Mesoporous ZSM-5 zeolite catalysts prepared by desilication with organic hydroxides and comparison with NaOH leaching

被引:290
作者
Abello, Sonia [1 ]
Bonilla, Adriana [1 ]
Perez-Ramirez, Javier [1 ,2 ]
机构
[1] Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain
[2] Passeig Lluis Co 23, Catalan Inst Res & Adv Studies ICREA, Barcelona 08010, Spain
关键词
Hierarchical zeolites; Mesoporous ZSM-5; Desilication; Organic base; Tetraalkylammonium hydroxide; NaOH; Benzene alkylation; ALKALI-TREATMENT; MFI ZEOLITES; PERFORMANCE; MECHANISM; DIFFUSION; METHANOL; BENZENE; H-ZSM-5; CO;
D O I
10.1016/j.apcata.2009.05.055
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Hierarchical zeolites combining micro- and mesoporosity were prepared by desilication of ZSM-5 (Si/Al = 42) in aqueous solutions of tetraalkylammonium hydroxides (TPAOH, TBAOH). Similarities between the treatment mediated by organic hydroxides and the conventional NaOH leaching comprised (i) the requirement to work with a starting zeolite in the optimal Si/Al window of 25-50 and (ii) the minor influence of the counter-cation (H+, NH4+, Na+) on the degree of mesoporosity developed. However, both desilication media presented distinctive kinetic and mechanistic characteristics. The use of organic hydroxides directly produced the protonic form of the mesoporous zeolite upon calcination, simplifying the final ion exchange with NH4NO3 characteristic of the NaOH treatment. Silicon dissolution in TPAOH (or TBAOH) was much slower than in NaOH, making the demetallation process highly controllable. The treatment in the organic base was less selective for silicon extraction, i.e. a higher amount of aluminum was leached to the solution compared to the NaOH treatment. The differences in porosity development and chemical composition of the final solid can be assigned to the effect of the bulky tetraalkylammonium cation. The optimal hierarchical ZSM-5 zeolite (treated in I M TPAOH at 338 K and 8 h) had a mesopore surface area of 160 m(2) g(-1) and the intrinsic zeolite properties were largely preserved. This sample displayed improved catalytic performance in the liquid-phase benzene alkylation with ethylene compared to the parent and NaOH-treated zeolites. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:191 / 198
页数:8
相关论文
共 35 条
[1]  
[Anonymous], 1996, ADV INORGANIC CHEM
[2]   THE DETERMINATION OF PORE VOLUME AND AREA DISTRIBUTIONS IN POROUS SUBSTANCES .1. COMPUTATIONS FROM NITROGEN ISOTHERMS [J].
BARRETT, EP ;
JOYNER, LG ;
HALENDA, PP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (01) :373-380
[3]   Methanol to gasoline over zeolite H-ZSM-5: Improved catalyst performance by treatment with NaOH [J].
Bjorgen, Morten ;
Joensen, Finn ;
Holm, Martin Spangsberg ;
Olsbye, Unni ;
Lillerud, Karl-Petter ;
Svelle, Stian .
APPLIED CATALYSIS A-GENERAL, 2008, 345 (01) :43-50
[4]   Alkylation of benzene with short-chain olefins over MCM-22 zeolite:: Catalytic behaviour and kinetic mechanism [J].
Corma, A ;
Martínez-Soria, V ;
Schnoeveld, E .
JOURNAL OF CATALYSIS, 2000, 192 (01) :163-173
[5]   HEATS OF MIXING AND HEATS OF DILUTION OF TETRAPROPYLAMMONIUM CHLORIDE - TEMPERATURE-DEPENDENCE [J].
ENSOR, DD ;
ANDERSON, HL ;
CONALLY, TG .
JOURNAL OF PHYSICAL CHEMISTRY, 1974, 78 (01) :77-80
[6]  
Fessenden RJ., 1982, ORGANIC CHEM, V2nd
[7]   Mesoporous ZSM-5 zeolites via alkali treatment for the direct hydroxylation of benzene to phenol with N2O [J].
Gopalakrishnan, S. ;
Zampieri, A. ;
Schwieger, W. .
JOURNAL OF CATALYSIS, 2008, 260 (01) :193-197
[8]   Mechanism of hierarchical porosity development in MFI zeolites by desilication:: The role of aluminium as a pore-directing agent [J].
Groen, JC ;
Peffer, LAA ;
Moulijn, JA ;
Pérez-Ramírez, J .
CHEMISTRY-A EUROPEAN JOURNAL, 2005, 11 (17) :4983-4994
[9]   Mesoporosity development in ZSM-5 zeolite upon optimized desilication conditions in alkaline medium [J].
Groen, JC ;
Peffer, LAA ;
Moulijn, JA ;
Pérez-Ramírez, J .
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 2004, 241 (1-3) :53-58
[10]   On the introduction of intracrystalline mesoporosity in zeolites upon desilication in alkaline medium [J].
Groen, JC ;
Peffer, LAA ;
Moulijn, JA ;
Pérez-Ramírez, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 2004, 69 (1-2) :29-34