原位晶化FCC催化剂传质性能的频率响应法辨析

引用本文: 秦玉才, 高雄厚, 石利飞, 张莉, 段林海, 宋丽娟. 原位晶化FCC催化剂传质性能的频率响应法辨析[J]. 物理化学学报, 2016, 32(2): 527-535. doi: 10.3866/PKU.WHXB201512033 shu

Citation: QIN Yu-Cai, GAO Xiong-Hou, SHI Li-Fei, ZHANG Li, DUAN Lin-Hai, SONG Li-Juan. Discrimination of the Mass Transfer Performance of In situ Crystallization FCC Catalysts by the Frequency Response Method[J]. Acta Physico-Chimica Sinica, 2016, 32(2): 527-535. doi: 10.3866/PKU.WHXB201512033 shu

原位晶化FCC催化剂传质性能的频率响应法辨析

秦玉才 ^1, ,
高雄厚 ^{2,
,} ,
石利飞 ^1, ,
张莉 ^2, ,
段林海 ^1, ,
宋丽娟 ^{1,
,}

1.
1 辽宁石油化工大学, 辽宁省石油化工催化科学与技术重点实验室, 辽宁抚顺 113001;
2.
2 中国石油天然气股份有限公司, 石油化工研究院兰州化工研究中心, 兰州 730060

通讯作者: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

基金项目:
国家自然科学基金(21076100,21376114) (21076100,21376114)

中国石油天然气股份有限公司(10-01A-01-01-01) (10-01A-01-01-01)

辽宁省高校创新团队资助项目

摘要: 以苯为探针分子,采用频率响应(FR)技术和智能重量分析仪(IGA)研究了原位晶化流化催化裂化(FCC)催化剂上的传质行为。结合N₂吸附和扫描电镜(SEM)剖析所得织构性质数据,并与传统半合成FCC催化剂以及稀土改性Y分子筛传质性能进行对比,结果表明原位晶化FCC催化剂所具有的独特纳米化和高度分散的分子筛组分分布状态,显著改善了基质大孔/介孔结构与分子筛微孔孔道的贯通性,削弱了分子筛孔道与基质界面间的传质阻力,从而优化了成型催化剂颗粒的传质性能。本研究再次证实了频率响应技术可以检测和辨析多孔催化材料体系中发生的复杂吸附-扩散过程,是一种有效的多级孔催化材料传质性能的研究手段。

关键词:

English

Discrimination of the Mass Transfer Performance of In situ Crystallization FCC Catalysts by the Frequency Response Method

1.
1 Key Laboratory of Petrochemical Catalytic Science and Technology of Liaoning Province, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China;
2.
2 Lanzhou Petrochemical Research Center, Petrochemical Research Institute, Petro China Company Limited, Lanzhou 730060, P. R. China

Corresponding author: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

Received Date: 27 August 2015
Fund Project:
国家自然科学基金(21076100,21376114)

中国石油天然气股份有限公司(10-01A-01-01-01)

辽宁省高校创新团队资助项目

Abstract: Mass transfer behaviors of benzene in an in situ crystallization fluid catalytic cracking (FCC) catalyst were measured and discriminated by the frequency response (FR) method and an intelligent gravimetric analyzer (IGA). The texture properties of the FCC catalysts were analyzed by N₂ adsorption and scanning electron microscope (SEM). By comparison with the mass transfer performance of a semi-synthetic FCC catalyst, as well as a zeolite Y, the results show that the in situ crystallization FCC catalyst has excellent and improved mass transfer behavior over the semi-synthetic FCC catalyst and that it reduces the mass transfer resistance between the interface of zeolite crystal and substrate, which can be attributed to the excellent porous connectivity of the former with the unique accumulation state of the highly dispersed nanosized Y zeolite crystals. It has been demonstrated that the FR technique can be used to measure and distinguish the complex mass transport processes in hierarchical porous catalytic materials.

Key words:

