Desulfurization reaction model and experimental analysis of high sulfur coal under hydrogen atmosphere

Guojie Zhang; Yannian Du; Yongfa Zhang; Ying Xu

Journal of Industrial and Engineering Chemistry, Vol.20, No.2, 487-493, March, 2014

DOI10.1016/j.jiec.2013.05.006 Export Citation

Desulfurization reaction model and experimental analysis of high sulfur coal under hydrogen atmosphere

Guojie Zhang^†, Yannian Du, Yongfa Zhang, and Ying Xu

Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, PR China

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The reaction between hydrogen and high-sulfur coal at high temperature was investigated. Crashed and sieved high-sulfur coal sample was placed in a 23 mm I.D. differential reactor. The release of hydrogen sulfide at run temperature and under different hydrogen atmospheres was recorded by a hydrogen sulfide detector. Desulfurization yield was obtained through the elemental analysis of residual char. The grain reaction and random pore models were modified to facilitate the description of reaction kinetics characteristics. Hydrogen was observed to promote the desulfurization rate considerably; i.e., more than 65% of sulfur in coal could be removed. The releasing curves of H2S in the hydropyrolysis process exhibited two peaks. The desulfurization process in the hydropyrolysis of high-sulfur coal could be regarded as two stages based on the evolution profiles of H2S. The first peak at 250-450 ℃ was derived from the desulfurization of aliphatic sulfide. The second peak at 450-650 ℃ was produced from the sulfur in pyrite and aromatic thiophenic structure. The desulfurization of high sulfur could be described more effectively with the grain reaction model than with the random pore model. The random pore model was only adopted in the initial stage of sulfur removal of high-sulfur coal under hydrogen atmosphere. The grain reaction model was adequate for the entire stage.

Keywords:High-sulfur coal;Hydropyrolysis desulfurization;Kinetics;Grain reaction model;Random pore model

[References]

Perraud I, Ayral RM, Rouessac F, Ayral A, Chem. Eng. J., 200-202, 1 (2012)
Tian Z, Wang Q, Bai S, Chem. Ind., 23, 53 (2009)
Wei J, Luo Y, Yu P, Cai B, Tan H, J. Ind. Eng. Chem., 15(1), 16 (2009)
Du Melle F, J. Power Sources, 71(1-2), 7 (1998)
Gungor A, Chem. Eng. J., 146(3), 388 (2009)
Fan W, Sun Y, Zhu T, Wen Y, Atmos. Environ., 56, 52 (2012)
Xu Q, Qian J, Coal Ash China, 4, 35 (2003)
Zhang YF, Zhang GJ, Zhao YQ, Li XL, Sun YL, Xu Y, Int. J. Hydrog. Energy, 37(8), 6363 (2012)
Zhang Y, Zhang G, Zhang B, Guo F, Sun Y, Chem. Eng. J., 173, 593 (2011)
Shang H, Du W, Liu Z, Zhang H, J. Ind. Eng. Chem., http://dx.doi.org/10.1016/j.jiec.2012.12.044 (2013)
Fu Z, Guo Z, Wang S, Chin. J. Process. Eng., 7, 910 (2007)
Sharma DK, Sulimma A, van Heek KH, Fuel, 65, 1571 (1986)
Stanczyk K, Kisielow W, Fuel, 73, 660 (1994)
Xu WC, Matsuoka K, Akiho H, Kumagai M, Tomita A, Fuel, 82(6), 677 (2003)
Chen H, Li B, Yang J, J. Fuel. Chem. Tech., 25, 114 (1997)
Guo H, Applied Chemical Engineering Kinetics, fourth ed., Chem. Ind. Press, Beijing, 2003. (2003)
Levenspiel O, Chemical Reaction Engineering, fourth ed., John Willey & Sons Inc., New York, 1999. (1999)
Liu J, Tang H, Guo Z, J. Ind. Eng., 155, 1335 (2004)
Lee KT, Koon OW, Chem. Eng. J., 146(1), 57 (2009)
Ishida M, Wen CY, Chem. Eng. Sci., 26, 1031 (1971)
Zhang G, Zhang Y, Xie K, Chem. Eng, 34, 55 (2006)
Miller BG, Clean. Coal. Eng. Tech., 133 (2011)
Hobbs ML, Radulovic PT, Smoot LD, Prog. Energy Combust. Sci., 19(6), 505 (1993)
Nowak MA, Paul AD, Srivastava RD, Radziwon A, Coal conversion, in: Encyclopedia of Energy, 2004, p. 425. (2004)
Chen P, J. Fuel. Chem. Tech., 25, 238 (1997)
Zhu Z, Cui H, Li Y, Environ. Chem., 14, 483 (1995)
Li B, Cao Y, Zhang J, Coal Conversion, 24, 6 (2001)
Yergey AL, Lampe FW, Vestal ML, Ind. Eng. Chem. Process Des. Dev., 13, 233 (1974)

