助剂促进的 Rh-Fe/Al2O3 催化剂上 CO 加氢制乙醇反应性能

doi:10.3724/SP.J.1088.2012.11215

催化学报 ›› 2012, Vol. 33 ›› Issue (6): 1007-1013.DOI: 10.3724/SP.J.1088.2012.11215

助剂促进的 Rh-Fe/Al₂O₃ 催化剂上 CO 加氢制乙醇反应性能

陈维苗1, 丁云杰1,2,*, 宋宪根1,3, 朱何俊1, 严丽1, 王涛1

1中国科学院大连化学物理研究所, 辽宁大连 116023; 2中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023; 3中国科学院研究生院, 北京 100049

收稿日期:2011-12-22 修回日期:2012-01-19 出版日期:2012-05-30 发布日期:2012-05-30

Performance of Promoted Rh-Fe/Al₂O₃ Catalysts for CO Hydrogenation to Ethanol

CHEN Weimiao1, DING Yunjie1,2,*, SONG Xiangeng1,3, ZHU Hejun1, YAN Li1, WANG Tao1

1Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 3Graduate University of Chinese Academy of Sciences, Beijing 100049

Received:2011-12-22 Revised:2012-01-19 Online:2012-05-30 Published:2012-05-30

摘要/Abstract

摘要： 考察了 Fe, Rh 载量以及助剂对 Rh-Fe/Al₂O₃ 催化剂上合成气制乙醇反应性能的影响. 结果表明, 随着 Fe 载量的增加, 甲醇选择性持续上升伴随着甲烷选择性的持续下降, 而乙醇选择性有最优值. 助剂的添加或多或少促进了甲醇耦合、CO 插入和解离的活性, 或抑制了催化剂加氢能力, 使得乙醇选择性有所上升, 甲醇选择性有所下降, 而烃类选择性变化不大. 随着 CO 加氢反应的进行, Rh-Fe/Al₂O₃ 催化剂上烃类选择性逐渐下降, 但甲醇的生成活性逐渐上升, 而乙醇选择性和生成活性逐渐下降; 然而, 助剂的添加并未提高催化剂的稳定性. 这可能是由于在反应过程中 Fe 物种逐渐被合成气还原使得乙醇生成活性位数量逐渐减少所致.

关键词: 铑, 铁, 氧化铝, 负载型催化剂, 一氧化碳, 加氢, 乙醇

Abstract: The effects of Rh and Fe loading, and promoters on CO hydrogenation performance over Rh-Fe/Al₂O₃ catalysts were investigated, as well as the stability of the catalysts. The results showed that with the increasing of Fe loading, methanol selectivity produced from syngas increased continuously accompanying by the decrease in methane selectivity, but the ethanol selectivity had a maximum value. The addition of alkaline or alkaline earth metals promoted methanol coupling or CO dissociation and insertion, or suppressed hydrogenation ability more or less, as a result, ethanol selectivity enhanced, and methanol selectivity decreased, but hydrocarbon selectivity remained almost unchanged. With CO hydrogenation reaction proceeding, hydrocarbon selectivity decreased, but methanol selectivity increased gradually, unfortunately, ethanol selectivity decreased, and the additions of promoters had little effect on it, probably due to the reduction of Fe species by syngas or decreasing of Rh-Fe interface areas during reaction.

Key words: rhodium, iron, alumina, supported catalyst, carbon monoxide, hydrogenation, ethanol

陈维苗, 丁云杰, 宋宪根, 朱何俊, 严丽, 王涛. 助剂促进的 Rh-Fe/Al₂O₃ 催化剂上 CO 加氢制乙醇反应性能[J]. 催化学报, 2012, 33(6): 1007-1013.

CHEN Wei-Miao, DING Yun-Jie, SONG Xian-Gen, ZHU He-Jun, YAN Li, WANG Tao. Performance of Promoted Rh-Fe/Al₂O₃ Catalysts for CO Hydrogenation to Ethanol[J]. Chinese Journal of Catalysis, 2012, 33(6): 1007-1013.

