性能优异的Rh改性的Pd/Al2O3密偶催化剂

催化学报 , 2015, (2): 229-236. doi: 10.1016/S1872-2067(14)60214-X

性能优异的Rh改性的Pd/Al2O3密偶催化剂

方瑞梅 ^1, , 崔亚娟 ^2, , 陈思洁 ^3, , 尚鸿燕 ^4, , 史忠华 ^5, , 龚茂初 ^6, , 陈耀强 ^7,

1.四川大学化学工程学院，四川成都610064; 四川大学化学学院绿色化学与技术教育部重点实验室，四川成都610064

2.四川大学建筑与环境学院，四川成都610064; 四川大学化学学院绿色化学与技术教育部重点实验室，四川成都610064

3.四川大学化学学院绿色化学与技术教育部重点实验室,四川成都,610064

4.四川大学化学工程学院，四川成都610064; 四川大学化学学院绿色化学与技术教育部重点实验室，四川成都610064

5.四川大学化学学院绿色化学与技术教育部重点实验室,四川成都,610064

6.四川大学化学学院绿色化学与技术教育部重点实验室,四川成都,610064

7.四川大学化学工程学院，四川成都610064; 四川大学化学学院绿色化学与技术教育部重点实验室，四川成都610064

基金项目: 国家自然科学基金(21173153) 国家高技术研究发展计划(863计划,2013AA065304) 四川省科技厅科技支撑项目(2011GZ0035,2012FZ0008)

关键词：密偶催化剂 , 钯 , 铑 , 丙烷 , 直接氧化反应 , 还原反应 , 蒸汽重整反应

A highly efficient Rh-modified Pd/Al2O3 close-coupled catalyst

Keywords： Close-coupled catalyst , Palladium , Rhodium , Propane , Direct oxidation reaction , Reduction reaction , Steam reforming reaction

采用等体积浸渍法制备了Pd/Al2O3和Rh-Pd/Al2O3密偶催化剂，运用H2程序升温还原、CO化学吸附和X射线光电子能谱等手段对催化剂进行了表征，并考察了催化剂对丙烷总包反应和单反应的转化活性.总包反应结果表明， Rh的添加使起燃温度和完全转化温度分别降低了23和18oC.单反应结果证明，添加Rh能提高各单反应丙烷的转化活性，尤其是有NO参与的反应.表征结果证明，掺杂Rh不仅可以抑制活性组分PdOx的烧结，提高PdOx的分散度，而且可以改变其电子状态.

The close‐coupled catalysts Pd/Al2O3 and Rh‐Pd/Al2O3 were prepared by the impregnation method and characterized by H2 temperature‐programmed reduction, CO chemisorption, and X‐ray photoe‐lectron spectroscopy. Both overall catalytic activity and specific reactions associated with C3H8 elimination were assessed. The light‐off temperature and complete conversion temperature de‐creased by 23 and 18 °C, respectively, upon addition of Rh to the Pd/Al2O3 catalyst. The addition of Rh promotes the catalytic activity during C3H8 reactions, particularly in the presence of NO. The introduction of Rh not only inhibits sintering of PdOx and increases the dispersion of these same species, but also changes the electronic state of the PdOx in the catalyst.