1. [1]
  (1) Chen, G. Q.; Luo, Z. H. Chem. Eng. Sci. 2014, 109, 38. doi: 10.1016/j.ces.2014.01.015(1) Chen, G. Q.; Luo, Z. H. Chem. Eng. Sci. 2014, 109, 38. doi: 10.1016/j.ces.2014.01.015
2. [2]
  (2) Stockwell, D. M. Studies in Surface Science and Catalysis 2007, 166, 137. doi: 10.1016/S0167-2991(07)80193-5(2) Stockwell, D. M. Studies in Surface Science and Catalysis 2007, 166, 137. doi: 10.1016/S0167-2991(07)80193-5
3. [3]
  (3) Mitchell, S.; Michels, N. L.; Pǒ rez-Ramí rez, J. Chem. Soc. Rev. 2013, 42, 6094. doi: 10.1039/c3cs60076a(3) Mitchell, S.; Michels, N. L.; Pǒ rez-Ramí rez, J. Chem. Soc. Rev. 2013, 42, 6094. doi: 10.1039/c3cs60076a
4. [4]
  (4) Liu, H. H.; Zhao, H. J.; Gao, X. H.; Ma, J. T. Catal. Today 2007, 125, 163. doi: 10.1016/j.cattod.2007.05.005(4) Liu, H. H.; Zhao, H. J.; Gao, X. H.; Ma, J. T. Catal. Today 2007, 125, 163. doi: 10.1016/j.cattod.2007.05.005
5. [5]
  (5) Liu, H. H.; Ma, J. T.; Gao, X. H. Catal. Lett. 2006, 110, 229. doi: 10.1007/s10562-006-0113-z(5) Liu, H. H.; Ma, J. T.; Gao, X. H. Catal. Lett. 2006, 110, 229. doi: 10.1007/s10562-006-0113-z
6. [6]
  (6) Liu, H. H.; Zhang, Y. M.; Zheng, S. Q.; Zhou, H. B. Petroleum Processing and Petrochemicals 2001, 32, 37. [刘宏海, 张永明, 郑淑琴, 周宏宝. 石油炼制与化工, 2001, 32, 37.](6) Liu, H. H.; Zhang, Y. M.; Zheng, S. Q.; Zhou, H. B. Petroleum Processing and Petrochemicals 2001, 32, 37. [刘宏海, 张永明, 郑淑琴, 周宏宝. 石油炼制与化工, 2001, 32, 37.]
7. [7]
  (7) Stockwell, D. M.; Brown, R. P.; Brown, S. H. StructureEnhanced Cracking Catalysts. US Patent 6943132, 2005-09-13 .(7) Stockwell, D. M.; Brown, R. P.; Brown, S. H. StructureEnhanced Cracking Catalysts. US Patent 6943132, 2005-09-13 .
8. [8]
  (8) Lussier, R. J. Acid-Reacted Metakaolin Catalyst and CatalystSupport Compositions. US Patent 4843052, 1989-06-27.(8) Lussier, R. J. Acid-Reacted Metakaolin Catalyst and CatalystSupport Compositions. US Patent 4843052, 1989-06-27.
9. [9]
  (9) Falco, M.; Morgado, E.; Amadeo, N.; Sedran, U. Appl. Catal. A -Gen. 2006, 315, 29. doi: 10.1016/j.apcata.2006.08.028(9) Falco, M.; Morgado, E.; Amadeo, N.; Sedran, U. Appl. Catal. A -Gen. 2006, 315, 29. doi: 10.1016/j.apcata.2006.08.028
10. [10]
  (10) Hosseinpour, N.; Mortazavi, Y.; Bazyari, A.; Khodadadi, A. A.Fuel Process. Technol. 2009, 90, 171. doi: 10.1016/j.fuproc.2008.08.013(10) Hosseinpour, N.; Mortazavi, Y.; Bazyari, A.; Khodadadi, A. A.Fuel Process. Technol. 2009, 90, 171. doi: 10.1016/j.fuproc.2008.08.013
11. [11]
  (11) Tonetto, G.; Atias, J.; De Lasa, H. Appl. Catal. A -Gen. 2004, 270, 9. doi: 10.1016/j.apcata.2004.03.042(11) Tonetto, G.; Atias, J.; De Lasa, H. Appl. Catal. A -Gen. 2004, 270, 9. doi: 10.1016/j.apcata.2004.03.042
12. [12]
  (12) Avila, A. M.; Bidabehere, C. M.; Sedran, U. Chem. Eng. J. 2007, 132, 67. doi: 10.1016/j.cej.2007.01.020(12) Avila, A. M.; Bidabehere, C. M.; Sedran, U. Chem. Eng. J. 2007, 132, 67. doi: 10.1016/j.cej.2007.01.020
13. [13]
  (13) Kä rger, J. Chem. Eng. J. 2009, 145, 522. doi: 10.1016/j.cej.2008.08.001(13) Kä rger, J. Chem. Eng. J. 2009, 145, 522. doi: 10.1016/j.cej.2008.08.001
