氧化铝载体和氧化钡助剂对钌基氨合成催化剂结构和性能的影响

doi:10.3866/PKU.WHXB20101223

Abstract

Abstract:

A series of Ba-Ru/Al₂O₃ catalysts were prepared by the impregnation method using industrial alumina (Al₂O₃-1) and synthesized alumina (Al₂O₃-2) as supports. The catalysts were characterized by X-ray diffraction, N2 adsorption-desorption, X-ray fluorescence spectroscopy, transmission electron microscopy, H₂ temperature-programmed reduction, NH₃ temperature-programmed desorption, and X-ray photoelectron spectroscopy. The effect of Al₂O₃ and the BaO promoter on the phase structure, texture properties, morphology, surface properties, and catalytic activity in ammonia synthesis were investigated. The results indicate that the physical and chemical properties of Al₂O₃ have a strong impact on the structure and activity of the ruthenium catalysts. The BaO promoter has a strong impact on the ruthenium catalyst in two ways: first, the amount of BaO added leads to a difference in the interaction between BaO and γ-Al₂O₃, which further influences the specific area and the porous structure of the catalysts; second, the addition of BaO influences the reduction process and the surface acidity and alkaline properties of the ruthenium catalysts. A proper amount of BaO promotes the activity and the optimal amount of BaO depends on the properties of the supports.

Key words: Ammonia synthesis, γ-Al₂O₃, Support, Ruthenium, Reduce, Acidity

MSC2000:

O643.3

YANG Xiao-Long, XIA Chun-Gu, TANG Li-Ping, XIONG Xu-Mao, MU Xin-Yuan, HU Bin. Effect of Alumina Support and Barium Oxide on the Structure and Catalytic Activity of Ruthenium Catalysts for Ammonia Synthesis[J].Acta Phys. -Chim. Sin., 2010, 26(12): 3263-3272.

