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Title: Wollastonite Carbonation in Water-Bearing Supercritical CO 2: Effects of Particle Size

Abstract

The performance of geologic CO 2 sequestration (GCS) can be affected by CO 2 mineralization and changes in the permeability of geologic formations resulting from interactions between water-bearing supercritical CO 2 (scCO 2) and silicates in reservoir rocks. However, without an understanding of the size effects, the findings in previous studies using nanometer- or micrometer-size particles cannot be applied to the bulk rock in field sites. In this study, we report the effects of particle sizes on the carbonation of wollastonite (CaSiO 3) at 60 °C and 100 bar in water-bearing scCO 2. After normalization by the surface area, the thickness of the reacted wollastonite layer on the surfaces was independent of particle sizes. After 20 h, the reaction was not controlled by the kinetics of surface reactions but by the diffusion of water-bearing scCO 2 across the product layer on wollastonite surfaces. Among the products of reaction, amorphous silica, rather than calcite, covered the wollastonite surface and acted as a diffusion barrier to water-bearing scCO 2. The product layer was not highly porous, with a specific surface area 10 times smaller than that of the altered amorphous silica formed at the wollastonite surface in aqueous solution. As a result,more » these findings can help us evaluate the impacts of mineral carbonation in water-bearing scCO 2.« less

Authors:
 [1];  [1];  [2];  [2]; ORCiD logo [1]
  1. Washington Univ., St. Louis, MO (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Nanoscale Control of Geologic CO2 (NCGC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1476570
Grant/Contract Number:  
[AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
[ Journal Volume: 51; Journal Issue: 21; Related Information: © 2017 American Chemical Society.]; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Min, Yujia, Li, Qingyun, Voltolini, Marco, Kneafsey, Timothy, and Jun, Young -Shin. Wollastonite Carbonation in Water-Bearing Supercritical CO2: Effects of Particle Size. United States: N. p., 2017. Web. doi:10.1021/acs.est.7b04475.
Min, Yujia, Li, Qingyun, Voltolini, Marco, Kneafsey, Timothy, & Jun, Young -Shin. Wollastonite Carbonation in Water-Bearing Supercritical CO2: Effects of Particle Size. United States. doi:10.1021/acs.est.7b04475.
Min, Yujia, Li, Qingyun, Voltolini, Marco, Kneafsey, Timothy, and Jun, Young -Shin. Mon . "Wollastonite Carbonation in Water-Bearing Supercritical CO2: Effects of Particle Size". United States. doi:10.1021/acs.est.7b04475. https://www.osti.gov/servlets/purl/1476570.
@article{osti_1476570,
title = {Wollastonite Carbonation in Water-Bearing Supercritical CO2: Effects of Particle Size},
author = {Min, Yujia and Li, Qingyun and Voltolini, Marco and Kneafsey, Timothy and Jun, Young -Shin},
abstractNote = {The performance of geologic CO2 sequestration (GCS) can be affected by CO2 mineralization and changes in the permeability of geologic formations resulting from interactions between water-bearing supercritical CO2 (scCO2) and silicates in reservoir rocks. However, without an understanding of the size effects, the findings in previous studies using nanometer- or micrometer-size particles cannot be applied to the bulk rock in field sites. In this study, we report the effects of particle sizes on the carbonation of wollastonite (CaSiO3) at 60 °C and 100 bar in water-bearing scCO2. After normalization by the surface area, the thickness of the reacted wollastonite layer on the surfaces was independent of particle sizes. After 20 h, the reaction was not controlled by the kinetics of surface reactions but by the diffusion of water-bearing scCO2 across the product layer on wollastonite surfaces. Among the products of reaction, amorphous silica, rather than calcite, covered the wollastonite surface and acted as a diffusion barrier to water-bearing scCO2. The product layer was not highly porous, with a specific surface area 10 times smaller than that of the altered amorphous silica formed at the wollastonite surface in aqueous solution. As a result, these findings can help us evaluate the impacts of mineral carbonation in water-bearing scCO2.},
doi = {10.1021/acs.est.7b04475},
journal = {Environmental Science and Technology},
number = [21],
volume = [51],
place = {United States},
year = {2017},
month = {10}
}

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