14. [14]
  (14) Lee, C. K.; Ashtekar, S.; Gladden, L. F.; Barrie, P. J. Chem. Eng. Sci. 2004, 59, 1131. doi: 10.1016/j.ces.2004.01.005(14) Lee, C. K.; Ashtekar, S.; Gladden, L. F.; Barrie, P. J. Chem. Eng. Sci. 2004, 59, 1131. doi: 10.1016/j.ces.2004.01.005
15. [15]
  (15) Barrie, P. J.; Lee, C. K.; Gladden, L. F. Chem. Eng. Sci. 2004, 59, 1139. doi: 10.1016/j.ces.2004.01.008(15) Barrie, P. J.; Lee, C. K.; Gladden, L. F. Chem. Eng. Sci. 2004, 59, 1139. doi: 10.1016/j.ces.2004.01.008
16. [16]
  (16) Kortunov, P.; Vasenkov, S.; Kä rger, J.; Fǒ Elí a, M.; Perez, M.; Stö cker, M.; Papadopoulos, G. K.; Theodorou, D.; Drescher, B.; McElhiney, G.; Bernauer, B.; Krystl, V.; Koč iř í k, M.; Ziká nová , A.; Jirglová , H.; Berger, C.; Glä ser, R.; Weitkamp, J.; Hansen, E.W. Chem. Mater. 2005, 17, 2466. doi: 10.1021/cm050031z(16) Kortunov, P.; Vasenkov, S.; Kä rger, J.; Fǒ Elí a, M.; Perez, M.; Stö cker, M.; Papadopoulos, G. K.; Theodorou, D.; Drescher, B.; McElhiney, G.; Bernauer, B.; Krystl, V.; Koč iř í k, M.; Ziká nová , A.; Jirglová , H.; Berger, C.; Glä ser, R.; Weitkamp, J.; Hansen, E.W. Chem. Mater. 2005, 17, 2466. doi: 10.1021/cm050031z
17. [17]
  (17) Rees, L. V. C.; Song, L. J. Frequency Response Method for theCharacterization of MicroporousSolids. In Membrane Science and Technology; Kanellopoulos, N. K. Ed.; Elsevier:Amsterdam, 2000; series 6, pp 139-212.(17) Rees, L. V. C.; Song, L. J. Frequency Response Method for theCharacterization of MicroporousSolids. In Membrane Science and Technology; Kanellopoulos, N. K. Ed.; Elsevier:Amsterdam, 2000; series 6, pp 139-212.
18. [18]
  (18) Li, F. F.; Gui, X. H.; Liu, D. S.; Song, L. J.; Sun, Z. L. Acta Phys. -Chim. Sin. 2008, 24 (4), 659. [李菲菲, 桂兴华, 刘道胜, 宋丽娟, 孙兆林. 物理化学学报, 2008, 24 (4), 659.] doi: 10.3866/PKU.WHXB20080419(18) Li, F. F.; Gui, X. H.; Liu, D. S.; Song, L. J.; Sun, Z. L. Acta Phys. -Chim. Sin. 2008, 24 (4), 659. [李菲菲, 桂兴华, 刘道胜, 宋丽娟, 孙兆林. 物理化学学报, 2008, 24 (4), 659.] doi: 10.3866/PKU.WHXB20080419
19. [19]
  (19) Qin, Y. C.; Mo, Z. S.; Yu, W. G.; Dong, S.W.; Duan, L. H.; Gao, X. H.; Song, L. J. Appl. Surf. Sci. 2014, 292, 5. doi: 10.1016/j.apsusc.2013.11.036(19) Qin, Y. C.; Mo, Z. S.; Yu, W. G.; Dong, S.W.; Duan, L. H.; Gao, X. H.; Song, L. J. Appl. Surf. Sci. 2014, 292, 5. doi: 10.1016/j.apsusc.2013.11.036
20. [20]
  (20) Qin, Y. C.; Gao, X. H.; Zhang, H. T.; Zhang, S. H.; Zheng, L.G.; Li, Q.; Mo, Z. S.; Duan, L. H.; Zhang, X. T.; Song, L. J.Catal. Today 2015, 245, 147. doi: 10.1016/j.cattod.2014.06.007(20) Qin, Y. C.; Gao, X. H.; Zhang, H. T.; Zhang, S. H.; Zheng, L.G.; Li, Q.; Mo, Z. S.; Duan, L. H.; Zhang, X. T.; Song, L. J.Catal. Today 2015, 245, 147. doi: 10.1016/j.cattod.2014.06.007
21. [21]
  (21) Song, L. J.; Rees, L. V. C. Microporous Mesoporous Mat. 2000, 35, 301.(21) Song, L. J.; Rees, L. V. C. Microporous Mesoporous Mat. 2000, 35, 301.
22. [22]
  (22) Onyestyá k, G.; Shen, D. N.; Rees, L. V. C. J. Chem. Soc. Faraday Trans. 1995, 91 (9), 1399. doi: 10.1039/ft9959101399(22) Onyestyá k, G.; Shen, D. N.; Rees, L. V. C. J. Chem. Soc. Faraday Trans. 1995, 91 (9), 1399. doi: 10.1039/ft9959101399
