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Title: Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers

Abstract

Magnesium-dominant olivine (Mg2SiO4) has received considerable attention for geologic and ex situ carbon mineralization due to its reaction potential with CO2 and its abundance in mafic and ultramafic rocks. To enable better predictions and optimization of its carbonation rate, here we compile the results of 15 separate studies into an internally consistent kinetic framework. Time-dependent transformation curves were determined, analyzed, and used to calculate temperature-dependent carbonation rate constants from 50-300 °C. The unified results clearly show that olivine carbonation is optimized at 185-200 °C, and indicate a change in the carbonation reaction mechanism above 90 °C. By comparison with related efforts focused solely on olivine dissolution rates, we demonstrate that the kinetics are controlled by growth of magnesium carbonates. Additional outcomes include the identification of important knowledge gaps and research frontiers for carbon mineralization, including those related to unraveling competitive serpentinization reactions, H2O-saturated supercritical CO2 (wet scCO2) reactivity, and the formation and impacts of secondary surface coatings. In addition to supporting the deployment of carbon storage technologies in a climate-responding world, the findings may help improve understanding of how carbonation and serpentinization processes influence critical geochemical cycles.

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [1]; ORCiD logo [1]
  1. BATTELLE (PACIFIC NW LAB)
  2. University of Wyoming
  3. UNIVERSITY OF WISCONSIN
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1572497
Report Number(s):
PNNL-SA-143712
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Environmental Science & Technology Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 8
Country of Publication:
United States
Language:
English

Citation Formats

Miller, Quin RS, Schaef, Herbert T., Kaszuba, John, Gadikota, Greeshma, McGrail, Bernard P., and Rosso, Kevin M. Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers. United States: N. p., 2019. Web. doi:10.1021/acs.estlett.9b00301.
Miller, Quin RS, Schaef, Herbert T., Kaszuba, John, Gadikota, Greeshma, McGrail, Bernard P., & Rosso, Kevin M. Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers. United States. doi:10.1021/acs.estlett.9b00301.
Miller, Quin RS, Schaef, Herbert T., Kaszuba, John, Gadikota, Greeshma, McGrail, Bernard P., and Rosso, Kevin M. Tue . "Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers". United States. doi:10.1021/acs.estlett.9b00301.
@article{osti_1572497,
title = {Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers},
author = {Miller, Quin RS and Schaef, Herbert T. and Kaszuba, John and Gadikota, Greeshma and McGrail, Bernard P. and Rosso, Kevin M.},
abstractNote = {Magnesium-dominant olivine (Mg2SiO4) has received considerable attention for geologic and ex situ carbon mineralization due to its reaction potential with CO2 and its abundance in mafic and ultramafic rocks. To enable better predictions and optimization of its carbonation rate, here we compile the results of 15 separate studies into an internally consistent kinetic framework. Time-dependent transformation curves were determined, analyzed, and used to calculate temperature-dependent carbonation rate constants from 50-300 °C. The unified results clearly show that olivine carbonation is optimized at 185-200 °C, and indicate a change in the carbonation reaction mechanism above 90 °C. By comparison with related efforts focused solely on olivine dissolution rates, we demonstrate that the kinetics are controlled by growth of magnesium carbonates. Additional outcomes include the identification of important knowledge gaps and research frontiers for carbon mineralization, including those related to unraveling competitive serpentinization reactions, H2O-saturated supercritical CO2 (wet scCO2) reactivity, and the formation and impacts of secondary surface coatings. In addition to supporting the deployment of carbon storage technologies in a climate-responding world, the findings may help improve understanding of how carbonation and serpentinization processes influence critical geochemical cycles.},
doi = {10.1021/acs.estlett.9b00301},
journal = {Environmental Science & Technology Letters},
number = 8,
volume = 6,
place = {United States},
year = {2019},
month = {8}
}