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Title: Gallioaluminosilicate molecular sieves with the faujasite structure

Abstract

Gallioaluminosilicate hydrogels with composition 0.1 Ga{sub 2}O{sub 3}:0.9 Al{sub 2}O{sub 3}:10 SiO{sub 2}:4.0 Na{sub 2}O:150 H{sub 2}O were prepared using sodium aluminate, colloidal silica, and a soluble galliosilicate with composition Ga{sub 2}O{sub 3}:15 SiO{sub 2}:10 Na{sub 2}O:400 H{sub 2}O as a source of gallia. The hydrothermal transformation of these gels at 95 C yields crystals with the faujasite structure when the crystallization reaction is performed in the absence of stirring and with the gmelinite structure (with minor amount of Pt) when crystallization is completed with stirring of the hydrogel. The crystallization time for Na(Ga,Al)Y can be decreased to 15 h from 48 h by raising the crystallization temperature to 110 C from 95 C. The calcined Na(Ga,Al)Y crystals have surface area in the 600 to 660 m{sup 2}/g range and, unless La-stabilized, suffer partial lattice degradation when, following an exchange with an NH{sub 4}NO{sub 3} solution, the NH{sub 4}(Ga,Al)Y crystals are calcined at 500 C in air. This finding is clearly indicated by {sup 27}Al, {sup 71}Ga, and {sup 29}Si MAS NMR spectroscopic results. The {sup 29}Si NMR spectra of samples exchanged and calcined in the absence of La are poorly resolved and their quantitative analysis indicates substantial loss ofmore » Al and Ga from the faujasite framework. Consistent with this interpretation, {sup 27}Al MAS NMR spectra reveal large amounts of octahedrally coordinated species in H(Ga,Al)Y. Moreover, the {sup 71}Ga spectra show no evidence of tetrahedrally coordinated framework Ga. In contrast, the multinuclear NMR data of the H(Ga,Al,La)Y crystals indicate only minor Al and Ga losses from the framework, thus revealing the stabilizing influence of La. Thermodesorption of pyridine and microcalorimetry results with NH{sub 3} have indicated that the La-stabilized H(Ga,Al,La)Y crystals have a more moderate acidity than the reference HY sample. Model fluid cracking catalyst (FCC)-containing H(Ga,Al,La)Y crystals are more active when cracking gas oil under microactivity testing conditions than similarly prepared FCC-containing HY-type zeolites and a reference equilibrium catalyst containing a rare-earth-stabilized HY, indicating that these crystals should be considered as acidic components in commercial FCC preparations.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
MLO Consultants, Atlanta, GA (US)
OSTI Identifier:
20076097
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 192; Journal Issue: 1; Other Information: PBD: 15 May 2000; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 02 PETROLEUM; MOLECULAR SIEVES; GALLIUM OXIDES; ALUMINIUM OXIDES; SILICON OXIDES; SODIUM OXIDES; CRYSTAL STRUCTURE; CHEMICAL PREPARATION; SURFACE AREA; GAS OILS; CATALYTIC CRACKING

Citation Formats

Occelli, M.L., Schweizer, A.E., Fild, C., Schwering, G., Eckert, H., and Auroux, A. Gallioaluminosilicate molecular sieves with the faujasite structure. United States: N. p., 2000. Web. doi:10.1006/jcat.2000.2841.
Occelli, M.L., Schweizer, A.E., Fild, C., Schwering, G., Eckert, H., & Auroux, A. Gallioaluminosilicate molecular sieves with the faujasite structure. United States. doi:10.1006/jcat.2000.2841.
Occelli, M.L., Schweizer, A.E., Fild, C., Schwering, G., Eckert, H., and Auroux, A. Mon . "Gallioaluminosilicate molecular sieves with the faujasite structure". United States. doi:10.1006/jcat.2000.2841.
@article{osti_20076097,
title = {Gallioaluminosilicate molecular sieves with the faujasite structure},
author = {Occelli, M.L. and Schweizer, A.E. and Fild, C. and Schwering, G. and Eckert, H. and Auroux, A.},
abstractNote = {Gallioaluminosilicate hydrogels with composition 0.1 Ga{sub 2}O{sub 3}:0.9 Al{sub 2}O{sub 3}:10 SiO{sub 2}:4.0 Na{sub 2}O:150 H{sub 2}O were prepared using sodium aluminate, colloidal silica, and a soluble galliosilicate with composition Ga{sub 2}O{sub 3}:15 SiO{sub 2}:10 Na{sub 2}O:400 H{sub 2}O as a source of gallia. The hydrothermal transformation of these gels at 95 C yields crystals with the faujasite structure when the crystallization reaction is performed in the absence of stirring and with the gmelinite structure (with minor amount of Pt) when crystallization is completed with stirring of the hydrogel. The crystallization time for Na(Ga,Al)Y can be decreased to 15 h from 48 h by raising the crystallization temperature to 110 C from 95 C. The calcined Na(Ga,Al)Y crystals have surface area in the 600 to 660 m{sup 2}/g range and, unless La-stabilized, suffer partial lattice degradation when, following an exchange with an NH{sub 4}NO{sub 3} solution, the NH{sub 4}(Ga,Al)Y crystals are calcined at 500 C in air. This finding is clearly indicated by {sup 27}Al, {sup 71}Ga, and {sup 29}Si MAS NMR spectroscopic results. The {sup 29}Si NMR spectra of samples exchanged and calcined in the absence of La are poorly resolved and their quantitative analysis indicates substantial loss of Al and Ga from the faujasite framework. Consistent with this interpretation, {sup 27}Al MAS NMR spectra reveal large amounts of octahedrally coordinated species in H(Ga,Al)Y. Moreover, the {sup 71}Ga spectra show no evidence of tetrahedrally coordinated framework Ga. In contrast, the multinuclear NMR data of the H(Ga,Al,La)Y crystals indicate only minor Al and Ga losses from the framework, thus revealing the stabilizing influence of La. Thermodesorption of pyridine and microcalorimetry results with NH{sub 3} have indicated that the La-stabilized H(Ga,Al,La)Y crystals have a more moderate acidity than the reference HY sample. Model fluid cracking catalyst (FCC)-containing H(Ga,Al,La)Y crystals are more active when cracking gas oil under microactivity testing conditions than similarly prepared FCC-containing HY-type zeolites and a reference equilibrium catalyst containing a rare-earth-stabilized HY, indicating that these crystals should be considered as acidic components in commercial FCC preparations.},
doi = {10.1006/jcat.2000.2841},
journal = {Journal of Catalysis},
issn = {0021-9517},
number = 1,
volume = 192,
place = {United States},
year = {2000},
month = {5}
}