23. [23]
  (23) Yasuda, Y. H. Chem. Rev. 1994, 1, 103.(23) Yasuda, Y. H. Chem. Rev. 1994, 1, 103.
24. [24]
  (24) Crank, J. The Mathematics of Diffusion; Oxford Press:London, 1975; pp 90-91.(24) Crank, J. The Mathematics of Diffusion; Oxford Press:London, 1975; pp 90-91.
25. [25]
  (25) Kondo, S.; Ishikawa, T.; Abe, I. Science of Adsorption, 2nded.; Chemical Industry Press: Beijing, 2005; pp 69-70; translated by Li, G. X. [近藤精一, 石川达雄, 安部郁夫. 吸附科学. 第二版. 李国希, 译. 北京: 化学工业出版社, 2005:69-70.](25) Kondo, S.; Ishikawa, T.; Abe, I. Science of Adsorption, 2nded.; Chemical Industry Press: Beijing, 2005; pp 69-70; translated by Li, G. X. [近藤精一, 石川达雄, 安部郁夫. 吸附科学. 第二版. 李国希, 译. 北京: 化学工业出版社, 2005:69-70.]
26. [26]
  (26) Qin, Y. C.; Gao, X. H.; Pei, T. T.; Zheng, L. G.; Wang, L.; Mo, Z. S.; Song, L. J. Journal of Fuel Chemistry and Technology 2013, 41 (7), 889. [秦玉才, 高雄厚, 裴婷婷, 郑兰歌, 王琳, 莫周胜, 宋丽娟. 燃料化学学报, 2013, 41 (7), 889.](26) Qin, Y. C.; Gao, X. H.; Pei, T. T.; Zheng, L. G.; Wang, L.; Mo, Z. S.; Song, L. J. Journal of Fuel Chemistry and Technology 2013, 41 (7), 889. [秦玉才, 高雄厚, 裴婷婷, 郑兰歌, 王琳, 莫周胜, 宋丽娟. 燃料化学学报, 2013, 41 (7), 889.]
27. [27]
  (27) Pǒ rez-Ramí rez, J.; Verboekend, D.; Bonilla, A.; Abelló , S. Adv. Funct. Mater. 2009, 19, 3972.(27) Pǒ rez-Ramí rez, J.; Verboekend, D.; Bonilla, A.; Abelló , S. Adv. Funct. Mater. 2009, 19, 3972.
28. [28]
  (28) Qin, Y. C.; Gao, X. H.; Duan, L. H.; Fan, Y. C.; Yu, W. G.; Zhang, H. T.; Song, L. J. Acta Phys. -Chim. Sin. 2014, 30 (3), 544. [秦玉才, 高雄厚, 段林海, 范跃超, 于文广, 张海涛, 宋丽娟. 物理化学学报, 2014, 30 (3), 544.] doi: 10.3866/PKU.WHXB201401021(28) Qin, Y. C.; Gao, X. H.; Duan, L. H.; Fan, Y. C.; Yu, W. G.; Zhang, H. T.; Song, L. J. Acta Phys. -Chim. Sin. 2014, 30 (3), 544. [秦玉才, 高雄厚, 段林海, 范跃超, 于文广, 张海涛, 宋丽娟. 物理化学学报, 2014, 30 (3), 544.] doi: 10.3866/PKU.WHXB201401021
29. [29]
  (29) Zhang, X. T.; Yu, W. G.; Qin, Y. C.; Dong, S.W.; Pei, T. T.; Wang, L.; Song, L. J. Acta Phys. -Chim. Sin. 2013, 29 (6), 1273. [张晓彤, 于文广, 秦玉才, 董世伟, 裴婷婷, 王琳, 宋丽娟. 物理化学学报, 2013, 29 (6), 1273.] doi: 10.3866/PKU.WHXB201303183(29) Zhang, X. T.; Yu, W. G.; Qin, Y. C.; Dong, S.W.; Pei, T. T.; Wang, L.; Song, L. J. Acta Phys. -Chim. Sin. 2013, 29 (6), 1273. [张晓彤, 于文广, 秦玉才, 董世伟, 裴婷婷, 王琳, 宋丽娟. 物理化学学报, 2013, 29 (6), 1273.] doi: 10.3866/PKU.WHXB201303183

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

原位晶化FCC催化剂传质性能的频率响应法辨析

通讯作者: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

English

Discrimination of the Mass Transfer Performance of In situ Crystallization FCC Catalysts by the Frequency Response Method

Corresponding author: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

原位晶化FCC催化剂传质性能的频率响应法辨析

通讯作者: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

English

Discrimination of the Mass Transfer Performance of In situ Crystallization FCC Catalysts by the Frequency Response Method

Corresponding author: 高雄厚, 宋丽娟; 高雄厚, 宋丽娟

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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