核壳结构Beta/MCM-22双微孔复合分子筛的合成与表征

张佩珊; 马波; 杨卫亚; 凌凤香; 沈智奇; 王少军; 候宇鑫

核壳结构Beta/MCM-22双微孔复合分子筛的合成与表征

1.
辽宁石油化工大学化学与材料科学学院, 辽宁抚顺 113001;
2.
中国石油化工股份有限公司抚顺石油化工研究院, 辽宁抚顺 113001;
3.
中国石油抚顺石化公司, 辽宁抚顺 113004

基金项目: 中国石油化工股份有限公司资助项目(113038)。

详细信息

通讯作者:
凌凤香,E-mail:lingfengxiang@outlook.com;Tel:+86-24-56389578。

中图分类号: O649
计量
- 文章访问数: 774
- HTML全文浏览量: 18
- PDF下载量: 478
- 被引次数: 0
出版历程
- 收稿日期: 2014-04-25
- 修回日期: 2014-07-03
- 刊出日期: 2014-10-30

Synthesis and characterization of core-shell Beta/MCM-22 micro-microporous composite zeolites

1.
Institute of Chemistry and Material Science, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, China;
2.
Fushun Research Institute of Petroleum and Petrochemicals, SINOPEC, Fushun 113001, China;
3.
China Petroleum Fushun Petrochemical Co, Fushun 113004, China

摘要

摘要: 以Beta分子筛为晶核,通过二步水热晶化法成功制备了形态良好的Beta/MCM-22核壳结构复合分子筛。采用X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)及N₂吸附-脱附技术等对分子筛进行了表征。结果表明,复合分子筛形态规整,Beta与MCM-22分别作为核壳而共生;Beta/MCM-22复合分子筛孔结构性质介于MCM-22、Beta分子筛之间。在酸性分布上,复合分子筛的中强酸及B酸所占比例显著增加(C_B/C_L=13.8)。通过Ar-H₂等离子体对Beta分子筛进行处理,使其表面能提高并使表面正电荷富集、硅羟基增加,这是形成良好Beta/MCM-22核壳结构的内在原因。
- Beta /
- MCM-22 /
- 核壳结构 /
- 复合分子筛 /
- 等离子体
Abstract: With Beta zeolite as the core crystals, core-shell Beta/MCM-22 composite zeolites with uniform morphology were synthesized by a two-step hydrothermal method. The composite zeolites were characterized by XRD, SEM, TEM, N₂-adsorption and FT-IR. The results showed the composite zeolites exhibit uniform structured morphology; Beta and MCM-22 zeolites act as core and shell, respectively. The pore structure of Beta/MCM-22 composite zeolites was between those of MCM-22 and Beta zeolites. The amounts of medium acidic sites and brnsted acidic sites are increased markedly (C_B/C_L = 13.80) in the composite zeolites. The surface energy, Si-OH groups and surficial positive charges of Beta zeolites are enriched through Ar-H₂ plasma surface treatment, which contributes to the formation of uniform core-shell Beta/MCM-22 composite zeolites.
- Beta /
- MCM-22 /
- core-shell structure /
- composite zeolites /
- plasma

HTML全文

参考文献(20)

李英霞, 陈标华, 孟伟娟, 李成岳, 王文兴, 曹钢. MCM-22沸石的孔结构和酸分布特性对苯与丙烯烷基化反应产物分布的影响[J]. 催化学报, 2003, 24(7): 494-498. (LI Ying-xia, CHEN Biao-hua, MENG Wei-juan, LI Cheng-yue, WANG Wen-xing, CAO Gang. Effect of pore structure and acidic property of MCM-22 zeolite on product distribution of benzene alkylation with propylene[J].Chinese Journal of Catalysis. 2003, 24(7): 494-498.)

郭群, 贾卫, 赵忠林, 于峰, 李瑞丰. Y/ZSM-5复合分子筛的合成及表征[J]. 太原理工大学学报, 2008, 39(3): 222-225. (GUO Qun, JIA Wei, ZHAO Zhong-lin, YU Feng, LI Rui-feng. Synthesis and characterization of Y/ZSM-5 composite zeolite[J]. Journal of TaiYuan University of Technology, 2008, 39(3): 222-225.)

FAN Y, LEI D, SHI G, BAO X. Synthesis of ZSM-5/SAPO-11 composite and its application in FCC gasoline hydro-upgrading catalyst[J]. Catal Today, 2006, 114(4): 388-396.

PIRNGRUBER G D, LAROCHE C, MARICAR-PICHON M, ROULEAU L, BOUIZI Y, VALTCHEV V. Core-shell zeolite composite with enhanced selectivity for the separation of branched paraffin isomers[J]. Microporous Mesoporous Mater, 2013, 169(15): 212-217.

范峰, 凌凤香, 王少军, 杨春燕, 秦波. 核壳结构的Beta-Y复合分子筛的合成与表征[J]. 燃料化学学报, 2012, 40(7): 861-865. (FAN Feng, LING Feng-xiang, WANG Shao-jun, YANG Chun-yan, QIN Bo. Synthesis and characterization of core-shell Beta-Y composite zeolites[J]. Journal of Fuel Chemistry and Technology, 2012, 40(7): 861-865.)

