留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

十元环分子筛在甲醇芳构化反应中催化性能的研究

耿蕊 董梅 王浩 牛宪军 樊卫斌 王建国 秦张峰

耿蕊, 董梅, 王浩, 牛宪军, 樊卫斌, 王建国, 秦张峰. 十元环分子筛在甲醇芳构化反应中催化性能的研究[J]. 燃料化学学报(中英文), 2014, 42(09): 1119-1127.
引用本文: 耿蕊, 董梅, 王浩, 牛宪军, 樊卫斌, 王建国, 秦张峰. 十元环分子筛在甲醇芳构化反应中催化性能的研究[J]. 燃料化学学报(中英文), 2014, 42(09): 1119-1127.
GENG Rui, DONG Mei, WANG Hao, NIU Xian-jun, FAN Wei-bin, WANG Jian-guo, QIN Zhang-feng. An investigation on the catalytic performance of 10 MR zeolites in methanol aromatization reaction[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1119-1127.
Citation: GENG Rui, DONG Mei, WANG Hao, NIU Xian-jun, FAN Wei-bin, WANG Jian-guo, QIN Zhang-feng. An investigation on the catalytic performance of 10 MR zeolites in methanol aromatization reaction[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1119-1127.

十元环分子筛在甲醇芳构化反应中催化性能的研究

基金项目: 国家自然科学基金(21103216,21273264,21273263);国家重点基础研究发展规划(973计划,2011CB201403);山西省自然科学基金(2012011005-2)。
详细信息
    通讯作者:

    樊卫斌,E-mail:fanwb@sxicc.ac.cn;董梅,E-mail:mdong@sxicc.ac.cn;Tel:0351-4046736。

  • 中图分类号: O643.3

An investigation on the catalytic performance of 10 MR zeolites in methanol aromatization reaction