参考文献

[1]	Zhu J, Zhang L L, Deng Y, Liu B, Dong L H, Gao F, Sun K Q, Dong L, Chen Y. Appl Catal B, 2010, 96:449,2010.
[2]	Li Z Q, Meng M, Dai F F, Hu T D, Xie Y N, Zhang J. Fuel, 2012, 93:606,2012.
[3]	Yu Q, Yao X J, Zhang H L, Gao F, Dong L. Appl Catal A, 2012, 423-424:42,2012.
[4]	Heck R M, Farrauto R J. Appl Catal A, 2001, 221:443,2001.
[5]	Kašpar J, Fornasiero P, Hickey N. Catal Today, 2003, 77:419,2003.
[6]	Fang R M, He S N, Cui Y J, Shi Z H, Gong M C, Chen Y Q. Chin J Catal(方瑞梅, 何胜楠, 崔亚娟, 史忠华, 龚茂初, 陈耀强. 催化学报), 2012, 33:1014,2012.
[7]	Wang G, Meng M, Zha Y Q, Ding T. Fuel, 2010, 89:2244,2010.
[8]	Kašpar J, Fornasiero P, Graziani M. Catal Today, 1999, 50:285,1999.
[9]	Neyertz C, Volpe M, Gigola C. Appl Catal A, 2004, 277:137,2004.
[10]	Spinicci R, Tofanari A. Appl Catal A, 2002, 227:159,2002.
[11]	Wilcox L, Burnside G, Kiranga B, Shekhawat R, Mazumder M K, Hawk R M, Lindquist D A, Burton S D. Chem Mater, 2003, 15:51,2003.
[12]	Wu X D, Yang B, Weng D. J Al oys Compd, 2004, 376:241,2004.
[13]	Liotta L F, Macaluso A, Arena G E, Livi M, Centi G, Deganello G. Catal Today, 2002, 75:439,2002.
[14]	Chen X Y, Liu Y, Niu G X, Yang Z X, Bian M Y, He A D. Appl Catal A, 2001, 205:159,2001.
[15]	Monteiro R S, Dieguez L C, Schmal M. Catal Today, 2001, 65:77,2001.
[16]	Fujimoto K-i, Ribeiro F H, Avalos-Borja M, Iglesia E. J Catal, 1998, 179:431,1998.
[17]	Briot P, Primet M. Appl Catal, 1991, 68:301,1991.
[18]	Rassoul M, Gaillard F, Garbowski E, Primet M. J Catal, 2001, 203:232,2001.
[19]	Farrauto R J, Lampert J K, Hobson M C, Waterman E M. Appl Catal B, 1995, 6:263,1995.
[20]	Narui K, Yata H, Furuta K, Nishida A, Kohtoku Y, Matsuzaki T. Appl Catal A, 1999, 179:165,1999.
[21]	Ahlström-Silversand A F, Odenbrand C U I. Appl Catal A, 1997, 153:157,1997.
[22]	Yao Y L, Fang R M, Shi Z H, Gong M C, Chen Y Q. Chin J Catal(姚艳玲, 方瑞梅, 史忠华, 龚茂初, 陈耀强. 催化学报), 2011, 32:589,2011.
[23]	Narui K, Furuta K, Yata H, Nishida A, Kohtoku Y, Matsuzaki T. Catal Today, 1998, 45:173,1998.
[24]	Wang Y, Shang H Y, Xu H D, Gong M C, Chen Y Q. Chin J Catal(王云,尚鸿燕, 徐海迪, 龚茂初, 陈耀强. 催化学报), 2014, 35:1157,2014.
[25]	Bonarowska M, Pielaszek J, Juszczyk W, Karpiński Z. J Catal, 2000, 195:304,2000.
[26]	Zhao B, Wang Q Y, Li G F, Zhou R X. J Environ Chem Eng, 2013, 1:534,2013.
[27]	Liu J Y, Zhao M, Xu C H, Liu S Y, Zhang X Q, Chen Y Q. Chin J Catal(刘建英, 赵明, 徐成华, 刘盛余, 张雪乔, 陈耀强. 催化学报), 2013, 34:751,2013.
[28]	Kobayashi T, Yamada T, Kayano K. Appl Catal B, 2001, 30:287,2001.
[29]	Maione A, André F, Ruiz P. Appl Catal A, 2007, 333:1,2007.
[30]	Bourane A, Derrouiche S, Bianchi D. J Catal, 2004, 228:288,2004.
[31]	Usami Y, Kagawa K, Kawazoe M, Matsuma Y, Sakurai H, Haruta M. Appl Catal A, 1998, 171:123,1998.
[32]	Shinjoh H, Muraki H, Fujitani Y. Appl Catal, 1989, 49:195,1989.
[33]	Mannila P, Salmi T, Haario H, Luoma M, Härkönen M, Sohlo J. Appl Catal B, 1996, 7:179,1996.
[34]	Li Y, Wang X X, Xie C, Song C S. Appl Catal A, 2009, 357:213,2009.
[35]	Yan C Y, Lan L, Chen S H, Zhao M, Gong M C, Chen Y Q, Chin J Catal(闫朝阳, 兰丽, 陈山虎, 赵明, 龚茂初, 陈耀强. 催化学报), 2012, 33:336,2012.

上一张下一张

计量

下载量()
访问量()

作者相关

文章评分

您的评分：
1

0%
2

0%
3

0%
4

0%
5

0%

材料期刊网