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Journal of Energy Chemistry 2013, Vol. 22 Issue (1) :58-64    DOI:
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Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol

Joseph T. Kozlowski, Robert J. Davis*

Department of Chemical Engineering, University of Virginia, 102 Engineers Way Charlottesville, VA 22904-4741, USA


Abstract

 The influences of adding sodium to zirconia on the acid-base properties of the surface and on the catalytic conversion of ethanol and acetone were investigated. The rates of ethanol dehydration, dehydrogenation and coupling were evaluated in a fixed-bed flow reactor operating at temperatures from 613 to 673 K. The rate of acetone condensation was evaluated in the same reactor operating at 473-573 K. Addition of 1.0 wt% Na to ZrO2 decreased the rate of ethanol dehydration by more than an order of magnitude, which was consistent with a neutralization of acid sites evaluated by ammonia adsorption microcalorimetry. Addition of 1.0 wt% Na to ZrO2 also increased the base site density quantified by carbon dioxide adsorption microcalorimetry and the rate of acetone condensation. Although the rate of ethanol coupling was not increased by the addition of Na, the overall selectivity of ethanol to butanol was improved over the 1.0 wt% Na/ZrO2 sample because of the significant inhibition of ethanol dehydration.
Keywords: Guerbet reaction alcohol condensation zirconia microcalorimetry acetone condensation   
Received: 2013-01-04; published: 2013-02-06
Corresponding Authors: Yong Wang  Email: rjd4f@virginia.edu
Cite this article:   
Joseph T. Kozlowski, Robert J. Davis* .Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol[J]  Journal of Energy Chemistry, 2013,V22(1): 58-64
URL:  
http://www.jenergchem.org/EN/     或     http://www.jenergchem.org/EN/Y2013/V22/I1/58
[1] Kirk-Othmer Publishing, Kirk-Othmer Encyclopedia of Chemical Technology, 5th ed., Wiley-Interscience, New York, 2004
[2] Guerbet M. Acad C R Sci Paris, 1899, 1002
[3] Wibaut J P. U. S. Patent 19105821933
[4] Fuchs O. U. S. Patent 19924801931
[5] Tsuchida T, Kubo J, Yoshioka T, Sakuma S, Takeguchi T, Ueda W. J Catal, 2008, 259: 183
[6] Koda K, Matsu-Ura T, Obora Y, Ishii Y. Chem Lett, 2009, 38: 838
[7] Ogo S, Onda A, Iwasa Y, Hara K, Fukuoka A, Yanagisawa K. J Catal, 2012, 296: 24
[8] Ogo S, Onda A, Yanagisawa K. Appl Catal A, 2011, 402: 188
[9] Gines M J L, Iglesia E. J Catal, 1998, 176: 155
[10] Di Cosimo J I, Diez V K, Xu M, Iglesia E, Apesteguia C R. J Catal, 1998, 178: 499
[11] Di Cosimo J I, Apesteguía C R, Ginés M J L, Iglesia E. J Catal, 2000, 190: 261
[12] Ndou A S, Plint N, Coville N J. Appl Catal A, 2003, 251: 337
[13] Ndou A S, Coville N J. Appl Catal A, 2004, 275: 103
[14] Jones M D, Keir C G, Di Iulio C, Robertson R A M, Williams C V, Apperley D C. Catal Sci Technol, 2011, 1: 267
[15] Sun J M, Zhu K K, Gao F, Wang C M, Liu J, Peden C H F, Wang Y. J Am Chem Soc, 2011, 133: 11096
[16] Ueda W, Kuwabara T, Ohshida T, Morikawa Y. J Chem Soc Chem Commun, 1990, 1558
[17] Axpuac S, Aramendía M A, Hidalgo-Carrillo J, Marinas A, Marinas J M, Montes-Jiménez V, Urbano F J, Borau V. Catal Today, 2012, 187: 183
[18] Minambres J F, Aramendía M A, Marinas A, Marinas J M, Urbano F J. J Mol Catal A, 2011, 338: 121
[19] Urbano F J, Aramendía M A, Marinas A, Marinas J M. J Catal, 2009, 268: 79
[20] López D E, Goodwin J G, Bruce D A, Lotero E. Appl Catal A, 2005, 295: 97
[21] Tanabe K, Yamaguchi T. Catal Today, 1994, 20: 185
[22] Zaki M I, Hasan M A, Pasupulety L. Langmuir, 2001, 17: 768
[23] Tai J, Davis R J. Catal Today, 2007, 123: 42
[24] Aramendía A M, Boráu V, Jimenez C, Marinas J M, Porras A, Urbano F J. J Chem Soc Faraday Trans, 1997, 93: 1431
[25] Cutrufello M S, Ferino I, Monaci R, Rombi E, Solinas V. Top Catal, 2002, 19: 225
[26] Yamaguchi T. Catal Today, 1994, 20: 199
[27] Lauron-Pernot H. Catal Rev-Sci Eng, 2006, 48, 315
[28] Marcu I, Tichit D, Fajula F, Tanchoux N. Catal Today, 2009, 147: 231
[29] Ordónez S, Díaz E, León M, Faba L. Catal Today, 2010, 167: 71
[30] Dvornikoff M N, Farrar M W. J Org Chem, 1957, 22: 540
[31] León M, Díaz E, Ordónez S. Catal Today, 2011, 164: 436
[32] Tsuchida T, Sakuma S, Takeguchi T, Ueda W. Ind Eng Chem, 2006, 45: 8634
[33] Carvalho D L, de Avillez R R, Rodrigues M T, Borges L E P, Appel L G. Appl Catal A, 2012, 96: 415
[34] Nagaraja V, Kuloor N R. Indian J Technol, 1966, 4: 46
[35] Nagaraja V. Indian J Technol, 1971, 9: 380
[36] Bordawekar S V, Doskocil E J, Davis R J. Langmuir, 1998, 14: 1734
[37] Bordawekar S V, Davis R J. J Catal, 2000, 189: 79
[38] Doskocil E J, Bordawekar S V, Davis R J. J Catal, 1997, 169: 327
[39] Bordawekar S V, Doskocil E J, Davis R J. Catal Lett, 1997, 44: 193
[40] Kozlowski J T, Aronson M T, Davis R J. Appl Catal B, 2010, 96: 508
[41] Auroux A, Gervasini A. J Phys Chem, 1990, 94: 6371
[42] Coluccia S, Garrone E, Borello E. J Chem Soc Faraday Trans, 1983, 79: 607
[43] Tsyganenko A A, Pozdnyakov D V, Filimonov V N. J Mol Struct, 1975, 29: 299
[44] Climent M J, Corma A, Fornés V, Guil-Lopez R, Iborra S. Adv Synth Catal, 2002, 344: 1090 3.0.CO;2-X target="_blank">
[45] Sádaba I, Ojeda M, Mariscal R, Fierro J L G, Granados M L. Appl Catal B, 2011, 101: 638
[46] Iglesia E, Barton D G, Biscardi J A, Gines M J L, Soled S L. Catal Today, 1997, 38: 339
[47] Birky T W, Kozlowski J T, Davis R J. J Catal, In Press, DOI: 10.1016/j. jcat.2012.11.014
[48] Rekoske J E, Barteau M A. Ind Eng Chem Res, 2011, 50: 41
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