[1] Perraud I, Ayral RM, Rouessac F, Ayral A, Chem. Eng. J., 200-202, 1 (2012)

[2] Tian Z, Wang Q, Bai S, Chem. Ind., 23, 53 (2009)

[3] Wei J, Luo Y, Yu P, Cai B, Tan H, J. Ind. Eng. Chem., 15(1), 16 (2009)

[4] Du Melle F, J. Power Sources, 71(1-2), 7 (1998)

[5] Gungor A, Chem. Eng. J., 146(3), 388 (2009)

[6] Fan W, Sun Y, Zhu T, Wen Y, Atmos. Environ., 56, 52 (2012)

[7] Xu Q, Qian J, Coal Ash China, 4, 35 (2003)

[8] Zhang YF, Zhang GJ, Zhao YQ, Li XL, Sun YL, Xu Y, Int. J. Hydrog. Energy, 37(8), 6363 (2012)

[9] Zhang Y, Zhang G, Zhang B, Guo F, Sun Y, Chem. Eng. J., 173, 593 (2011)

[10] Shang H, Du W, Liu Z, Zhang H, J. Ind. Eng. Chem., http://dx.doi.org/10.1016/j.jiec.2012.12.044 (2013)

[11] Fu Z, Guo Z, Wang S, Chin. J. Process. Eng., 7, 910 (2007)

[12] Sharma DK, Sulimma A, van Heek KH, Fuel, 65, 1571 (1986)

[13] Stanczyk K, Kisielow W, Fuel, 73, 660 (1994)

[14] Xu WC, Matsuoka K, Akiho H, Kumagai M, Tomita A, Fuel, 82(6), 677 (2003)

[15] Chen H, Li B, Yang J, J. Fuel. Chem. Tech., 25, 114 (1997)

[16] Guo H, Applied Chemical Engineering Kinetics, fourth ed., Chem. Ind. Press, Beijing, 2003. (2003)

[17] Levenspiel O, Chemical Reaction Engineering, fourth ed., John Willey & Sons Inc., New York, 1999. (1999)

[18] Liu J, Tang H, Guo Z, J. Ind. Eng., 155, 1335 (2004)

[19] Lee KT, Koon OW, Chem. Eng. J., 146(1), 57 (2009)

[20] Ishida M, Wen CY, Chem. Eng. Sci., 26, 1031 (1971)

[21] Zhang G, Zhang Y, Xie K, Chem. Eng, 34, 55 (2006)

[22] Miller BG, Clean. Coal. Eng. Tech., 133 (2011)

[23] Hobbs ML, Radulovic PT, Smoot LD, Prog. Energy Combust. Sci., 19(6), 505 (1993)

[24] Nowak MA, Paul AD, Srivastava RD, Radziwon A, Coal conversion, in: Encyclopedia of Energy, 2004, p. 425. (2004)

[25] Chen P, J. Fuel. Chem. Tech., 25, 238 (1997)

[26] Zhu Z, Cui H, Li Y, Environ. Chem., 14, 483 (1995)

[27] Li B, Cao Y, Zhang J, Coal Conversion, 24, 6 (2001)

[28] Yergey AL, Lampe FW, Vestal ML, Ind. Eng. Chem. Process Des. Dev., 13, 233 (1974)