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Title: CO 2 Absorption and Magnesium Carbonate Precipitation in MgCl 2–NH 3–NH 4Cl Solutions: Implications for Carbon Capture and Storage

Abstract

CO 2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO 2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO 2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO 2 gas to carbonates in MgCl 2–NH 3–NH 4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limiting step of CO 2 absorption when proceeding chiefly through interactions between CO 2(aq) and NH 3(aq). We further quantified the reaction kinetic constant of the CO 2–NH 3 reaction. Our results indicate that higher initial concentration of NH 4Cl ( ≥2mol∙L -1) leads to the precipitation of roguinite [(NH 4) 2Mg(CO 3) 2∙4H 2O], while nesquehonite appears to be the dominant Mg-carbonate without NH 4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO 2 mineral carbonation that indicates the potential of this technique for futuremore » application to industrial-scale CO 2 sequestration.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [3];  [1]
  1. Nanjing Univ. (China). School of Earth Sciences and Engineering
  2. Univ. of Southern California, Los Angeles, CA (United States). Department of Earth Sciences
  3. Nanjing Univ. (China). School of Earth Sciences and Engineering; George Washington Univ., Washington, DC (United States). Department of Chemistry
Publication Date:
Research Org.:
George Washington Univ., Washington, DC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1429294
Grant/Contract Number:  
FG02-02ER15366
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Minerals
Additional Journal Information:
Journal Volume: 7; Journal Issue: 9; Journal ID: ISSN 2075-163X
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 58 GEOSCIENCES; absorption rate; carbon dioxide; carbon capture and storage; magnesium carbonate

Citation Formats

Zhu, Chen, Wang, Han, Li, Gen, An, Siyu, Ding, Xiaofeng, Teng, Hui, and Zhao, Liang. CO2 Absorption and Magnesium Carbonate Precipitation in MgCl2–NH3–NH4Cl Solutions: Implications for Carbon Capture and Storage. United States: N. p., 2017. Web. doi:10.3390/min7090172.
Zhu, Chen, Wang, Han, Li, Gen, An, Siyu, Ding, Xiaofeng, Teng, Hui, & Zhao, Liang. CO2 Absorption and Magnesium Carbonate Precipitation in MgCl2–NH3–NH4Cl Solutions: Implications for Carbon Capture and Storage. United States. doi:10.3390/min7090172.
Zhu, Chen, Wang, Han, Li, Gen, An, Siyu, Ding, Xiaofeng, Teng, Hui, and Zhao, Liang. Tue . "CO2 Absorption and Magnesium Carbonate Precipitation in MgCl2–NH3–NH4Cl Solutions: Implications for Carbon Capture and Storage". United States. doi:10.3390/min7090172. https://www.osti.gov/servlets/purl/1429294.
@article{osti_1429294,
title = {CO2 Absorption and Magnesium Carbonate Precipitation in MgCl2–NH3–NH4Cl Solutions: Implications for Carbon Capture and Storage},
author = {Zhu, Chen and Wang, Han and Li, Gen and An, Siyu and Ding, Xiaofeng and Teng, Hui and Zhao, Liang},
abstractNote = {CO2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO2 gas to carbonates in MgCl2–NH3–NH4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limiting step of CO2 absorption when proceeding chiefly through interactions between CO2(aq) and NH3(aq). We further quantified the reaction kinetic constant of the CO2–NH3 reaction. Our results indicate that higher initial concentration of NH4Cl ( ≥2mol∙L-1) leads to the precipitation of roguinite [(NH4)2Mg(CO3)2∙4H2O], while nesquehonite appears to be the dominant Mg-carbonate without NH4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO2 sequestration.},
doi = {10.3390/min7090172},
journal = {Minerals},
number = 9,
volume = 7,
place = {United States},
year = {Tue Sep 19 00:00:00 EDT 2017},
month = {Tue Sep 19 00:00:00 EDT 2017}
}

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Works referenced in this record:

CO2 Mineral Sequestration: Chemically Enhanced Aqueous Carbonation of Serpentine
journal, June 2003

  • Park, Ah-Hyung Alissa; Jadhav, Raja; Fan, Liang-Shih
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mineral sequestration: physically activated dissolution of serpentine and pH swing process
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