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Received March 7, 2014
Accepted July 9, 2014
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Development of the Al2O3-supported NaNO3-Na2Mg(CO3)2 sorbent for CO2 capture with facilitated sorption kinetics at intermediate temperatures
Green Chemistry Process Research Division, Korea Research Institute of Chemical Technology, Daejeon 305-600, Korea 1Department of Fire Safety, Gwangju University, Gwangju 503-703, Korea
dklee@gwangju.ac.kr
Korean Journal of Chemical Engineering, January 2015, 32(1), 51-61(11), 10.1007/s11814-014-0195-z
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Abstract
For the development of a dry solid sorbent having quite fast CO2 sorption kinetics in an intermediate temperature range of 245-300 ℃ to be applicable to a riser-type fluidized bed carbonator, samples of Al2O3-supported MgCO3 (1.2mmol/g) promoted with different molar amounts of Na2CO3 (1.2, 1.8mmol/g) and/or NaNO3 (0.6mmol/g) were prepared by incipient wetness pore volume impregnation. For a reference, an unsupported bulk phase sorbent of NaNO3-Na2Mg(CO3)2 was also prepared. From the sorption reaction using a gas mixture containing CO2 by 2.5-10% at 1 bar for the sorbents after their activation to MgO, Al2O3-supported sorbents were featured by their rapid carbonation kinetics in contrast to the unsupported sorbent showing a quite slow carbonation behavior. The addition of Na2CO3 to the MgCO3/Al2O3 sorbent made MgO species more reactive for the carbonation, bringing about a markedly enhanced kinetic rate and conversion, as compared with the unpromoted MgCO3/Al2O3 sorbent having a small negligible reactivity. The addition of NaNO3 to MgCO3/Al2O3 or to Na2CO3-MgCO3/Al2O3 induced the same promotional effects, but to a lesser magnitude, as observed for the Na2CO3 addition. It was also characteristic for all these MgCO3-based sorbents that initial carbonation conversions with time appeared as sigmoid curves. For the Al2O3-supported sorbent comprised of NaNO3, Na2CO3, and MgCO3 by 0.6, 1.8, and 1.2mmols, respectively, per gram sorbent,_x000D_
showing the best kinetic performance, a kinetic equation capable of reflecting such sigmoid conversion behavior was established, and its applicability to a riser carbonator was examined throughout a simple model calculation based on the kinetics obtained.
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Abanades JC, Anthony EJ, Lu DY, Salvador C, Alvarez D, AIChE J., 50(7), 1614 (2004)
Yu CH, Huang CH, Tan CS, Aerosol Air Quality Res., 12, 745 (2012)
Kim K, Kim D, Park YK, Lee KS, Int. J. Greenhous Gas Control, 26, 135 (2014)
Iijima M, Nagayasu T, Kamijyo T, Nakatani S, Mitsubishi Heavy Industries Technical Review, 48, 26 (2011)
Yi CK, Jo SH, Seo Y, Lee JB, Ryu CK, Int. J. Greenhouse Gas Control, 1, 31 (2007)
Choi JH, Yi CK, Jo SH, Korean J. Chem. Eng., 28(4), 1144 (2011)
Veneman R, Li ZS, Hogendoorn JA, Kersten SRA, Brilman DWF, Chem. Eng. J., 207, 18 (2012)
Lee DK, Min DY, Seo H, Kang NY, Choi WC, Park YK, Ind. Eng. Chem. Res., 52(26), 9323 (2013)
Monazam ER, Shadle LJ, Miller DC, Pennline HW, Fauth DJ, Hoffman JS, Gray ML, AIChE J., 59(3), 923 (2013)
Zhang K, Li XS, Duan Y, King DL, Singh P, Li L, Int. J. Greenhouse Gas Control, 12, 351 (2013)
Mayorga SG, Weigel SJ, Gaffney TR, Brzozowski JR, US Patent, 6,280,503 B1 (2001)
Bauer T, Laing D, Kroner U, Tamme R, Int. J. Thermophys., 33, 91 (2012)
Berg RW, Kerridge DH, Larsen PH, J. Chem. Eng. Data, 51(1), 34 (2006)
Zhao CW, Chen XP, Zhao CS, Ind. Eng. Chem. Res., 51(44), 14361 (2012)
Zhao CW, Chen XP, Zhao CS, Energy Fuels, 26(2), 1401 (2012)
Patience GS, Chaouki J, Berruti F, Wong SR, Powder Technol., 72, 31 (1992)
Geankoplis CJ, Transport processes and separation process principles, 4th Ed., Prentice Hall, U.S.A. (2003)
Kunii D, Levenspiel O, Fluidization Engineering, Wiley, N.Y. (1969)