Direct synthesis of hierarchical ZSM-5 zeolite using cetyltrimethylammonium as structure directing agent for methanol-to-hydrocarbons conversion

L. Meng, B. Mezari, M.G. Goesten, W. Wannapakdee, R. Pestman, L. Gao, J. Wiesfeld, E.J.M. Hensen

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Abstract

Hierarchical ZSM-5 zeolite can be obtained in a one-step synthesis approach using cetyltrimethyl–ammonium (CTA) as the sole organic template. The reduced crystal domain size and the presence of mesopores result in improved catalytic performance in methanol-to-hydrocarbon (MTH) reaction as compared to bulk ZSM-5. We investigated the role of the base (LiOH, NaOH, KOH, RbOH, CsOH), the H2O/CTA ratio, the Si/Al ratio and counter-ion of CTA (OH−vs. Br−). The crucial role of KOH and RbOH is evident as only these bases allow dissolution of the amorphous silica–alumina precursor to such extent that zeolite crystallization occurs. With other bases, silica dissolution is too limited to start zeolite crystallization, corroborated by the observation that seeding the synthesis gel rapidly led to mesoporous ZSM-5 zeolite for all bases. With KOH, mesoporous zeolite was obtained in the H2O/CTAOH 800–3200 range. The role of Al is also important as without it only ZSM-48 zeolite could be formed, while a too high Si/Al ratio of 20 did not lead to nucleation. A highly crystalline, hierarchical ZSM-5 free from extraframework Al synthesized from a gel with KOH as base, H2O/CTAOH and Si/Al ratios of 800 and 50, respectively displayed the highest catalytic performance in the MTH reaction, outperforming bulk ZSM-5.
Original languageEnglish
Pages (from-to)4520-4533
Number of pages14
JournalCatalysis Science & Technology
Volume7
DOIs
Publication statusPublished - 31 Aug 2017

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Zeolites
Hydrocarbons
Methanol
Dissolution
Gels
Crystallization
Radiation counters
Nucleation
Silica
Crystalline materials
Crystals
Silicon Dioxide
ZSM-5 zeolite
cetrimonium

Cite this

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title = "Direct synthesis of hierarchical ZSM-5 zeolite using cetyltrimethylammonium as structure directing agent for methanol-to-hydrocarbons conversion",
abstract = "Hierarchical ZSM-5 zeolite can be obtained in a one-step synthesis approach using cetyltrimethyl–ammonium (CTA) as the sole organic template. The reduced crystal domain size and the presence of mesopores result in improved catalytic performance in methanol-to-hydrocarbon (MTH) reaction as compared to bulk ZSM-5. We investigated the role of the base (LiOH, NaOH, KOH, RbOH, CsOH), the H2O/CTA ratio, the Si/Al ratio and counter-ion of CTA (OH−vs. Br−). The crucial role of KOH and RbOH is evident as only these bases allow dissolution of the amorphous silica–alumina precursor to such extent that zeolite crystallization occurs. With other bases, silica dissolution is too limited to start zeolite crystallization, corroborated by the observation that seeding the synthesis gel rapidly led to mesoporous ZSM-5 zeolite for all bases. With KOH, mesoporous zeolite was obtained in the H2O/CTAOH 800–3200 range. The role of Al is also important as without it only ZSM-48 zeolite could be formed, while a too high Si/Al ratio of 20 did not lead to nucleation. A highly crystalline, hierarchical ZSM-5 free from extraframework Al synthesized from a gel with KOH as base, H2O/CTAOH and Si/Al ratios of 800 and 50, respectively displayed the highest catalytic performance in the MTH reaction, outperforming bulk ZSM-5.",
author = "L. Meng and B. Mezari and M.G. Goesten and W. Wannapakdee and R. Pestman and L. Gao and J. Wiesfeld and E.J.M. Hensen",
year = "2017",
month = "8",
day = "31",
doi = "10.1039/C7CY01603D",
language = "English",
volume = "7",
pages = "4520--4533",
journal = "Catalysis Science & Technology",
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Direct synthesis of hierarchical ZSM-5 zeolite using cetyltrimethylammonium as structure directing agent for methanol-to-hydrocarbons conversion. / Meng, L.; Mezari, B.; Goesten, M.G.; Wannapakdee, W.; Pestman, R.; Gao, L.; Wiesfeld, J.; Hensen, E.J.M.

