Relationship between structural properties and CO2 capture performance of CaO-based sorbents obtained from different organometallic precursors

被引:107
作者
Lu, Hong [1 ]
Khan, Ataullah [1 ]
Smirniotis, Panagiotis G. [1 ]
机构
[1] Univ Cincinnati, Dept Chem & Mat Engn, Cincinnati, OH 45221 USA
关键词
D O I
10.1021/ie8002182
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
A series of CaO-based sorbents were synthesized from various organometallic precursors, namely, calcium propionate, calcium acetate, calcium acetylacetonate, calcium oxalate, and calcium 2-ethylhexanoate, by a simple calcination technique. In general, the five organometallic precursors (OMPs) exhibit a three-step weight loss regime in their respective thermogravimetic (TG) profiles. The first weight loss occurs because of dehydration in the temperature range of 50-200 degrees C. The second one results from decomposition leading to the formation of calcium carbonate in the temperature range of 450-550 degrees C. The calcium carbonate so formed then undergoes decarboxylation at higher temperatures of 710-750 degrees C and results in the formation of calcium oxide. Among the various precursors evaluated, CaO-sorbents obtained from calcium propionate and calcium acetate precursors were found to exhibit the highest CO(2) capture capacity. The observed results were correlated with the intrinsic properties of the precursors by means of various techniques like thermogravimetric analysis (TGA), pore-size distribution (PSD), and differential scanning calorimetry (DSC). It was found that these two sorbents possessed higher surface area and larger pore volume compared to other sorbents prepared in this work. Thermal decomposition of these two OMPs resulted in the maximum evolution of heat, which could eventually lead to the generation of larger macropores, thus explaining the resultant CO(2)-uptake capacity we observed. Interestingly, the CO(2) capture capacity of the sorbents was found to be directly proportional to the porosity per unit surface area. In summary, we were successful in correlating the intrinsic properties of an OMP to the eventual CO(2) capture capacity of the sorbent. From the present investigation, it seems that the amount of heat evolved during the course of decomposition plays a direct role in the resultant porosity and thereby regulates the eventual CO(2) capture capacity.
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页码:6216 / 6220
页数:5
相关论文
共 13 条
[1]   Separation of CO2 from flue gas:: A review [J].
Aaron, D ;
Tsouris, C .
SEPARATION SCIENCE AND TECHNOLOGY, 2005, 40 (1-3) :321-348
[2]   Cost structure of a postcombustion CO2 capture system using CaO [J].
Abanades, J. Carlos ;
Grasa, G. ;
Alonso, M. ;
Rodriguez, N. ;
Anthony, E. J. ;
Romeo, L. M. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (15) :5523-5527
[3]   Development of porous solid reactant for thermal-energy storage and temperature upgrade using carbonation/decarbonation reaction [J].
Aihara, M ;
Nagai, T ;
Matsushita, J ;
Negishi, Y ;
Ohya, H .
APPLIED ENERGY, 2001, 69 (03) :225-238
[4]   Post-combustion decarbonisation processes [J].
Bailey, DW ;
Feron, PHM .
OIL & GAS SCIENCE AND TECHNOLOGY-REVUE D IFP ENERGIES NOUVELLES, 2005, 60 (03) :461-474
[5]  
BARKER R, 1973, J APPL CHEM BIOTECHN, V23, P733
[6]   EFFECT OF THE PRODUCT LAYER ON THE KINETICS OF THE CO2-LIME REACTION [J].
BHATIA, SK ;
PERLMUTTER, DD .
AICHE JOURNAL, 1983, 29 (01) :79-86
[7]   Carbonation-calcination cycle using high reactivity calcium oxide for carbon dioxide separation from flue gas [J].
Gupta, H ;
Fan, LS .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2002, 41 (16) :4035-4042
[8]   Deactivation of Ca-based sorbents by coal-derived minerals during multicycle CO2 sorption under elevated pressure and temperature [J].
Kuramoto, K ;
Shibano, S ;
Fujimoto, S ;
Kimura, T ;
Suzuki, Y ;
Hatano, H ;
Lin, SY ;
Harada, M ;
Morishita, K ;
Takarada, T .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2003, 42 (15) :3566-3570
[9]   Repetitive carbonation-calcination reactions of Ca-based sorbents for efficient CO2 sorption at elevated temperatures and pressures [J].
Kuramoto, K ;
Fujimoto, S ;
Morita, A ;
Shibano, S ;
Suzuki, Y ;
Hatano, H ;
Lin, SY ;
Harada, M ;
Takarada, T .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2003, 42 (05) :975-981
[10]   Effect of preparation temperature on cyclic CO2 capture and multiple carbonation-calcination cycles for a new Ca-based CO2 sorbent [J].
Li, ZS ;
Cai, NS ;
Huang, YY .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2006, 45 (06) :1911-1917