V2O5负载量对V2O5/Al2O3氧化活化正庚烷催化裂解反应的影响

doi:10.3866/PKU.WHXB20110806

物理化学学报 >> 2011, Vol. 27 >> Issue (09): 2209-2216.doi: 10.3866/PKU.WHXB20110806

V₂O₅负载量对V₂O₅/Al₂O₃氧化活化正庚烷催化裂解反应的影响

胡晓燕, 李春义, 杨朝合

中国石油大学(华东), 重质油国家重点实验室, 山东青岛 266555

收稿日期:2011-03-14 修回日期:2011-05-30 发布日期:2011-08-26
通讯作者: 李春义 E-mail:chyli@upc.edu.cn
基金资助:
国家重点基础研究发展规划项目(973) (2006CB202505)资助

Influences of V₂O₅ Loadings on V₂O₅/Al₂O₃ Oxidative Activation Performances for n-Heptane Catalytic Cracking

HU Xiao-Yan, LI Chun-Yi, YANG Chao-He

State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266555, Shandong Province, P. R. China

Received:2011-03-14 Revised:2011-05-30 Published:2011-08-26
Contact: LI Chun-Yi E-mail:chyli@upc.edu.cn
Supported by:
The project was supported by the National Key Basic Research Program of China (973) (2006CB202505).

摘要/Abstract

摘要： 采用X射线衍射, 低温氮气吸脱附, 氨气程序升温脱附和吡啶吸附红外光谱分析方法对不同活性组分负载量V₂O₅/Al₂O₃的性质进行了表征. 根据表面VO_x单元密度, 推测V₂O₅负载量为20%-25% (w)对应着V₂O₅/Al₂O₃表面达单层覆盖状态; V₂O₅的负载使Al₂O₃表面Lewis 酸量减少, 并出现Brønsted 酸, 对应着氧化态VO_x单元中的V―OH; 随着负载量的增加, Brønsted 酸量增加至负载量为20%时达到最大值. 对V₂O₅/Al₂O₃中活性组分负载量对其氧化活化正庚烷催化裂解反应的影响进行了考察. 结果表明, 在V₂O₅负载量为20%-25%时,V₂O₅/Al₂O₃的引入对正庚烷在HZSM-5 平衡剂上催化裂解反应的促进作用最明显, 此时VO_x单元在V₂O₅/Al₂O₃表面形成单层覆盖状态, 可提供最大量的表面晶格氧, 因而对正庚烷具有最强的氧化活化作用; V₂O₅负载量继续增加形成体相的V₂O₅和AlVO₄, 不利于晶格氧参与正庚烷的转化, 因而反应性能有所下降.

关键词: V₂O₅/Al₂O₃, V₂O₅负载量, VO_x结构形态, 晶格氧, 氧化活化

Abstract: X-ray diffraction (XRD), nitrogen adsorption-desorption, ammonia-temperature programmed desorption (NH₃-TPD), and pyridine-Fourier transform infrared (pyridine-FT-IR) spectroscopy analyses were performed to characterize V₂O₅/Al₂O_x with different V₂O₅ loadings. We conclude that a 20%-25% (w) V₂O₅ loading corresponds to the monolayer coverage of VO_x units over the surface of V₂O₅/Al₂O₃ according to the VO_x unit surface density values. The impregnation of V₂O₅ led to a decrease in the Lewis acidity of the alumina and the formation of Brønsted acid sites, which resulted from the V―OH groups of the oxidized VO_x units. With an increase in V₂O₅ loading the amount of Brønsted acid sites increased and reached a maximum at a V₂O₅ loading of about 20%. The influence of V₂O₅ loading in V₂O₅/Al₂O₃ on the oxidative activation performance during n-heptane catalytic cracking was studied. The results show that the highest promotion was obtained upon introducing V₂O₅/Al₂O₃ with a 20%-25% V₂O₅ loading into the HZSM-5 equilibrium catalyst. V₂O₅/Al₂O₃ (20%-25% V₂O₅) had a monolayer coverage of VO_x units over its surface and it provided the largest amount of surface lattice oxygen and thus the strongest oxidative activation toward n-heptane was achieved. The performance decreased when the V₂O₅ loading increased further because of the inhibited participation of surface lattice oxygen in the reaction, which was caused by the formation of bulk V₂O₅ and AlVO₄.

Key words: V₂O₅/Al₂O₃, Vanadia loading, VO_x configuration, Lattice oxygen, Oxidative activation

胡晓燕, 李春义, 杨朝合. V₂O₅负载量对V₂O₅/Al₂O₃氧化活化正庚烷催化裂解反应的影响[J]. 物理化学学报, 2011, 27(09), 2209-2216. doi: 10.3866/PKU.WHXB20110806

HU Xiao-Yan, LI Chun-Yi, YANG Chao-He. Influences of V₂O₅ Loadings on V₂O₅/Al₂O₃ Oxidative Activation Performances for n-Heptane Catalytic Cracking[J]. Acta Phys. -Chim. Sin. 2011, 27(09), 2209-2216. doi: 10.3866/PKU.WHXB20110806

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110806

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I09/2209

参考文献

(1) Corma, A.; Melo, F. V.; Sauvanaud, L.; Ortega, F. J. Appl. Catal. A 2004, 265, 195.

