Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (1): 58-64.

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

收稿日期:2013-01-04 修回日期:2013-01-10 出版日期:2013-01-20 发布日期:2013-02-06
通讯作者: Yong Wang

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

Received:2013-01-04 Revised:2013-01-10 Online:2013-01-20 Published:2013-02-06
Contact: Yong Wang

摘要/Abstract

摘要： 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.

关键词: Guerbet reaction, alcohol condensation, zirconia, microcalorimetry, acetone condensation

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.

Key words: Guerbet reaction, alcohol condensation, zirconia, microcalorimetry, acetone condensation

Joseph T. Kozlowski, Robert J. Davis* . Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol[J]. 能源化学(英文), 2013, 22(1): 58-64.

Joseph T. Kozlowski, Robert J. Davis* . Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol[J]. Journal of Energy Chemistry, 2013, 22(1): 58-64.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.jenergychem.com/CN/

https://www.jenergychem.com/CN/Y2013/V22/I1/58

参考文献

[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
[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

Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol

Sodium modification of zirconia catalysts for ethanol coupling to 1-butanol

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	Yujun Zhao, Huanhuan Zhang, Yuxi Xu, Shengnian Wang, Yan Xu, Shengping Wang, Xinbin Ma. Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst[J]. 能源化学(英文版), 2020, 49(10): 248-256.
[2]	Yuefeng Song, Xiaomin Zhang, Yingjie Zhou, Houfu Lv, Qingxue Liu, Weicheng Feng, Guoxiong Wang, Xinhe Bao. Improving the performance of solid oxide electrolysis cell with gold nanoparticles-modified LSM-YSZ anode[J]. 能源化学(英文), 2019, 28(8): 181-187.
[3]	Zhiheng Ren, Peng Wang, Jiao Kong, Meijun Wang, Liping Chang. Structures and oxygen storage/release capacities of Ce_xZr_1-xO₂: Effects of Zr content and preparation method[J]. 能源化学(英文), 2017, 26(4): 647-654.
[4]	Qi Zhang, Jing Dong, Yongmei Liu, Yangdong Wang, Yong Cao. Towards a green bulk-scale biobutanol from bioethanol upgrading[J]. 能源化学(英文), 2016, 25(6): 907-910.
[5]	Min Chen, Zhanglong Guo, Jian Zheng, Fangli Jing, Wei Chu. CO₂ selective hydrogenation to synthetic natural gas (SNG) over four nano-sized Ni/ZrO₂ samples: ZrO₂ crystalline phase & treatment impact[J]. 能源化学(英文), 2016, 25(6): 1070-1077.
[6]	Weizhen Li, Hongpeng Zhang, Xiaohui He, Haichao Liu. Promoting effect of chloride ions on selective oxidation of methanol to methyl formate over zirconia-supported ruthenium oxide catalysts[J]. 能源化学(英文), 2013, 22(3): 512-516.
[7]	Hongpeng Zhang, Haichao Liu* . Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation[J]. 能源化学(英文), 2013, 22(1): 98-106.
[8]	Lian Wang, Qun Liu, Minghao Zhou, Guomin Xiao*. Synthesis of glycerin triacetate over molding zirconia-loaded sulfuric acid catalyst[J]. 能源化学(英文), 2012, 21(1): 25-28.
[9]	Mengdie Cai, Jie Wen*, Wei Chu, Xueqing Cheng, Zejun Li . Methanation of carbon dioxide on Ni/ZrO₂-Al₂O₃ catalysts: Effects of ZrO₂ promoter and preparation method of novel ZrO₂-Al₂O₃ carrier[J]. 能源化学(英文), 2011, 20(3): 318-324.
[10]	Yanqiao Zhao;*;Jixiang Chen;Jiyan Zhang. Effects of ZrO2 on the Performance of CuO-ZnO-Al2O3/HZSM-5 Catalyst for Dimethyl Ether Synthesis from CO2 Hydrogenation[J]. 能源化学(英文), 2007, 16(4): 389-392.
[11]	Xiulan Cai;Xinfa Dong;Weiming Lin. Autothermal Reforming of Methane over Ni Catalysts Supported on CuO-ZrO2-CeO2-Al2O3[J]. 能源化学(英文), 2006, 15(2): 122-126.
[12]	Mariana M. V. M. Souza;Octavio R. Macedo Neto;Martin Schmal. Synthesis Gas Production from Natural Gas on Supported Pt Catalysts[J]. 能源化学(英文), 2006, 15(1): 21-27.
[13]	Xinmei Liu;Gaoqing Lu;Zifeng Yan. Preliminary Synthesis and Characterization of Mesoporous Nanocrystalline Zirconia[J]. 能源化学(英文), 2003, 12 (3): 161-166.
[14]	Chunlin Li;Yilu Fu;Guozhu Bian;Tiandou Hu;Yaning Xie;Jing Zhan. CO2 Reforming of CH4 over Ni/CeO2-ZrO2-Al2O3 Prepared by Hydrothermal Synthesis Method[J]. 能源化学(英文), 2003, 12 (3): 167-177.
[15]	Renjin He;Yihua Ma. STUIDES ON THE CERAMIC MEMBRANE REACTOR FOR OXIDATIVE COUPLING OF METHANE[J]. 能源化学(英文), 1996, 5 (4): 306-319.