Synthesis of High-Silica Aluminosilicate Zeolites

407 Pages·1987·11.25 MB·English

by  Johan A., Jacobs, Peter A., Martens

Studies in Surface Science and Catalysis 33
SYNTHESIS OF HIGH-SILICA ALUMINOSILICATE ZEOLITES
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Studies in Surface Science and Catalysis
Advisory Editors: B. Delman and J.T. Yates
Vol. 33
SYNTHESIS OF HIGH-SILICA
ALUMINOSILICATE
ZEOLITES
Peter A. Jacobs and Johan A. Martens
Leboretorium voor Oppervlektecnemie, Katholieke Universiteit Leuven,
B-3030 Leuven, Belgium
with technical assistance from M. Geelen, L. l.eplat. J. Pierre, M.J. Struyven
and M. Tielen
ELSEVIER Amsterdam - Oxford - New York - Tokyo 1987
ELSEVIER SCIENCE PUBLISHERS B.V.
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ISBN 0-444-42814-3 (Vol. 33)
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© Elsevier Science Publishers B.V., 1987
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v
CONTENTS
Studies in Surface Science and Catalysis (other volumes x
in the series)
Scope of the work xv
Acknowledgements XVI
PART I : SELECTED RECIPES FOR THE SYNTHESIS OF HIGH-SILICA
ZEOLITES
* Introduction 3
* General procedure used for the synthesis of high-silica zeolites 3
* Specific recipes 6
1. Synthesis of ZSM-34 6
2. Synthesis of ferrieritejZSM-35-type materials 8
3. Synthesis of ZSM-39 10
4. Synthesis of high-silica ZSM-6 with TMA 11
5. Synthesis of high-silica mordenite 12
6. Synthesis of ZSM-12 13
7. Synthesis of zeolite PHI 15
8. Synthesis of zeolite BETA 16
9. Synthesis of zeolite ZSM-25 17
10. Synthesis of ZSM-5 with TPA 17
11. Synthesis of ZSM-ll 20
12. Synthesis of ZSM-8 21
13. Synthesis of ZSM-48 22
14. Synthesis of ZSM-22 24
* General comments 25
* References 44
PART II HIGH-SILICA ZEOLITES WITH SOLVED STRUCTURE-TYPE 45
CHAPTER I SYNTHESIS OF ZSM-5 ZEOLITES IN THE PRESENCE OF
TETRAPROPYLAMMONIUM IONS 47
* Introduction 47
VI
* The chemistry of aqueous tetrapropylammonium silicate solutions 48
* The Argauer-Landolt invention 53
* The isothermal metastable phase transformation 55
* The dominant factors influencing the crystallization of the MFI
structure 58
1. The Si0 ratio of the gel 58
2A1 203
2. The TPA/Si0 ratio of the gel 61
2
3. The degree of dilution or the H ratio 64
20/Si0 2
4. The M/Si0 ratio 65
2
5. The OH/Si0 ratio 70
2
6. The nature of the silica source 71
* Morphology of ZSM-5 zeolites 72
* Mechanism of ZSM-5 synthesis 80
* The repartition of aluminium throughout the ZSM-5 crystal 91
* Synthesis of ZSM-5 from reactive mixtures prepared with unusual
reactants 96
* Forming of ZSM-5 crystals 97
* Use of seeds 100
* The ZSM-5-silicalite dispute 103
* References 107
CHAPTER II SYNTHESIS OF THE MFI TYPE OF STRUCTURE IN THE
ABSENCE OF TPA 113
* Introduction 113
* Synthesis of ZSM-5 in the presence of quaternary ammonium cations
different from TPA 113
* Synthesis of ZSM-5 in the presence of amines 119
* Synthesis of ZSM-5 in the presence of alcohols 125
* The use of various templates in ZSM-5 synthesis 132
* Synthesis of ZSM-5 in the absence of any organic compound 134
* References 144
CHAPTER III SYNTHESIS OF HIGH-SILICA ZEOLITES WITH THE MEL TYPE
OF STRUCTURE 147
* Introduction 147
* Quaternary salts used as templates in the synthesis of ZSM-ll 147
VII
* Parameters influencing the crystallization rate of ZSM-11 153
* Synthesis of the MEL structure type using diamines 157
* X-ray invisible ZSM-11 zeolites 162
* References 166
CHAPTER IV POTENTIAL MEMBERS OF THE PENTASIL FAMILY OF HIGH-
SILICA ZEOLITES 167
* Introduction 167
* Crystallographic structure of ZSM-5 and ZSM-11 167
* Intergrowths in the pentasil family of zeolites 177
* Experimental discrimination between pure ZSM-5, ZSM-11 zeolites and
their intergrowths 180
* Symmetry changes of ZSM-5 zeolites 185
* Overview of some pentasil-type zeolites claimed in the literature 188
1. ZSM-8 191
2. ZETA-l 193
3. ZETA-3 195
4. NU-4 195
5. NU-5 197
6. Other pentasils 198
* References 212
CHAPTER V : HIGH-SILICA ZEOLITES OF THE FERRIERITE FAMILY 217
* Structure 217
* Synthesis of FER-type materials using inorganic gels 217
* Synthesis of FER-type zeolites in the presence of organics 220
* Differences between various proprietary FER-type materials 226
* References 231
CHAPTER VI : ZEOLITES WITH TON STRUCTURE TYPE 233
* Structure 233
* Synthesis of TON structure types 243
* Differences between the TON-type proprietary zeolites 248
* References 249
VIII
CHAPTER VII: HIGH-SILICA ZEOLITES WITH MTT FRAMEWORK TOPOLOGY 251
* MTT structure types 251
* Synthesis of MTT and related zeolites 260
* References 274
CHAPTER VIII A FAMILY OF ZEOLITES WITH DISORDERED
FERRIERITE-TYPE STRUCTURE 275
* Members of the family 275
* Structure of zeolite ZSM-48 275
* Synthesis of ZSM-48 and related materials 281
1. General conditions 281
2. Influences of silica: alumina ratio 283
3. Nature of templates 284
* Morphology and sorption capacity 289
* References 295
CHAPTER IX : HIGH-SILICA ZEOLITES WITH MTW FRAMEWORK TOPOLOGY 297
* Potential family members of MTW zeolites 297
* Structure of ZSM-12 297
* Synthesis of MTW zeolites 303
* Retention of organics in MTW zeolites 312
* References 319
CHAPTER X SYNTHESIS OF ZEOLITES THAT DO NOT BELONG TO THE
HIGH-SILICA AND/OR SHAPE-SELECTIVE CLASS OF ZEOLITES 321
* Synthesis of siliceous mordenite 321
* Materials with MTN structure type 330
* Siliceous Levynite zeolites 333
* Offretite-erionite zeolites and their intergrowths 342
* Faujasite-type siliceous zeolites 343
* References 346
IX
CHAPTER XI GENERAL CONSIDERATIONS 349
PART III BRIEF DESCRIPTION OF POTENTIAL HIGH-SILICA ZEOLITES
WITH UNKNOWN STRUCTURE 355
* Introduction 357
* ZSM-43 357
* CSZ-l 357
* ZSM-18 358
* Zeolite PHI 358
* Zeolites BETA and NU-2 359
* ZSM-25 359
* EU-7 and EU-12 359
* NU-23 360
* NU-6(l) 360
* TMA-zeolites FU-l and NU-l 361
* ZSM-6 and ZSM-47 361
* ZSM-50 361
* ISI-6 362
* PSH-3 362
* References 382
Subject index 385