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参考文献

1 Subramani V, Gangwal S K. Energy Fuels, 2008, 22: 814
2 Subramanian N D, Gao J, Mo X, Goodwin J G, Rorres W, Spivey J J. J Catal, 2010, 272: 204
3 Gao J, Mo X, Chien A C-Y, Torres W, Goodwin J G Jr. J Catal, 2009, 262: 119
4 Wang J, Zhang Q, Wang Y. Catal Today, 2011, 171: 257
5 陈明英, 翁维正, 华卫琦, 伊晓东, 万惠霖. 催化学报 (Chen M Y, Weng W Zh, Hua W Q, Yi X D, Wan H L. Chin J Catal), 2011, 32: 672
6 Chen G, Guo C, Huang Z, Yuan G. Chem Eng Res Des, 2011, 89: 249
7 Chen G, Guo C, Zhang X, Huang Z, Yuan G. Fuel Process Technol, 2011, 92: 456
8 Fan Z, Chen W, Pan X, Bao X. Catal Today, 2009, 147: 86
9 Pan X L, Fan Z L, Chen W, Ding Y J, Luo H Y, Bao X H. Nat Mater, 2007, 6: 507
10 黄利宏, 储伟, 洪景萍, 罗仕忠. 催化学报 (Huang L H, Chu W, Hong J P, Luo Sh Zh. Chin J Catal), 2006, 27: 596
11 Ngo H, Liu Y, Murata K. React Kinet Mech Catal, 2011, 102: 425
12 Wang K, Cook R A. US 200710 004 588. 2007
13 Haider M A, Gogate M R, Davis R J. J Catal, 2009, 261: 9
14 Gogate M R, Davis R J. Catal Commun, 2010, 11: 901
15 Gogate M R, Davis R J. ChemCatChem, 2009, 1: 295
16 Egbebi A, Schwartz V, Overbury S H, Spivey J J. Catal Today, 2010, 149: 91
17 Schwartz V, Campos A, Egbebi A, Spivey J J, Overburg S H. ACS Catal, 2011, 1: 1298
18 Liu Y, Murata K, Inaba M, Takahara I, Okabe K. Catal Today, 2011, 164: 308
19 Burch R, Hayes M J. J Catal, 1997, 165: 249
20 Ojeda M, Granados M L, Rojas S, Terreros P, Garcia-Garcia J L G, Fierro J L G. Appl Catal A, 2004, 261: 47
21 Zakumbaeva G D, Beketaeva L A, Uvaliev T Yu, Khlystov A S, Litvyakova E N. React Kinet Catal Lett, 1985, 28: 425
22 李经伟, 丁云杰, 林荣和, 龚磊峰, 宋宪根, 陈维苗, 王涛, 罗洪原. 催化学报 (Li J W, Ding Y J, Lin R H, Gong L F, Song X G, Chen W M, Wang T, Luo H Y. Chin J Catal), 2010, 31: 365
23 Chen W M, Ding Y J, Song X G, Wang T, Luo H Y. Appl Catal A, 2011, 407: 231
24 Niemantsverdriet J W, van der Kraan A M, Delgass W N. J Catal, 1984, 89: 138
25 Ichikawa M, Fukushima T, Shikakura K. (Proceedings of 8th International Congress on Catalysis, II.
26 Fukuoka A, Ichikawa M, Hriljac J A, Shriver D F. Inorg Chem, 1987, 26: 3643
27 Bowker M. Catal Today, 1992, 15: 77
28 Ichikawa M, Fukushima T. J Chem Soc, Chem Commun, 1985: 321
29 Egbebi A, Spivey J J. Catal Commun, 2008, 9: 2308
30 Zhang X, Li Z, Guo Q, Zheng Y, Xie K. Fuel Process Technol, 2010, 91: 379
31 Hargis D C, Dubeck M. US 4 309 314. 1982
32 Hargis D C, Dubeck M. US 4 370 507. 1983
33 Xu M, Iglesia E. J Catal, 1999, 188: 125
34 Khodakov A, Chu W, Fongarland P. Chem Rev, 2007, 107: 1692
35 Hayashi H, Chen L Z, Tago T, Kishida M, Wakabayashi K. Appl Catal A, 2002, 231: 81

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助剂促进的 Rh-Fe/Al₂O₃ 催化剂上 CO 加氢制乙醇反应性能

Performance of Promoted Rh-Fe/Al₂O₃ Catalysts for CO Hydrogenation to Ethanol

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