References

1. Liang, C. H.; Wei, Z. B.; Xin, Q.; Li, C. Appl. Catal. A., 2001, 208: 193
2. Yang, X. L.; Hu, B.; Xia, C. G.; Xiong, X. M.; Mu, X. Y. Ind. Catal., 2010, 18: 5
[杨晓龙, 胡斌, 夏春谷, 熊绪茂, 慕新元. 工业催化, 2010, 18: 5]
3. You, Z. X.; Inazu, K.; Aika, K.; Baba, T. J. Catal., 2007, 251: 321
4. Zhang, X. B.; Li, X. N.; Huo, C.; Cen, Y. Q.; Zhu, Y. F.; Liu, H. Z. Chin. J. Catal., 2002, 23: 207
[张新波, 李小年, 霍超, 岑亚青, 祝一峰, 刘化章. 催化学报, 2002, 23: 207]
5. Szmigiel, D.; Raróg-Pilecka, W.; MiSkiewicz, E.; Gliński, M.; Kielak, M.; Kaszkur, Z.; Kowalczyk, Z. Appl. Catal. A, 2004, 273: 105
6. Xu, Q. C.; Lin, J. D.; Fu, X. Z.; Liao, D. W. Catal. Commun., 2008, 9: 1214
7. Ni, J.;Wang, R.; Lin, J. X.;Wei, K. M. Acta Phys. -Chim. Sin., 2009, 25(3): 519
[倪军, 王榕, 林建新, 魏可镁. 物理化学学报, 2009, 25(3): 519]
8. Luo, X. J.;Wang, R.; Ni, J.; Lin, J. X.; Lin, B. Y.; Xu, X. M.;Wei, K. M. Catal. Lett., 2009, 133: 382
9. Larichev, Y. V.; Moroz, B. L.; Zaikovskii, V. L.; Yunusov, S. M.; Kalyuzhnaya, E. S.; Shur, V. B.; Bukhtiyarov, V. I. J. Phys. Chem. C, 2007, 111: 9427
10. Miyazaki, A.; Balint, I.; Aika, K.; Nakano, Y. J. Catal., 2001, 204: 364
11. Kadowaki, Y.; Aika, K. J. Catal., 1996, 161: 178
12. Siporin, S. E.; Davis, R. J. J. Catal., 2004, 225: 359
13. Wang, R.;Wei, K. M.; Lin, J. X.; Yu, X. J.; Mao, S. L. Ind. Catal., 2005, 13: 31
[王榕, 魏可镁, 林建新, 俞秀金, 毛树禄. 工业催化, 2005, 13: 31]
14. Mao, S. L.; Wang, R.; Yu, X. J.; Lin, J. X.;Wei, K. M. Chin. Rare Earth, 2004, 25: 18
[毛树禄, 王榕, 俞秀金, 林建新, 魏可镁. 稀土, 2004, 25: 18]
15. Fu,W. J. The Preparation and Study of the Ruthenium Catalysts for Ammonia Synthesis
[D]. Fuzhou: Fuzhou University, 2003
[傅武俊. 钌催化剂的制备及氨合成催化性能的研究
[D]. 福州: 福州大学, 2003]
16. Liu, H. Z. Ammoina synthesis catalysis: practice and theory. Beijing: Chemical Industry Press, 2007: 309, 293
[刘化章. 氨合成催化剂实践与理论. 北京: 化学工业出版社, 2007: 309, 293]
17. Okal, J. Catal. Commun. 2010, 11: 508
18. Huo, C.; Yan, G.; Zheng, Y. F.; Yu, F.W.; Liu, H. Z. Chin. J. Catal., 2007, 28: 484
[霍超, 晏刚, 郑遗凡, 于凤文, 刘化章. 催化学报, 2007, 28: 484]
19. Sharma, L. D.; Kumar, M.; Saxena, A. K.; Chand, M.; Gupta, J. K. J. Mol. Catal. A, 2002, 185: 135
20. Li,Y.; Yang, Q. H.; Yang, J.; Li, C. Microporous Mesopor Mat., 2006, 91: 85
21. Yuan, Z. Y.;Wang, J. Z.; Zhang, Z. L.; Chen, T. H.; Li, H. X. Microporous Mesoporous Mat., 2001, 43: 227
22. Groen, J. C.; Pérez-Ramírez, J. Appl. Catal. A, 2004, 268: 121
23. Jacobsen, C. J. H.; Dahl, S.; Hansen, P. L.; Törnqvist, E.; Jensen, L.; Topsφe, H.; Prip, D. V.; Mφenshaug, P. B.; Chorkendorff, I. J. Mol. Catal. A, 2000, 163: 19
24. Seetharamulu, P.; Siva Kumar, V.; Padmasri, A. H.; David Raju, B.; Rama Rao, K. S. J. Mol. Catal. A, 2007, 263: 253
25. Seetharamulu, P.; Hari Prasad Reddy, K.; Padmasri, A. H.; Rama Rao, K. S.; David Raju, B. Catal. Today, 2009, 141: 94
26. Huo, C.; Xia, Q. H.; Luo, Y.; Yang, X. Z.; Liu, H. Z. Chin. J. Catal., 2009, 30: 537
[霍超, 夏庆华, 骆燕, 杨霞珍, 刘化章. 催化学报, 2009, 30: 537-542]
27. Hanse, T.W.;Wagner, J. B.; Hansen, P. L.; Dahl, S.; Topsφe, H.; Jacobsen, C. J. H. Science, 2001, 294: 1508
28. Dahl, S.; Logadottir, A.; Jacobsen, C. J. H.; Nφrskov, J. K. Appl. Catal. A, 2001, 222: 19
29. Zhao, Y. Ind. Catal., 2002, 10: 54
[赵琰, 工业催化, 2002, 10: 54]
30. Walker, G. S.; Pyke, D. R.;Werrett, C. R.;Williams, E.; Bhattacharya, A. K. Appl. Surf. Sci., 1999, 147: 228
31. Somorjai, G. A. Science, 1978, 201: 489
32. Nagai, M.; Koizumi, K.; Omi, S. Catal. Today, 1997, 35: 393
33. Elmasides, C.; Kondarides, D. I., Grünert,W.; Verykios, X. E. J. Phys. Chem. B, 1999, 103: 5227

