The mechanism for catalytic fast pyrolysis of levoglucosan, furfural and furan over HZSM-5: An experimental and theoretical investigation

Amin Osatiashtiani; Jiajun Zhang; Stylianos D. Stefanidis; Xiaolei Zhang; Tony Bridgwater

doi:10.1016/j.fuel.2022.125279

The mechanism for catalytic fast pyrolysis of levoglucosan, furfural and furan over HZSM-5: An experimental and theoretical investigation

Amin Osatiashtiani, Jiajun Zhang, Stylianos D. Stefanidis, Xiaolei Zhang, Tony Bridgwater

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

Abstract

In this work, we have investigated the complicated reaction network of biomass catalytic fast pyrolysis, particularly the decomposition of the key cellulose pyrolysis intermediate, levoglucosan. Fast pyrolysis of levoglucosan using a Py-GC-MS-FID system in the presence of HZSM-5 suggested that furan and furfural are key intermediates to aromatic hydrocarbons. This was followed by theoretical modelling adopting density functional theory (DFT) to unravel the details of the catalytic reaction mechanism from levoglucosan to furan. Our investigations revealed for the first time a direct route from levoglucosan to furan without furfural as an intermediate, with the highest energy barrier along the most favourable pathway to be 2.15 eV. Combined with previously reported mechanisms in the literature, we provide here a detailed reaction network for the conversion of cellulose-derived intermediates to aromatic hydrocarbons.

Original language	English
Article number	125279
Journal	Fuel
Volume	328
Early online date	29 Jul 2022
DOIs	https://doi.org/10.1016/j.fuel.2022.125279
Publication status	Published - 15 Nov 2022

Bibliographical note

© 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license

The authors would like to acknowledge financial support from the Leverhulme Trust Research Grant (RPG-2017-254) and support from EPSRC First Grant (EP/R010986/1). The authors are also grateful for computational support from the UK Materials and Molecular Modelling Hub, which is partially funded by EPSRC (EP/P020194), for which access was obtained via the UKCP consortium and funded by EPSRC grant ref EP/P022561/1.

Keywords

Catalytic fast pyrolysis
Zeolite
DFT modelling
Levoglucosan

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10.1016/j.fuel.2022.125279Licence: CC BY 4.0

The mechanism for catalytic fast pyrolysis of levoglucosan
© 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license 4.0
Final published version, 2.77 MBLicence: CC BY 4.0

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@article{29889789136b423e8e6e2ba19b834834,

title = "The mechanism for catalytic fast pyrolysis of levoglucosan, furfural and furan over HZSM-5: An experimental and theoretical investigation",

abstract = "In this work, we have investigated the complicated reaction network of biomass catalytic fast pyrolysis, particularly the decomposition of the key cellulose pyrolysis intermediate, levoglucosan. Fast pyrolysis of levoglucosan using a Py-GC-MS-FID system in the presence of HZSM-5 suggested that furan and furfural are key intermediates to aromatic hydrocarbons. This was followed by theoretical modelling adopting density functional theory (DFT) to unravel the details of the catalytic reaction mechanism from levoglucosan to furan. Our investigations revealed for the first time a direct route from levoglucosan to furan without furfural as an intermediate, with the highest energy barrier along the most favourable pathway to be 2.15 eV. Combined with previously reported mechanisms in the literature, we provide here a detailed reaction network for the conversion of cellulose-derived intermediates to aromatic hydrocarbons.",

keywords = "Catalytic fast pyrolysis, Zeolite, DFT modelling, Levoglucosan",

author = "Amin Osatiashtiani and Jiajun Zhang and Stefanidis, {Stylianos D.} and Xiaolei Zhang and Tony Bridgwater",

note = "{\textcopyright} 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license The authors would like to acknowledge financial support from the Leverhulme Trust Research Grant (RPG-2017-254) and support from EPSRC First Grant (EP/R010986/1). The authors are also grateful for computational support from the UK Materials and Molecular Modelling Hub, which is partially funded by EPSRC (EP/P020194), for which access was obtained via the UKCP consortium and funded by EPSRC grant ref EP/P022561/1.",

year = "2022",

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doi = "10.1016/j.fuel.2022.125279",

language = "English",

volume = "328",

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TY - JOUR

T1 - The mechanism for catalytic fast pyrolysis of levoglucosan, furfural and furan over HZSM-5: An experimental and theoretical investigation

AU - Osatiashtiani, Amin

AU - Zhang, Jiajun

AU - Stefanidis, Stylianos D.

AU - Zhang, Xiaolei

AU - Bridgwater, Tony

N1 - © 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license The authors would like to acknowledge financial support from the Leverhulme Trust Research Grant (RPG-2017-254) and support from EPSRC First Grant (EP/R010986/1). The authors are also grateful for computational support from the UK Materials and Molecular Modelling Hub, which is partially funded by EPSRC (EP/P020194), for which access was obtained via the UKCP consortium and funded by EPSRC grant ref EP/P022561/1.

PY - 2022/11/15

Y1 - 2022/11/15

N2 - In this work, we have investigated the complicated reaction network of biomass catalytic fast pyrolysis, particularly the decomposition of the key cellulose pyrolysis intermediate, levoglucosan. Fast pyrolysis of levoglucosan using a Py-GC-MS-FID system in the presence of HZSM-5 suggested that furan and furfural are key intermediates to aromatic hydrocarbons. This was followed by theoretical modelling adopting density functional theory (DFT) to unravel the details of the catalytic reaction mechanism from levoglucosan to furan. Our investigations revealed for the first time a direct route from levoglucosan to furan without furfural as an intermediate, with the highest energy barrier along the most favourable pathway to be 2.15 eV. Combined with previously reported mechanisms in the literature, we provide here a detailed reaction network for the conversion of cellulose-derived intermediates to aromatic hydrocarbons.

AB - In this work, we have investigated the complicated reaction network of biomass catalytic fast pyrolysis, particularly the decomposition of the key cellulose pyrolysis intermediate, levoglucosan. Fast pyrolysis of levoglucosan using a Py-GC-MS-FID system in the presence of HZSM-5 suggested that furan and furfural are key intermediates to aromatic hydrocarbons. This was followed by theoretical modelling adopting density functional theory (DFT) to unravel the details of the catalytic reaction mechanism from levoglucosan to furan. Our investigations revealed for the first time a direct route from levoglucosan to furan without furfural as an intermediate, with the highest energy barrier along the most favourable pathway to be 2.15 eV. Combined with previously reported mechanisms in the literature, we provide here a detailed reaction network for the conversion of cellulose-derived intermediates to aromatic hydrocarbons.

KW - Catalytic fast pyrolysis

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KW - DFT modelling

KW - Levoglucosan

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DO - 10.1016/j.fuel.2022.125279

M3 - Article

SN - 0016-2361

VL - 328

JO - Fuel

JF - Fuel

M1 - 125279

ER -

The mechanism for catalytic fast pyrolysis of levoglucosan, furfural and furan over HZSM-5: An experimental and theoretical investigation

Abstract

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Keywords

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