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Unraveling Cellulose Microfibrils: A Twisted Tale
Author(s) -
Hadden Jodi A.,
French Alfred D.,
Woods Robert J.
Publication year - 2013
Publication title -
biopolymers
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.556
H-Index - 125
eISSN - 1097-0282
pISSN - 0006-3525
DOI - 10.1002/bip.22279
Subject(s) - microfibril , van der waals force , chemistry , hydrogen bond , cellulose , molecular dynamics , force field (fiction) , solvent , chemical physics , molecule , cellulase , work (physics) , computational chemistry , crystallography , thermodynamics , organic chemistry , physics , quantum mechanics
Molecular dynamics (MD) simulations of cellulose microfibrils are pertinent to the paper, textile, and biofuels industries for their unique capacity to characterize dynamic behavior and atomic‐level interactions with solvent molecules and cellulase enzymes. While high‐resolution crystallographic data have established a solid basis for computational analysis of cellulose, previous work has demonstrated a tendency for modeled microfibrils to diverge from the linear experimental structure and adopt a twisted conformation. Here, we investigate the dependence of this twisting behavior on computational approximations and establish the theoretical basis for its occurrence. We examine the role of solvent, the effect of nonbonded force field parameters [partial charges and van der Waals (vdW) contributions], and the use of explicitly modeled oxygen lone pairs in both the solute and solvent. Findings suggest that microfibril twisting is favored by vdW interactions, and counteracted by both intrachain hydrogen bonds and solvent effects at the microfibril surface. © 2013 Wiley Periodicals, Inc. Biopolymers 99: 746–756, 2013.