WANG X, GUO S, ZHAO L. Synthesis of Hβ (core)/SAPO-11 (shell) composite molecular sieve and its catalytic performances in the methylation of naphthalene with methanol[J]. Bull Korean Chem Soc, 2013, 34(12): 3829-3834.

贾卫, 郭群, 崔晓静, 潘大海, 李瑞丰. 以乙二胺为模板剂合成Y/ZSM-5复合分子筛[J]. 石油化工, 2006, 35(9): 832-836. (JIA Wei, GUO Qun, CUI Xiao-jing, PAN Da-hai, LI Rui-feng. Synthesis of Y/ZSM-5 composite molecular sieve with ethylenediamine as template[J]. Petrochemical Technology, 2006, 35(9): 832-836.)

ZHANG Q, LI C, XU S, SHAN H, YANG C. Synthesis of a ZSM-5 (core)/SAPO-5 (shell) composite and its application in FCC[J]. J Porous Mater, 2013, 20(1): 171-176.

张强, 李春义, 山红红, 杨朝合. 分步晶化法合成ZSM-5/SAPO-5复合材料[J]. 燃料化学学报, 2009, 37(6): 722-727. (ZHANG Qiang, LI Chun-yi, SHAN Hong-hong, YANG Chao-he. Synthesis of ZSM-5/SAPO-5 composite by teo-step hydrothermal crystallization process[J]. Journal of Fuel Chemistry and Technology, 2009, 37(6): 722-727.)

闫萍, 马波, 张喜文, 张志智. EU-1/ZSM-5复合分子筛的合成与表征[J]. 石油炼制与化工, 2011, 42(6): 17-22. (YAN Ping, MA Bo, ZHANG Xi-wen, ZHANG Zhi-zhi. Synthesis and characterization of EU-1/ZSM-5 composite zeolite[J]. Petroleum Processing and Petrochemicals, 2011, 42(6): 17-22.)

张强, 李春义, 山红红, 杨朝合. 预先负载原料法合成ZSM-5/SAPO-5复合分子筛[J]. 高等学校化学学报, 2011, 32(12): 2721-2726. (ZHANG Qiang, LI Chun-yi, SHAN Hong-hong, YANG Chao-he. Synthesis of ZSM-5/SAPO-5 composite with the advance loaded raw material[J]. Chemical Journal of Chinese Universities, 2011, 32(12): 2721-2726.)

鲁凤, 王凯. 复合分子筛的发展现状[J]. 化学与黏合, 2012, 35(4): 57-59. (LU Feng, WANG Kai. Develop status of composite zeolite[J]. Chemistry and Adhesion, 2012, 35(4): 57-59.)

王俊宏. 复合分子筛研究新进展及应用前景[J]. 化工技术与开发, 2012, 41(8): 18-21, 43. (WANG Jun-hong. The research progress and application prospects of composite zeolite[J]. Technology and Development of Chemical Industry, 2012, 41(8): 18-21, 43.)

杨瑞娟, 杨冬花, 武正簧, 冯晓娜, 窦涛, 吴忠华, 李志宏, 闫泽, 王凡, 汤琼. 含铁微孔EU-1/ZSM-5复合分子筛的合成和表征[J]. 燃料化学学报, 2013, 41(5): 601-606. (YANG Rui-juan,YANG Dong-hua,WU Zheng-huang, FENG Xiao-na, TOU Tao, WU Zhong-hua, LI Zhi-hong, YAN Ze,WANG Fan, TANG Qiong. Synthesis and characterization of microporous EU-1/ZSM-5 composite zeolite containing iron[J]. Journal of Fuel Chemistry and Technology, 2013, 41(5): 601-606.)

GANJALA V S P, NEELI C K P, PRAMOD C V, KHAGGA M, RAO K S R, BURRI D R. Eco-friendly nitration of benzenes over zeolite-β-SBA-15 composite catalyst[J]. Catal Commun, 2014, 49(5): 82-86.

JIN Z, LIU S, QIN L, LIU Z, WANG Y, XIE Z, LEI X, WANG Q. Methane dehydroaromatization by Mo-supported MFI-type zeolite with core-shell structure[J]. Appl Catal A: Gen, 2013, 453(26): 295-301.

祝新利, 刘昌俊, 张月萍. 分子筛酸性增强方法研究进展[J]. 现代化工, 2004, 24(12): 12-15. (ZHU Xin-li, LIU Chang-jun, ZHANG Yue-ping. Process in enhancement of zeolite acidity[J]. Modern Chemical Industry, 2004, 24(12): 12-15.)

LIU C, VISSOKOV G P, JANG B W L. Catalyst preparation using plasma technologies[J]. Catal Today, 2002, 72(3): 173-184.

FURUKAWA K, TIAN S R, YAMAUCHI H, YAMAZAKI S, IJIRI H, ARIGA K, KATSUNORI M. Characterization of H-Y zeolite modified by a radio-frequency CF₄ plasma[J]. Chem Phys Lett, 2000, 318(1): 22-26.

TERAMOTO Y, KIM H H, OGATA A, NEGISHI N. Study of plasma-induced surface active oxygen on zeolite-supported silver nanoparticles[J]. Catal Lett, 2013, 143(12): 1374-1378.

施引文献

资源附件(0)

访问统计