(2) Hu, X. Y.; Li, C. Y.; Yang, C. H. Acta Phys. ?Chim. Sin. 2010, 26, 3291. [胡晓燕, 李春义, 杨朝合. 物理化学学报, 2010, 26, 3291.]
(3) Liu, X. B.; Xu, H. Y.; Li,W. Z.; Chen, Y. X. Acta Petrolei Sinica (Petro. Pro. Sec.) 2004, 20, 88. [刘雪斌, 徐恒泳, 李文钊, 陈燕馨. 石油学报: 石油加工, 2004, 20, 88.]
(4) Zhang, C. L.; Zhu, H. O.; Liu, X. B.; Li,W. Z.; Xu, H. Y. J. Fuel Chem. Tech. 2006, 34, 439. [张存龙, 朱海欧, 刘雪斌, 李文钊, 徐恒泳. 燃料化学学报, 2006, 34, 439.]
(5) Hu, X. Y.; Li, C. Y.; Yang, C. H. Catal. Today 2010, 158, 504.

(6) Haber, J. Catal. Today 2009, 142, 100.

(7) Abon, M.; Volta, J. C. Appl. Catal. A 1997, 157, 173.

(8) Centi, G.; Perathoner, S.; Trifirb, F. Appl. Catal. A 1997, 157, 143.

(9) Shishido, T.; Konishi, T.; Matsuura, I.;Wang, Y.; Takaki, K.; Takehira, K. Catal. Today 2001, 41, 77.
(10) Isaguliants, G. V.; Belomestnykh, I. P. Catal. Today 2005, 100, 441.

(11) Kung, H. H. Adv. Catal. 1994, 40, 1.

(12) Kung, H. H.; Kung, M. C. Appl. Catal. A 1997, 157, 105.

(13) Blasco, T.; Nieto, J. M. L. Appl. Catal. A 1997, 157, 117.

(14) Wielers, A. F. H.; Vaarkamp, M.; Post, M. F. M. J. Catal. 1991, 127, 51.

(15) Wachs, I. E.;Weckhuysen, B. M. Appl. Catal. A 1997, 157, 67.

(16) Grzybowska-Swierkosz, B. Appl. Catal. A 1997, 157, 409.

(17) Ferreira, M. L.; Volpe, M. J. Mol. Catal. A 1999, 149, 33.

(18) Christodoulakis, A.; Machli, M.; Lemonidou, A. A.; Boghosian, S. J. Catal. 2004, 222, 293.

(19) Steinfeldt, N.; Müller, D.; Berndt, H. Appl. Catal. A 2004, 272, 201.

(20) Wu, Z.; Kim, H. S.; Stair, P. C.; Rugmini, S.; Jackson, S. D. J. Phys. Chem. B 2005, 109, 2793.

(21) Martínez-Huerta, M. V.; Gao, X.; Tian, H.;Wachs, I. E.; Fierro, J. L. G.; Ba?ares, M. A. Catal. Today 2006, 118, 279.

(22) Pak, C.; Bell, A. T.; Tilley, T. D. J. Catal. 2002, 206, 49.

(23) Balderas-Tapia, L.; Hernández-Pérez, I.; Schacht, P.; C?rdova, I. R.; Aguilar-Ríos, G. G. Catal. Today 2005, 107-108, 371.
(24) Kim, T.;Wachs, I. E. J. Catal. 2008, 197, 133.
(25) Argyle, M. D.; Chen, K.; Bell, A. T.; Iglesia, E. J. Catal. 2002, 208, 139.

(26) Khader, M. M. J. Mol. Catal. A 1995, 104, 87.

(27) Turek, A. M.;Wachs. I. E. J. Phys. Chem. 1992, 96, 5000.

[1]	郑倩, 曹玥晗, 黄南建, 张瑞阳, 周莹. BN诱导BiOI富氧{110}面的暴露并增强其可见光催化氧化性能[J]. 物理化学学报, 2021, 37(8): 2009063 - .
[2]	程飞,杨建,闫亮,赵军,赵华华,宋焕玲,丑凌军. 固体酸WO₃/TiO₂负载锂锰催化剂组成对其甲烷氧化偶联反应性能的影响[J]. 物理化学学报, 2019, 35(9): 1027 -1036 .
[3]	吴倩,翁维正,刘春丽,黄传敬,夏文生,万惠霖. 制备方法对Nd₂O₃上过氧物种光诱导生成的影响[J]. 物理化学学报, 2017, 33(10): 2064 -2071 .
[4]	张洁, 张江浩, 张长斌, 贺泓. 不同晶相结构二氧化锰催化完全氧化乙醇[J]. 物理化学学报, 2015, 31(2): 353 -359 .
[5]	李绪渊,张自萍,马建泰,朱宗祯,孟益民. 钙钛矿型La_1+X/2Sr_1-x/2Co_1-xCu_xO₃催化CO氧化活性与表征[J]. 物理化学学报, 1996, 12(06): 502 -507 .
[6]	王必勋,伏义路,方书农. Cu-ZSM-5分子筛上[Cu-O-Cu]²⁺物种的原位红外光谱研究[J]. 物理化学学报, 1995, 11(11): 974 -978 .
[7]	余林,徐奕德,郭燮贤. 红外光谱研究甲烷和氧与SrO-La₂O₃/CaO表面的相互作用[J]. 物理化学学报, 1995, 11(10): 902 -906 .

V₂O₅负载量对V₂O₅/Al₂O₃氧化活化正庚烷催化裂解反应的影响

Influences of V₂O₅ Loadings on V₂O₅/Al₂O₃ Oxidative Activation Performances for n-Heptane Catalytic Cracking

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 7

Metrics

推荐阅读 0