低温水热合成ZSM-5/堇青石整体式催化剂

石油炼制与化工 ›› 2015, Vol. 46 ›› Issue (8): 49-53.

低温水热合成ZSM-5/堇青石整体式催化剂

刘一鸣,刘华彦,俞喆雷,陈银飞

浙江工业大学化学工程学院，浙江省绿色化学合成与技术重点实验室

收稿日期:2015-01-19 修回日期:2015-03-18 出版日期:2015-08-12 发布日期:2015-07-27
通讯作者: 刘华彦 E-mail:hyliu@zjut.edu.cn
基金资助:
浙江省社会发展科研项目

LOW TEMPERATURE HYDROTHERMAL SYNTHESIS OF ZSM-5/ CORDIERITE MONOLITH CATALYST

Received:2015-01-19 Revised:2015-03-18 Online:2015-08-12 Published:2015-07-27

摘要/Abstract

摘要： 以蜂窝状堇青石为载体，采用原位水热合成法在120 ℃晶化温度下制备了ZSM-5/堇青石整体式催化剂。采用XRD、SEM对制备得到的整体式催化剂进行表征，并对整体式催化剂进行了牢固度测试以及NO催化氧化活性研究。结果表明，在120 ℃晶化温度下成功制备了15 μm厚负载量为25.8%的ZSM-5分子筛涂层；和传统的170 ℃的晶化温度相比，120 ℃晶化温度下制备的整体式催化剂上分子筛涂层的均匀性更好，牢固度更高。NO催化氧化结果表明，低温晶化下得到的整体式催化剂表现出良好的NO催化氧化效率。

Abstract: A low temperature hydrothermal synthesis method in situ at crystallization temperature 120 ℃ was used to prepare ZSM-5 zeolite coating on cordierite honeycomb ceramic support. The prepared monolith catalysts were characterized by means of X-ray diffractometer (XRD) and scanning electron microscopy (SEM). The firmness of the coating was tested by ultrasonic and thermal shock experiments and the NO oxidation activity of the monolith catalyst at room temperature was investigated. It is found that zeolite coatings with 15 μm thickness (loading 25.8% ZSM-5) are successful synthesized at crystallization temperature of 120 ℃ and that low synthesis temperature favors to the formation of homogeneous distribution of ZSM-5 zeolite on cordierite support. And the thermal shock tests indicate that zeolites coatings synthesized at 120 ℃ show a higher homogeneity and better firmness than that synthesized at 170 ℃. The monolith catalyst synthesized at 120 ℃ also show higher catalytic activity of NO oxidation compared with that synthesized at 170 ℃.

刘一鸣刘华彦俞喆雷陈银飞. 低温水热合成ZSM-5/堇青石整体式催化剂[J]. 石油炼制与化工, 2015, 46(8): 49-53.

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, [1]Vesna Toma?i?, Application of the monoliths in DeNOx catalysis, Catalysis Today. 119 (2007) 106–113.
[2] ZHAI Yanqing, XIONG Jieming, LI Cuiqin,et al. Influence of preparation method on performance of a metal supported perovskite catalyst for combustion of methane[J]. Journal of Rare Earths, 2010, (1):54-58.
[3]Li L, Zhang F, Guan N. Ir/ZSM-5/cordierite monolith for catalytic NOx reduction from automobile exhaust[J]. Catalysis Communi-cations, 2008, 9:409–415.
[4] 王珂, 林志娇, 江志东. 甲烷催化燃烧整体型催化剂研究进展[J]. 天然气化工, 2009, (1):71-78.
[5]赵阳, 郑亚锋, 辛峰. 整体式催化剂性能及应用的研究进展[J]. 化学反应工程与工艺, 2004, (4):357-362.
[6] WANG J, TIAN D, HAN L, et al. In situ synthesized Cu-ZSM-5/cordierite for reduction of NO[J]. Transactions of Nonferrous Metals Society of China, 2011, 21:353–358.
[7] Juan M. Zamaro?, Eduardo E. MiróInstituto de Investigaciones en Catálisis y Petroquímica, Novel binderless zeolite-coated monolith reactor for environmental applications, Argentina Chemical Engineering Journal .165 (2010) 701–708.
[8] Zamaro J M, Ulla M A, Miró E E. Zeolite washcoating onto cordierite honeycomb reactors for environmental applications[J]. Chemical Engineering Journal, 2005, 106(1): 25-33.
[9] Avila P, Montes M, Miró E E. Monolithic reactors for environmental applications : A review on preparation technologies[J]. Chemical Engineering Journal, 2005, 109:11–36.
[10] Yang J, Yu S, Hu H, et al. Synthesis of ZSM-5 hierarchical microsphere-like particle by two stage varying temperature crystallization without secondary template[J]. Chemical Engineering Journal, 2011, 166(3): 1083-1089.
[11] Kim W J, Lee M C, Hayhurst D T. Synthesis of ZSM-5 at low temperature and atmospheric pressure in a pilot-scale batch reac-tor[J]. Microporous and Mesoporous Materials, 1998, 26:133–141.
[12] Ulla M A, Mallada R, Coronas J, et al. Synthesis and characterization of ZSM-5 coatings onto cordierite honeycomb supports[J]. Applied Catalysis A: General, 2003, 253:257–269.
[13] Basaldella E I, Kikot A, Bengoa J F, et al. ZSM-5 zeolite films on cordierite modules. Effect of dilution on the synthesis medium[J]. Materials Letters, 2002, 52:350–354.
[14] Wong W C, Au L T Y, Ariso C T, et al. Effects of synthesis parameters on the zeolite membrane growth[J]. Journal of Membrane Science, 2001, 191:143–163.
[15] Ni Y, Sun A, Wu X, et al. The preparation of nano-sized H[Zn, Al]ZSM-5 zeolite and its application in the aromatization of metha-nol[J]. Mrooro and Mooro Maral, 2011, (2-3):435-442.
[16] Xue Z, Ma J, Zhang T, et al. Synthesis of nanosized ZSM-5 zeolite with intracrystalline mesopores[J]. Materials Letters, 2012:1–3.