Synthesis of mesoporous ZSM-5 zeolite encapsulated in an ultrathin protective shell of silicalite-1 for MTH conversion

Farnoosh Goodarzi, Irene Pinilla Herrero, Georgios N. Kalantzopoulos, Stian Svelle, Andrea Lazzarini, Pablo Beato, Unni Olsbye, Søren Kegnæs*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Coke formation is a major reason in deactivation of acidic zeolite catalysts in industrial processes such as methanol to hydrocarbons conversion. Protecting the surface of acidic zeolite with an inert porous shell can greatly hinder the coke formation on the surface, and hence boost the lifetime of the catalyst. In this work, a solid-state steam-assisted method for synthesis of such optimized protective shell (silicate-1, ~15 nm thickness) is designed. This general and simple protocol can be applied to acidic zeolite catalysts to improve their catalytic lifetime. The silicalite-1 shell is synthesized on mesoporous ZSM-5 zeolite to explore its catalytic activity in methanol to hydrocarbons conversion. XPS and TEM analysis confirm the coverage of mesoporous zeolite crystals by non-acidic shell. In addition, nitrogen physisorption shows the accessibility of mesoporous ZSM-5 via microporous silicalite-1 network. Applying this protective shell increases the lifetime of the catalyst by 100% and its conversion capacity by 130%, in comparison to mesoporous ZSM-5 without the shell. The controlled formation of thin layer of microporous silicalite-1 around mesoporous ZSM-5 crystals (without growth of individual silicalite-1) accounts for enhanced catalytic improvement.
Original languageEnglish
Article number109730
JournalMicroporous and mesoporous materials
Volume292
Number of pages10
ISSN1387-1811
DOIs
Publication statusPublished - 2020

Keywords

  • Shell
  • Coke
  • Zeloite
  • Mesoporous
  • Hetergeneous catalysis
  • Methanol

Cite this

Goodarzi, Farnoosh ; Herrero, Irene Pinilla ; Kalantzopoulos, Georgios N. ; Svelle, Stian ; Lazzarini, Andrea ; Beato, Pablo ; Olsbye, Unni ; Kegnæs, Søren. / Synthesis of mesoporous ZSM-5 zeolite encapsulated in an ultrathin protective shell of silicalite-1 for MTH conversion. In: Microporous and mesoporous materials. 2020 ; Vol. 292.
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title = "Synthesis of mesoporous ZSM-5 zeolite encapsulated in an ultrathin protective shell of silicalite-1 for MTH conversion",
abstract = "Coke formation is a major reason in deactivation of acidic zeolite catalysts in industrial processes such as methanol to hydrocarbons conversion. Protecting the surface of acidic zeolite with an inert porous shell can greatly hinder the coke formation on the surface, and hence boost the lifetime of the catalyst. In this work, a solid-state steam-assisted method for synthesis of such optimized protective shell (silicate-1, ~15 nm thickness) is designed. This general and simple protocol can be applied to acidic zeolite catalysts to improve their catalytic lifetime. The silicalite-1 shell is synthesized on mesoporous ZSM-5 zeolite to explore its catalytic activity in methanol to hydrocarbons conversion. XPS and TEM analysis confirm the coverage of mesoporous zeolite crystals by non-acidic shell. In addition, nitrogen physisorption shows the accessibility of mesoporous ZSM-5 via microporous silicalite-1 network. Applying this protective shell increases the lifetime of the catalyst by 100{\%} and its conversion capacity by 130{\%}, in comparison to mesoporous ZSM-5 without the shell. The controlled formation of thin layer of microporous silicalite-1 around mesoporous ZSM-5 crystals (without growth of individual silicalite-1) accounts for enhanced catalytic improvement.",
keywords = "Shell, Coke, Zeloite, Mesoporous, Hetergeneous catalysis, Methanol",
author = "Farnoosh Goodarzi and Herrero, {Irene Pinilla} and Kalantzopoulos, {Georgios N.} and Stian Svelle and Andrea Lazzarini and Pablo Beato and Unni Olsbye and S{\o}ren Kegn{\ae}s",
year = "2020",
doi = "10.1016/j.micromeso.2019.109730",
language = "English",
volume = "292",
journal = "Microporous and Mesoporous Materials",
issn = "1387-1811",
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Synthesis of mesoporous ZSM-5 zeolite encapsulated in an ultrathin protective shell of silicalite-1 for MTH conversion. / Goodarzi, Farnoosh; Herrero, Irene Pinilla; Kalantzopoulos, Georgios N.; Svelle, Stian; Lazzarini, Andrea; Beato, Pablo; Olsbye, Unni; Kegnæs, Søren.