In: Catalysis Science & Technology, Vol. 7, 31.08.2017, p. 4520-4533.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Direct synthesis of hierarchical ZSM-5 zeolite using cetyltrimethylammonium as structure directing agent for methanol-to-hydrocarbons conversion

AU - Meng, L.

AU - Mezari, B.

AU - Goesten, M.G.

AU - Wannapakdee, W.

AU - Pestman, R.

AU - Gao, L.

AU - Wiesfeld, J.

AU - Hensen, E.J.M.

PY - 2017/8/31

Y1 - 2017/8/31

N2 - Hierarchical ZSM-5 zeolite can be obtained in a one-step synthesis approach using cetyltrimethyl–ammonium (CTA) as the sole organic template. The reduced crystal domain size and the presence of mesopores result in improved catalytic performance in methanol-to-hydrocarbon (MTH) reaction as compared to bulk ZSM-5. We investigated the role of the base (LiOH, NaOH, KOH, RbOH, CsOH), the H2O/CTA ratio, the Si/Al ratio and counter-ion of CTA (OH−vs. Br−). The crucial role of KOH and RbOH is evident as only these bases allow dissolution of the amorphous silica–alumina precursor to such extent that zeolite crystallization occurs. With other bases, silica dissolution is too limited to start zeolite crystallization, corroborated by the observation that seeding the synthesis gel rapidly led to mesoporous ZSM-5 zeolite for all bases. With KOH, mesoporous zeolite was obtained in the H2O/CTAOH 800–3200 range. The role of Al is also important as without it only ZSM-48 zeolite could be formed, while a too high Si/Al ratio of 20 did not lead to nucleation. A highly crystalline, hierarchical ZSM-5 free from extraframework Al synthesized from a gel with KOH as base, H2O/CTAOH and Si/Al ratios of 800 and 50, respectively displayed the highest catalytic performance in the MTH reaction, outperforming bulk ZSM-5.

AB - Hierarchical ZSM-5 zeolite can be obtained in a one-step synthesis approach using cetyltrimethyl–ammonium (CTA) as the sole organic template. The reduced crystal domain size and the presence of mesopores result in improved catalytic performance in methanol-to-hydrocarbon (MTH) reaction as compared to bulk ZSM-5. We investigated the role of the base (LiOH, NaOH, KOH, RbOH, CsOH), the H2O/CTA ratio, the Si/Al ratio and counter-ion of CTA (OH−vs. Br−). The crucial role of KOH and RbOH is evident as only these bases allow dissolution of the amorphous silica–alumina precursor to such extent that zeolite crystallization occurs. With other bases, silica dissolution is too limited to start zeolite crystallization, corroborated by the observation that seeding the synthesis gel rapidly led to mesoporous ZSM-5 zeolite for all bases. With KOH, mesoporous zeolite was obtained in the H2O/CTAOH 800–3200 range. The role of Al is also important as without it only ZSM-48 zeolite could be formed, while a too high Si/Al ratio of 20 did not lead to nucleation. A highly crystalline, hierarchical ZSM-5 free from extraframework Al synthesized from a gel with KOH as base, H2O/CTAOH and Si/Al ratios of 800 and 50, respectively displayed the highest catalytic performance in the MTH reaction, outperforming bulk ZSM-5.

U2 - 10.1039/C7CY01603D

DO - 10.1039/C7CY01603D

M3 - Article

VL - 7

SP - 4520

EP - 4533

JO - Catalysis Science & Technology

JF - Catalysis Science & Technology

SN - 2044-4753

ER -