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Title: Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors

Here, the catalytic fast pyrolysis (CFP) of biomass is a promising technology for producing renewable transportation fuels and chemicals. MFI-type catalysts have shown promise for CFP because they produce gasoline range hydrocarbons from oxygenated pyrolysis compounds; however, rapid catalyst deactivation due to coking is one of the major technical barriers inhibiting the commercialization of this technology. Coke deposited on the surface of the catalysts blocks access to active sites in the micropores leading to rapid catalyst deactivation. Our strategy is to minimize rapid catalyst deactivation by adding mesoporosity through forming MFI nanosheet materials. The synthesized MFI nanosheet catalysts were fully characterized and evaluated for cellulose pyrolysis vapor upgrading to produce olefins and aromatic hydrocarbons. The data obtained from pyrolysis-GCMS (py-GCMS), showed that fresh MFI nanosheets produced similar aromatic hydrocarbon and olefin yields compared to conventional HZSM-5. However, MFI nanosheets demonstrated a longer lifetime than HZSM-5 even though coke contents were also higher than for HZSM-5 because the mesopores enabled better accessibility to active acid sites. This conclusion was supported by results from post-reaction analysis of various spent catalysts collected at different points during the deactivation experiments.
Authors:
 [1] ;  [2] ;  [2] ;  [1] ;  [3] ;  [3] ;  [2] ;  [2] ;  [3] ;  [1]
  1. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Colorado School of Mines, Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5100-68461
Journal ID: ISSN 2168-0485
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 5; Journal Issue: 6; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; HZSM-5 deactivation; mesoporous zeolite; catalytic fast pyrolysis; coke formation; mesoporosity; zeolite acidity
OSTI Identifier:
1364155

Xu, Mengze, Mukarakate, Calvin, Iisa, Kristiina, Budhi, Sridhar, Menart, Martin, Davidson, Malcolm, Robichaud, David J., Nimlos, Mark R., Trewyn, Brian G., and Richards, Ryan M.. Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors. United States: N. p., Web. doi:10.1021/acssuschemeng.7b00817.
Xu, Mengze, Mukarakate, Calvin, Iisa, Kristiina, Budhi, Sridhar, Menart, Martin, Davidson, Malcolm, Robichaud, David J., Nimlos, Mark R., Trewyn, Brian G., & Richards, Ryan M.. Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors. United States. doi:10.1021/acssuschemeng.7b00817.
Xu, Mengze, Mukarakate, Calvin, Iisa, Kristiina, Budhi, Sridhar, Menart, Martin, Davidson, Malcolm, Robichaud, David J., Nimlos, Mark R., Trewyn, Brian G., and Richards, Ryan M.. 2017. "Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors". United States. doi:10.1021/acssuschemeng.7b00817. https://www.osti.gov/servlets/purl/1364155.
@article{osti_1364155,
title = {Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors},
author = {Xu, Mengze and Mukarakate, Calvin and Iisa, Kristiina and Budhi, Sridhar and Menart, Martin and Davidson, Malcolm and Robichaud, David J. and Nimlos, Mark R. and Trewyn, Brian G. and Richards, Ryan M.},
abstractNote = {Here, the catalytic fast pyrolysis (CFP) of biomass is a promising technology for producing renewable transportation fuels and chemicals. MFI-type catalysts have shown promise for CFP because they produce gasoline range hydrocarbons from oxygenated pyrolysis compounds; however, rapid catalyst deactivation due to coking is one of the major technical barriers inhibiting the commercialization of this technology. Coke deposited on the surface of the catalysts blocks access to active sites in the micropores leading to rapid catalyst deactivation. Our strategy is to minimize rapid catalyst deactivation by adding mesoporosity through forming MFI nanosheet materials. The synthesized MFI nanosheet catalysts were fully characterized and evaluated for cellulose pyrolysis vapor upgrading to produce olefins and aromatic hydrocarbons. The data obtained from pyrolysis-GCMS (py-GCMS), showed that fresh MFI nanosheets produced similar aromatic hydrocarbon and olefin yields compared to conventional HZSM-5. However, MFI nanosheets demonstrated a longer lifetime than HZSM-5 even though coke contents were also higher than for HZSM-5 because the mesopores enabled better accessibility to active acid sites. This conclusion was supported by results from post-reaction analysis of various spent catalysts collected at different points during the deactivation experiments.},
doi = {10.1021/acssuschemeng.7b00817},
journal = {ACS Sustainable Chemistry & Engineering},
number = 6,
volume = 5,
place = {United States},
year = {2017},
month = {5}
}