  • 摘要: 合成了ZSM-5、ZSM-22、EU-1、MCM-22和ITQ-13具有十元环孔道结构的5种分子筛,研究了分子筛结构、酸性分布等因素对其在甲醇芳构化反应中催化性能的影响。研究表明,不同结构分子筛的形貌、酸性及孔径均存在较大差异,进而影响了其在甲醇制芳烃反应中的催化活性和稳定性。研究的5种分子筛中,ZSM-5表现出最佳的芳构化活性,芳烃收率达34.8%,MCM-22芳烃收率约为21.9%,而其他3种结构的分子筛催化剂基本未表现出甲醇芳构化活性。通过添加具有芳构化性能的Ga物种对ZSM-5和MCM-22进行改性,可显著提升芳烃收率,Ga/ZSM-5上芳烃收率达到40.8%,Ga/MCM-22上芳烃收率可提高到27.1%。另外,采用TG/DTA、GC等方法研究了失活催化剂的积炭情况,发现分子筛结构对积炭量、积炭组成及积炭分布存在显著影响。
  • TRAVALLONI L, GOMES A C L, GASPAR A B, SILVA M A P. Methanol conversion over acid solid catalysts[J]. Catal Today, 2008, 133-135: 406-412.
    STÖCKER M. Methanol to hydrocarbons: Catalytic materials and their behavior[J]. Microporous Mesoporous Mater, 1999, 29(1/2): 3-48.
    KIM J, CHOI M, RYOO R. Effect of mesoporosity against the deactivation of MFI zeolite catalyst during the methanol to hydrocarbon conversion process[J]. J Catal, 2010, 269(1): 219-228.
    CHEN J Q, BOZZANO A, GLOVER B, FUGLERUD T, KVISLE S. Recent advancements in ethylene and propylene production using the UOP/Hydro MTO process[J]. Catal Today, 2005, 106(1/4): 103-107.
    MOKRANI T, SCURRELL M. Gas conversion to liquid fuels and chemicals: The methanol route-catalysis and processes development[J]. Catal Rev, 2009, 51(1): 1-145.
    KUMAR R, RATNASWAMY P. Isomerization and formation of xylenes over ZSM-5 and ZSM-23 zeolites[J]. J Catal, 1989, 116(2): 440-448.
    BRISCOE N A, JOHNSON D W, SHANNON M D. The framework topology of zeolite EU-1[J]. Zeolites, 1988, 8(1): 74-76.
    BOXI T, PUCHE M, CAMBLOR M A. Synthetic porous crystalline material, used as catalyst and adsorbent, comprises sets of generally parallel channels defined by specific rings of tetrahedrally coordinated atoms, which intersect mutually: US, 6471941. 2002.
    BAERLOCHER C H, MCCUSKER L B, OLSON D H. Atlas of zeolite framework types sixth revised edition[M]. Netherlands: Elsevier Science Ltd, 2007.
    ROBSON H, LILLERUD K P. Verified synthesis of zeolitic materials[M]. Netherlands: Elsevier Science Ltd, 2001.
    苗青, 董梅, 牛宪军, 王浩, 樊卫斌, 王建国, 秦张峰. 含镓ZSM-5 分子筛的制备及其在甲醇芳构化反应中的催化性能[J]. 燃料化学学报, 2012, 40(10): 1230-1239. (MIAO Qing, DONG Mei, NIU Xian-jun, WANG Hao, FAN Wei-bin, WANG Jian-guo, QIN Zhang-feng. Synthesis of gallium-containing ZSM-5 molecular sieves and their catalytic performance in methanol aromatization[J]. Journal of Fuel Chemistry and Technology, 2012, 40(10): 1230-1239.)
    JOLY J F, AJOT H, MERLEN E, RAATZ F, ALARIO F. Parameters affecting the dispersion of the gallium phase of gallium H-MFI aromatization catalysts[J]. Appl Catal A: Gen, 1991, 79(2): 249-263.
    TEKETEL S. Shape selectivity in the conversion of methanol to hydrocarbons: The catalytic performance of one-dimensional 10-ring zeolites: ZSM-22, ZSM-23, ZSM-48, and EU-1[J]. ACS Catal, 2012, 2(1): 26-37.
    BJØRGEN M, OLSBYE U, PETERSEN D, KOLBOE S. The methanol to hydrocarbons reaction: Insight into the reaction mechanism from 12C benzene and 13C methanol coreactions over zeolite H-beta[J]. J Catal, 2004, 221(1): 1-10.
    TEKETEL S, OLSBYE U, LILLERUD K P, BEATO P, SVELLE S. Selectivity control through fundamental mechanistic insight in the conversion of methanol to hydrocarbons over zeolites[J]. Microporous Mesoporous Mater, 2010, 136(1/3): 33-41.
    BEECKMAN J W, FROMENT G F. Catalyst deactivation by active site coverage and pore blockage[J]. Ind Eng Chem Fundam, 1979, 18(3): 245-256.
    BEECKMAN J W, FROMENT G F. Catalyst deactivation by site coverage and pore blockage: Finite rate of growth of the carbonaceous deposit[J]. Chem Eng Sci, 1980, 35(4): 805-815.
    ROLLMANN L D, WALSH D E. Shape selectivity and carbon formation in zeolites[J]. J Catal, 1979, 56(1): 139-140.
    刘中民, 陈国权, 王清遐, 梁娟, 蔡光宇. 分子筛催化剂的失活与积炭[J]. 催化学报, 1994, 15(4): 301-303. (LIU Zhong-min, CHEN Guo-quan, WANG Qing-xia, LIANG Juan, CAI Guang-yu. Deactivation and coke formation on zeolite catalysts[J]. Chinese Journal of Catalysis, 1994, 15(4): 301-303.)
    BJØRGEN M, SVELLE S, JOENSEN F, NERLOV J, KOLBOE S, BONINO F, PALUMBO L, BORDIGA S, OLSBYE U. Conversion of methanol to hydrocarbons over zeolite H-ZSM-5: On the origin of the olefinic species[J]. J Catal, 2007, 249(2): 195-207.
    BLEKEN F, SKISTAD W, BARBERA K, KUSTOVA M, BORDIGA S, BEATO P, LILLERUD K P, SVELLE S, OLSBYE U. Conversion of methanol over 10-ring zeolites with differing volumes at channel intersections: Comparison of TNU-9, IM-5, ZSM-11 and ZSM-5[J]. Phys Chem Chem Phys, 2011, 13(7): 2539-2549.
  • 加载中
计量
  • 文章访问数:  798
  • HTML全文浏览量:  23
  • PDF下载量:  645
  • 被引次数: 0
出版历程
  • 收稿日期:  2014-01-17
  • 修回日期:  2014-03-05
  • 刊出日期:  2014-09-30

目录

    /

    返回文章
    返回