Chirality and bound water in the hierarchical cellulose structure

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Chirality and bound water in the hierarchical cellulose structure. / Paajanen, Antti; Ceccherini, Sara; Maloney, Thaddeus; Ketoja, Jukka A.

In: Cellulose, Vol. 26, No. 10, 15.07.2019, p. 5877-5892.

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Paajanen, Antti ; Ceccherini, Sara ; Maloney, Thaddeus ; Ketoja, Jukka A. / Chirality and bound water in the hierarchical cellulose structure. In: Cellulose. 2019 ; Vol. 26, No. 10. pp. 5877-5892.

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@article{015d21412a384910bbd791950182e8d4,
title = "Chirality and bound water in the hierarchical cellulose structure",
abstract = "Abstract: The origins of the unique properties of natural fibres have remained largely unresolved because of the complex interrelations between structural hierarchy, chirality and bound water. In this paper, analysis of the melting endotherms for bleached hardwood pulps indicates that the amount of non-freezing bound water (0.21 g/g) is roughly half of the amount of freezing bound water (0.42 g/g). We link this result to the two smallest constitutive units, microfibrils and their bundles, using molecular dynamics simulations at both hierarchical levels. The molecular water layers found in the simulations correspond quite accurately to the measured amount of non-freezing and freezing bound water. Disorder that results from the microfibril twist and amphiphilicity prevents co-crystallisation, leaving routes for water molecules to diffuse inside the microfibril bundle. Moreover, the simulations predict correctly the magnitude of the right-handed twist at different hierarchical levels. Significant changes in hydroxymethyl group conformations are seen during twisting that compare well with existing experimental data. Our findings go beyond earlier modelling studies in predicting the twist and structure of the microfibril bundle.",
keywords = "Bound water, Cellulose, Macrofibril, Microfibril, Molecular dynamics, Twist",
author = "Antti Paajanen and Sara Ceccherini and Thaddeus Maloney and Ketoja, {Jukka A.}",
year = "2019",
month = "7",
day = "15",
doi = "10.1007/s10570-019-02525-7",
language = "English",
volume = "26",
pages = "5877--5892",
journal = "Cellulose",
issn = "0969-0239",
number = "10",

}

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TY - JOUR

T1 - Chirality and bound water in the hierarchical cellulose structure

AU - Paajanen, Antti

AU - Ceccherini, Sara

AU - Maloney, Thaddeus

AU - Ketoja, Jukka A.

PY - 2019/7/15

Y1 - 2019/7/15

N2 - Abstract: The origins of the unique properties of natural fibres have remained largely unresolved because of the complex interrelations between structural hierarchy, chirality and bound water. In this paper, analysis of the melting endotherms for bleached hardwood pulps indicates that the amount of non-freezing bound water (0.21 g/g) is roughly half of the amount of freezing bound water (0.42 g/g). We link this result to the two smallest constitutive units, microfibrils and their bundles, using molecular dynamics simulations at both hierarchical levels. The molecular water layers found in the simulations correspond quite accurately to the measured amount of non-freezing and freezing bound water. Disorder that results from the microfibril twist and amphiphilicity prevents co-crystallisation, leaving routes for water molecules to diffuse inside the microfibril bundle. Moreover, the simulations predict correctly the magnitude of the right-handed twist at different hierarchical levels. Significant changes in hydroxymethyl group conformations are seen during twisting that compare well with existing experimental data. Our findings go beyond earlier modelling studies in predicting the twist and structure of the microfibril bundle.

AB - Abstract: The origins of the unique properties of natural fibres have remained largely unresolved because of the complex interrelations between structural hierarchy, chirality and bound water. In this paper, analysis of the melting endotherms for bleached hardwood pulps indicates that the amount of non-freezing bound water (0.21 g/g) is roughly half of the amount of freezing bound water (0.42 g/g). We link this result to the two smallest constitutive units, microfibrils and their bundles, using molecular dynamics simulations at both hierarchical levels. The molecular water layers found in the simulations correspond quite accurately to the measured amount of non-freezing and freezing bound water. Disorder that results from the microfibril twist and amphiphilicity prevents co-crystallisation, leaving routes for water molecules to diffuse inside the microfibril bundle. Moreover, the simulations predict correctly the magnitude of the right-handed twist at different hierarchical levels. Significant changes in hydroxymethyl group conformations are seen during twisting that compare well with existing experimental data. Our findings go beyond earlier modelling studies in predicting the twist and structure of the microfibril bundle.

KW - Bound water

KW - Cellulose

KW - Macrofibril

KW - Microfibril

KW - Molecular dynamics

KW - Twist

UR - http://www.scopus.com/inward/record.url?scp=85066860589&partnerID=8YFLogxK

U2 - 10.1007/s10570-019-02525-7

DO - 10.1007/s10570-019-02525-7

M3 - Article

VL - 26

SP - 5877

EP - 5892

JO - Cellulose

JF - Cellulose

SN - 0969-0239

IS - 10

ER -

ID: 34643365