TY - JOUR
T1 - Experimental study and atomic level description of adsorption process of CO2 on doped alkaline earth oxides
AU - Sasaki, Kohei
AU - Wakuta, Koji
AU - Tokuda, Natsuki
AU - Belosludov, Rodion V.
AU - Ueda, Shigeru
AU - Inoue, Ryo
AU - Kawazoe, Yoshiyuki
AU - Ariyama, Tatsuro
N1 - Funding Information:
We would like to thank Werner Vogelsang for providing the theoretical calculations used in this paper. We ?>also thank the Fermilab staff and the technical staffs ?>of the participating institutions for their vital con ?>tributions. This work was supported by the U.S. Department of Energy and National Science Foundation; the Italian Istituto Nazionale di Fisica Nucleare; the Ministry of Education, Culture, Sports, Science and Technology of Japan; the Natural Sciences and Engineering Research Council of Canada; the National Science Council of the Republic of China; the Swiss National Science Foundation; the A. P. Sloan Foundation; the Bundesministerium fuer Bildung und Forschung, Germany; the Korean Science and Engineering Foundation and the Korean Research Foundation; the Particle Physics and Astronomy Research Council and the Royal Society, UK; the Russian Foundation for Basic Research; the Comision Interministerial de Ciencia y Tecnologia, Spain; work supported in part by the European Community’s Human Potential Programme under Contract No. HPRN-CT-20002, Probe for New Physics; and this work was supported by Research Fund of Istanbul University Project No. 1755/21122001.
PY - 2012
Y1 - 2012
N2 - To realize CO2 capture and storage, many methods for CO 2 sequestration should be investigated from a long-term viewpoint. The development of novel CO2 absorbent material is considered to be a candidate for the effective CO2 sequestration. Investigation of CO2 absorbent material is usually based on the experiment with following thermodynamic analysis of obtained data. Recently, the introduction of large-scale simulation based on modern computational chemistry methods is found to be a powerful approach in order to explain and understand the experimental data. In the present study, the experimental measurements and ab-initio calculations were employed for studying the adsorption process of CO2 on both clean and doped CaO (001) surface. The effect of addition of other alkaline earth metal oxide to CaO on adsorption energy of CO2 was analyzed in detail. The relationship between the standard free energy change of carbonation of added alkaline earth metal oxide and extent of variation in the adsorption energy was not clear. However, the structural deformation of CaO surface caused by formation of compound or solid solution would vary the adsorption energy and in the case of CaO/BeO, it leads to significantly improve the capture of carbon dioxide during the first step of adsorption process. Reactivity of CaO with CO2 was investigated by experimental. The experimental results agree with calculation result. Atomistic level description of adsorption process of CO2 on the doped alkaline earth oxides was successfully carried out by ab-initio calculations.
AB - To realize CO2 capture and storage, many methods for CO 2 sequestration should be investigated from a long-term viewpoint. The development of novel CO2 absorbent material is considered to be a candidate for the effective CO2 sequestration. Investigation of CO2 absorbent material is usually based on the experiment with following thermodynamic analysis of obtained data. Recently, the introduction of large-scale simulation based on modern computational chemistry methods is found to be a powerful approach in order to explain and understand the experimental data. In the present study, the experimental measurements and ab-initio calculations were employed for studying the adsorption process of CO2 on both clean and doped CaO (001) surface. The effect of addition of other alkaline earth metal oxide to CaO on adsorption energy of CO2 was analyzed in detail. The relationship between the standard free energy change of carbonation of added alkaline earth metal oxide and extent of variation in the adsorption energy was not clear. However, the structural deformation of CaO surface caused by formation of compound or solid solution would vary the adsorption energy and in the case of CaO/BeO, it leads to significantly improve the capture of carbon dioxide during the first step of adsorption process. Reactivity of CaO with CO2 was investigated by experimental. The experimental results agree with calculation result. Atomistic level description of adsorption process of CO2 on the doped alkaline earth oxides was successfully carried out by ab-initio calculations.
KW - Ab-initio calculation
KW - Absorption
KW - CaO
KW - Double oxide system
KW - Global warming
KW - Solid absorption material
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U2 - 10.2355/isijinternational.52.1233
DO - 10.2355/isijinternational.52.1233
M3 - Article
AN - SCOPUS:84864971758
VL - 52
SP - 1233
EP - 1240
JO - Transactions of the Iron and Steel Institute of Japan
JF - Transactions of the Iron and Steel Institute of Japan
SN - 0915-1559
IS - 7
ER -