Ab Initio Screening Approach for the Discovery of Lignin Polymer Breaking Pathways
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MarJPCA15.pdf
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Author(s)
Liu, Fang
Mar, Brendan D.
Qi, Helena Wen
Kulik, Heather Janine
Date Issued
May 2015
Journal
Journal of Physical Chemistry A
Publisher
American Chemical Society (ACS)
Citation
Mar, Brendan D., Helena W. Qi, Fang Liu, and Heather J. Kulik. “Ab Initio Screening Approach for the Discovery of Lignin Polymer Breaking Pathways.” Journal of Physical Chemistry A 119, no. 24 (June 18, 2015): 6551-6562.
Version
Author's final manuscript
Abstract
The directed depolymerization of lignin biopolymers is of utmost relevance for the valorization or commercialization of biomass fuels. We present a computational and theoretical screening approach to identify potential cleavage pathways and resulting fragments that are formed during depolymerization of lignin oligomers containing two to six monomers. We have developed a chemical discovery technique to identify the chemically relevant putative fragments in eight known polymeric linkage types of lignin. Obtaining these structures is a crucial precursor to the development of any further kinetic modeling. We have developed this approach by adapting steered molecular dynamics calculations under constant force and varying the points of applied force in the molecule to diversify the screening approach. Key observations include relationships between abundance and breaking frequency, the relative diversity of potential pathways for a given linkage, and the observation that readily cleaved bonds can destabilize adjacent bonds, causing subsequent automatic cleavage.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1021/acs.jpca.5b03503
