Supercritical fluid removal of hydrocarbons adsorbed on wide-pore zeolite catalysts

Lucia M. Petkovic; Daniel M. Ginosar; Kyle C. Burch

doi:10.1016/j.jcat.2005.06.027

Supercritical fluid removal of hydrocarbons adsorbed on wide-pore zeolite catalysts

Lucia M. Petkovic
, Daniel M. Ginosar
, Kyle C. Burch

Materials, Manufacturing, & Bioenergy S&T

Research output: Contribution to journal › Article › peer-review

37 Scopus citations

Abstract

The effect of zeolite pore structure on coke removal by supercritical fluid regeneration (SFR) was studied on a series of wide-pore zeolites, including acidic Y, beta, and mordenite zeolites. Catalyst samples were deactivated under isobutane/butene reaction conditions and treated under flowing supercritical isobutane for 60 min. The chemical nature of the species remaining on the catalyst surface was analyzed by temperature-programmed oxidation, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and ultraviolet-visible spectroscopy. Even though most adsorbed hydrocarbons were removed in some catalysts, DRIFTS spectra indicated that none of the catalysts was completely free of hydrocarbon deposits after SFR. Cyclic reaction/SFR experiments on USY and beta zeolites showed that neither catalyst recovered its initial performance, and also demonstrated a continuous decrease in activity. However, the decrease of activity between cycles was slower in the beta sample, probably due to hindered formation of unsaturated cyclic or polycyclic compounds.

Original language	English
Pages (from-to)	328-339
Number of pages	12
Journal	Journal of Catalysis
Volume	234
Issue number	2
DOIs	https://doi.org/10.1016/j.jcat.2005.06.027
State	Published - Sep 10 2005

Keywords

Acidic zeolites
BEA
Coke analysis
FAU
Isobutane/butene alkylation
MOR
Supercritical fluid regeneration

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10.1016/j.jcat.2005.06.027

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@article{44f4655618c7460ba85c08fe8e4616c7,

title = "Supercritical fluid removal of hydrocarbons adsorbed on wide-pore zeolite catalysts",

abstract = "The effect of zeolite pore structure on coke removal by supercritical fluid regeneration (SFR) was studied on a series of wide-pore zeolites, including acidic Y, beta, and mordenite zeolites. Catalyst samples were deactivated under isobutane/butene reaction conditions and treated under flowing supercritical isobutane for 60 min. The chemical nature of the species remaining on the catalyst surface was analyzed by temperature-programmed oxidation, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and ultraviolet-visible spectroscopy. Even though most adsorbed hydrocarbons were removed in some catalysts, DRIFTS spectra indicated that none of the catalysts was completely free of hydrocarbon deposits after SFR. Cyclic reaction/SFR experiments on USY and beta zeolites showed that neither catalyst recovered its initial performance, and also demonstrated a continuous decrease in activity. However, the decrease of activity between cycles was slower in the beta sample, probably due to hindered formation of unsaturated cyclic or polycyclic compounds.",

keywords = "Acidic zeolites, BEA, Coke analysis, FAU, Isobutane/butene alkylation, MOR, Supercritical fluid regeneration",

author = "Petkovic, \{Lucia M.\} and Ginosar, \{Daniel M.\} and Burch, \{Kyle C.\}",

note = "Funding Information: This research was supported through the INL Laboratory Directed Research and Development Program under DOE Idaho Operations Office Contract DE-AC07-99ID13727. The authors thank Joseph L. Rodriguez for contributing to the experimental work during his internship at INL. The valuable comments made by the editor and the reviewers are also gratefully acknowledged, but of course the authors alone are responsible for any deficiencies that may persist. ",

year = "2005",

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doi = "10.1016/j.jcat.2005.06.027",

language = "English",

volume = "234",

pages = "328--339",

journal = "Journal of Catalysis",

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T1 - Supercritical fluid removal of hydrocarbons adsorbed on wide-pore zeolite catalysts

AU - Petkovic, Lucia M.

AU - Ginosar, Daniel M.

AU - Burch, Kyle C.

N1 - Funding Information: This research was supported through the INL Laboratory Directed Research and Development Program under DOE Idaho Operations Office Contract DE-AC07-99ID13727. The authors thank Joseph L. Rodriguez for contributing to the experimental work during his internship at INL. The valuable comments made by the editor and the reviewers are also gratefully acknowledged, but of course the authors alone are responsible for any deficiencies that may persist.

PY - 2005/9/10

Y1 - 2005/9/10

N2 - The effect of zeolite pore structure on coke removal by supercritical fluid regeneration (SFR) was studied on a series of wide-pore zeolites, including acidic Y, beta, and mordenite zeolites. Catalyst samples were deactivated under isobutane/butene reaction conditions and treated under flowing supercritical isobutane for 60 min. The chemical nature of the species remaining on the catalyst surface was analyzed by temperature-programmed oxidation, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and ultraviolet-visible spectroscopy. Even though most adsorbed hydrocarbons were removed in some catalysts, DRIFTS spectra indicated that none of the catalysts was completely free of hydrocarbon deposits after SFR. Cyclic reaction/SFR experiments on USY and beta zeolites showed that neither catalyst recovered its initial performance, and also demonstrated a continuous decrease in activity. However, the decrease of activity between cycles was slower in the beta sample, probably due to hindered formation of unsaturated cyclic or polycyclic compounds.

AB - The effect of zeolite pore structure on coke removal by supercritical fluid regeneration (SFR) was studied on a series of wide-pore zeolites, including acidic Y, beta, and mordenite zeolites. Catalyst samples were deactivated under isobutane/butene reaction conditions and treated under flowing supercritical isobutane for 60 min. The chemical nature of the species remaining on the catalyst surface was analyzed by temperature-programmed oxidation, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and ultraviolet-visible spectroscopy. Even though most adsorbed hydrocarbons were removed in some catalysts, DRIFTS spectra indicated that none of the catalysts was completely free of hydrocarbon deposits after SFR. Cyclic reaction/SFR experiments on USY and beta zeolites showed that neither catalyst recovered its initial performance, and also demonstrated a continuous decrease in activity. However, the decrease of activity between cycles was slower in the beta sample, probably due to hindered formation of unsaturated cyclic or polycyclic compounds.

KW - Acidic zeolites

KW - BEA

KW - Coke analysis

KW - FAU

KW - Isobutane/butene alkylation

KW - MOR

KW - Supercritical fluid regeneration

UR - https://www.scopus.com/pages/publications/23944436010

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DO - 10.1016/j.jcat.2005.06.027

M3 - Article

AN - SCOPUS:23944436010

SN - 0021-9517

VL - 234

SP - 328

EP - 339

JO - Journal of Catalysis

JF - Journal of Catalysis

IS - 2

ER -

Supercritical fluid removal of hydrocarbons adsorbed on wide-pore zeolite catalysts

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