[1]	Peng PENG,Hongtao LIU,Bin WU,Qingxin TANG,Yunqi LIU. Nitrogen Doped Graphene with a p-Type Field-Effect and Its Fine Modulation [J]. Acta Physico-Chimica Sinica, 2019, 35(11): 1282-1290.
[2]	Lulu XU,Zhenchao ZHAO,Rongrong ZHAO,Rui YU,Weiping ZHANG. Effects of Magnesium Modification on the Catalytic Performances of HZSM-5 Zeolite for the Conversion of Ethene to Propene [J]. Acta Phys. -Chim. Sin., 2019, 35(1): 92-100.
[3]	Hengwei WANG,Junling LU. Atomic Layer Deposition: A Gas Phase Route to Bottom-up Precise Synthesis of Heterogeneous Catalyst [J]. Acta Phys. -Chim. Sin., 2018, 34(12): 1334-1357.
[4]	Jie XIAO,Bo ZHANG,Zhao-Lei ZHENG. Development and Validation of a Reduced Chemical Kinetic Mechanism for HCCI Engine of Biodiesel Surrogate [J]. Acta Phys. -Chim. Sin., 2017, 33(9): 1752-1764.
[5]	Lin-Jun ZHAN,Xiao-Yan SUN,Ying ZHOU,Qiu-Lian ZHU,Yin-Fei CHEN,Han-Feng Lu. Deactivation Mechanism of CeO₂-Based Mixed Oxide Catalysts Supported on SiO₂ [J]. Acta Phys. -Chim. Sin., 2017, 33(7): 1474-1482.
[6]	Hassan GOLMOHAMMADI,Zahra DASHTBOZORGI,Sajad KHOOSHECHIN. Prediction of Blood-to-Brain Barrier Partitioning of Drugs and Organic Compounds Using a QSPR Approach [J]. Acta Phys. -Chim. Sin., 2017, 33(6): 1160-1170.
[7]	Zhou-Sheng MO,Yu-Cai QIN,Xiao-Tong ZHANG,Lin-Hai DUAN,Li-Juan SONG. Influencing Mechanism of Cyclohexene on Thiophene Adsorption over CuY Zeolites [J]. Acta Phys. -Chim. Sin., 2017, 33(6): 1236-1241.
[8]	Hassan GOLMOHAMMADI,Zahra DASHTBOZORGI,Sajad KHOOSHECHIN. Developing a Support Vector Machine Based QSPR Model to PredictGas-to-Benzene Solvation Enthalpy of Organic Compounds [J]. Acta Phys. -Chim. Sin., 2017, 33(5): 918-926.
[9]	Yi-Hao HU,Tong-Yang SONG,Yue-Juan WANG,Geng-Sheng HU,Guan-Qun XIE,Meng-Fei LUO. Gas Phase Dehydrochlorination of 1, 1, 2-Trichloroethane over Zn/SiO₂ Catalysts: Acidity and Deactivation [J]. Acta Phys. -Chim. Sin., 2017, 33(5): 1017-1026.
[10]	Yong-Min XIE,Xiao-Qiang WANG,Jiang LIU,Chang-Lin YU. Fabrication and Performance of Tubular Electrolyte-Supporting Direct Carbon Solid Oxide Fuel Cell by Dip Coating Technique [J]. Acta Phys. -Chim. Sin., 2017, 33(2): 386-392.
[11]	Shen-Hui LI,Jing LI,An-Min ZHENG,Feng DENG. Solid-State NMR Characterization of the Structure and Catalytic Reaction Mechanism of Solid Acid Catalysts [J]. Acta Phys. -Chim. Sin., 2017, 33(2): 270-282.
[12]	Pengfei CAO,Yang HU,Youwei ZHANG,Jing PENG,Maolin ZHAI. Radiation Induced Synthesis of Amorphous Molybdenum Sulfide/Reduced Graphene Oxide Nanocomposites for Efficient Hydrogen Evolution Reaction [J]. Acta Phys. -Chim. Sin., 2017, 33(12): 2542-2549.
[13]	Ji ZHENG,Li-Rui XING,Dan LI. Extreme Long and Extreme Short Cu-Cu Distances:Nature of Cuprophilicity and Luminescence Modification in Cu (Ⅰ)-based Cyclic Trinuclear Complexes [J]. Acta Phys. -Chim. Sin., 2017, 33(11): 2133-2140.
[14]	Yang CHEN,Xiao-Yan YANG,Peng ZHANG,Dao-Sheng LIU,Jian-Zhou GUI,Hai-Long PENG,Dan LIU. Noble Metal-Supported on Rod-Like ZnO Photocatalysts with Enhanced Photocatalytic Performance [J]. Acta Phys. -Chim. Sin., 2017, 33(10): 2082-2091.
[15]	Xiang-Dong ZENG,Xiao-Yu ZHAO,Hui-Ge WEI,Yan-Fei WANG,Na TANG,Zuo-Liang SHA. Specific Capacitance and Supercapacitive Properties of Polyaniline-Reduced Graphene Oxide Composite [J]. Acta Phys. -Chim. Sin., 2017, 33(10): 2035-2041.

Effect of Alumina Support and Barium Oxide on the Structure and Catalytic Activity of Ruthenium Catalysts for Ammonia Synthesis

PDF (PC)

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Metrics

Comments

Recommended 10