-Marc, Jérémie
  • Environmental Science & Technology, Vol. 42, Issue 1
  • DOI: 10.1021/es070853s

Armouring of well cement in H2S–CO2 saturated brine by calcite coating – Experiments and numerical modelling
journal, March 2012


Effect of Inorganic Anions on the Morphology and Structure of Magnesium Calcite
journal, April 2004

  • Kralj, Damir; Kontrec, Jasminka; Brečević, Ljerka
  • Chemistry - A European Journal, Vol. 10, Issue 7
  • DOI: 10.1002/chem.200305313

Degradation of Well Cement by CO 2 under Geologic Sequestration Conditions
journal, July 2007

  • Kutchko, Barbara G.; Strazisar, Brian R.; Dzombak, David A.
  • Environmental Science & Technology, Vol. 41, Issue 13
  • DOI: 10.1021/es062828c

Rate of CO 2 Attack on Hydrated Class H Well Cement under Geologic Sequestration Conditions
journal, August 2008

  • Kutchko, Barbara G.; Strazisar, Brian R.; Lowry, Gregory V.
  • Environmental Science & Technology, Vol. 42, Issue 16
  • DOI: 10.1021/es800049r

CO 2 Reaction with Hydrated Class H Well Cement under Geologic Sequestration Conditions: Effects of Flyash Admixtures
journal, May 2009

  • Kutchko, Barbara G.; Strazisar, Brian R.; Huerta, Nicolas
  • Environmental Science & Technology, Vol. 43, Issue 10
  • DOI: 10.1021/es803007e

H2S–CO2 reaction with hydrated Class H well cement: Acid-gas injection and CO2 Co-sequestration
journal, July 2011

  • Kutchko, Barbara G.; Strazisar, Brian R.; Hawthorne, Steven B.
  • International Journal of Greenhouse Gas Control, Vol. 5, Issue 4
  • DOI: 10.1016/j.ijggc.2011.02.008

Chemical Reactions of Portland Cement with Aqueous CO 2 and Their Impacts on Cement’s Mechanical Properties under Geologic CO 2 Sequestration Conditions
journal, May 2015

  • Li, Qingyun; Lim, Yun Mook; Flores, Katharine M.
  • Environmental Science & Technology, Vol. 49, Issue 10
  • DOI: 10.1021/es5063488

Effects of Sulfate during CO 2 Attack on Portland Cement and Their Impacts on Mechanical Properties under Geologic CO 2 Sequestration Conditions
journal, May 2015

  • Li, Qingyun; Lim, Yun Mook; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 49, Issue 11
  • DOI: 10.1021/es506349u

Influence of pH on the formation of gypsum in cement materials during sulfate attack
journal, September 2015


The confused world of sulfate attack on concrete
journal, August 2004


Effects of gypsum formation on the performance of cement mortars during external sulfate attack
journal, March 2003


Characterization of cement from a well at Teapot Dome Oil Field: Implications for geological sequestration
journal, January 2011

  • Scherer, George W.; Kutchko, Barbara; Thaulow, Niels
  • International Journal of Greenhouse Gas Control, Vol. 5, Issue 1
  • DOI: 10.1016/j.ijggc.2010.06.010

The passivation of calcite by acid mine water. Column experiments with ferric sulfate and ferric chloride solutions at pH 2
journal, December 2008


Does gypsum formation during sulfate attack on concrete lead to expansion?
journal, January 2000


Expansion of Alite Paste Caused by Gypsum Formation during Sulfate Attack
journal, February 2000


Channel Flow Cell Studies of the Inhibiting Action of Gypsum on the Dissolution Kinetics of Calcite: A Laboratory Approach with Implications for Field Monitoring
journal, April 2001

  • Wilkins, Shelley J.; Compton, Richard G.; Taylor, Mark A.
  • Journal of Colloid and Interface Science, Vol. 236, Issue 2
  • DOI: 10.1006/jcis.2000.7418

Review of integrity of existing wells in relation to CO2 geological storage: What do we know?
journal, July 2011


Characterization of pozzolan-amended wellbore cement exposed to CO2 and H2S gas mixtures under geologic carbon storage conditions
journal, November 2013

  • Zhang, Liwei; Dzombak, David A.; Nakles, David V.
  • International Journal of Greenhouse Gas Control, Vol. 19
  • DOI: 10.1016/j.ijggc.2013.09.004

Rate of H2S and CO2 attack on pozzolan-amended Class H well cement under geologic sequestration conditions
journal, August 2014

  • Zhang, Liwei; Dzombak, David A.; Nakles, David V.
  • International Journal of Greenhouse Gas Control, Vol. 27
  • DOI: 10.1016/j.ijggc.2014.02.013