In: Microporous and mesoporous materials, Vol. 292, 109730, 2020.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Synthesis of mesoporous ZSM-5 zeolite encapsulated in an ultrathin protective shell of silicalite-1 for MTH conversion

AU - Goodarzi, Farnoosh

AU - Herrero, Irene Pinilla

AU - Kalantzopoulos, Georgios N.

AU - Svelle, Stian

AU - Lazzarini, Andrea

AU - Beato, Pablo

AU - Olsbye, Unni

AU - Kegnæs, Søren

PY - 2020

Y1 - 2020

N2 - Coke formation is a major reason in deactivation of acidic zeolite catalysts in industrial processes such as methanol to hydrocarbons conversion. Protecting the surface of acidic zeolite with an inert porous shell can greatly hinder the coke formation on the surface, and hence boost the lifetime of the catalyst. In this work, a solid-state steam-assisted method for synthesis of such optimized protective shell (silicate-1, ~15 nm thickness) is designed. This general and simple protocol can be applied to acidic zeolite catalysts to improve their catalytic lifetime. The silicalite-1 shell is synthesized on mesoporous ZSM-5 zeolite to explore its catalytic activity in methanol to hydrocarbons conversion. XPS and TEM analysis confirm the coverage of mesoporous zeolite crystals by non-acidic shell. In addition, nitrogen physisorption shows the accessibility of mesoporous ZSM-5 via microporous silicalite-1 network. Applying this protective shell increases the lifetime of the catalyst by 100% and its conversion capacity by 130%, in comparison to mesoporous ZSM-5 without the shell. The controlled formation of thin layer of microporous silicalite-1 around mesoporous ZSM-5 crystals (without growth of individual silicalite-1) accounts for enhanced catalytic improvement.

AB - Coke formation is a major reason in deactivation of acidic zeolite catalysts in industrial processes such as methanol to hydrocarbons conversion. Protecting the surface of acidic zeolite with an inert porous shell can greatly hinder the coke formation on the surface, and hence boost the lifetime of the catalyst. In this work, a solid-state steam-assisted method for synthesis of such optimized protective shell (silicate-1, ~15 nm thickness) is designed. This general and simple protocol can be applied to acidic zeolite catalysts to improve their catalytic lifetime. The silicalite-1 shell is synthesized on mesoporous ZSM-5 zeolite to explore its catalytic activity in methanol to hydrocarbons conversion. XPS and TEM analysis confirm the coverage of mesoporous zeolite crystals by non-acidic shell. In addition, nitrogen physisorption shows the accessibility of mesoporous ZSM-5 via microporous silicalite-1 network. Applying this protective shell increases the lifetime of the catalyst by 100% and its conversion capacity by 130%, in comparison to mesoporous ZSM-5 without the shell. The controlled formation of thin layer of microporous silicalite-1 around mesoporous ZSM-5 crystals (without growth of individual silicalite-1) accounts for enhanced catalytic improvement.

KW - Shell

KW - Coke

KW - Zeloite

KW - Mesoporous

KW - Hetergeneous catalysis

KW - Methanol

U2 - 10.1016/j.micromeso.2019.109730

DO - 10.1016/j.micromeso.2019.109730

M3 - Journal article

VL - 292

JO - Microporous and Mesoporous Materials

JF - Microporous and Mesoporous Materials

SN - 1387-1811

M1 - 109730

ER -