Dynamics of water bound to crystalline cellulose

Hugh O'Neill; Sai Venkatesh Pingali; Loukas Petridis; Junhong He; Eugene Mamontov; Liang Hong; Volker Urban; Barbara Evans; Paul Langan; Jeremy C. Smith; Brian H. Davison

doi:10.1038/s41598-017-12035-w

Dynamics of water bound to crystalline cellulose

Hugh O'Neill, Sai Venkatesh Pingali, Loukas Petridis, Junhong He, Eugene Mamontov, Liang Hong, Volker Urban, Barbara Evans, Paul Langan, Jeremy C. Smith, Brian H. Davison

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90 Scopus citations

Abstract

Interactions of water with cellulose are of both fundamental and technological importance. Here, we characterize the properties of water associated with cellulose using deuterium labeling, neutron scattering and molecular dynamics simulation. Quasi-elastic neutron scattering provided quantitative details about the dynamical relaxation processes that occur and was supported by structural characterization using small-angle neutron scattering and X-ray diffraction. We can unambiguously detect two populations of water associated with cellulose. The first is "non-freezing bound" water that gradually becomes mobile with increasing temperature and can be related to surface water. The second population is consistent with confined water that abruptly becomes mobile at ∼260 K, and can be attributed to water that accumulates in the narrow spaces between the microfibrils. Quantitative analysis of the QENS data showed that, at 250 K, the water diffusion coefficient was 0.85 ± 0.04 × 10^-10 m²sec^-1 and increased to 1.77 ± 0.09 × 10^-10 m²sec^-1 at 265 K. MD simulations are in excellent agreement with the experiments and support the interpretation that water associated with cellulose exists in two dynamical populations. Our results provide clarity to previous work investigating the states of bound water and provide a new approach for probing water interactions with lignocellulose materials.

Original language	English
Article number	11840
Journal	Scientific Reports
Volume	7
Issue number	1
DOIs	https://doi.org/10.1038/s41598-017-12035-w
State	Published - Dec 1 2017

Funding

H.O’N., J.H., B.E., J.C.S., P.L. and B.H.D. acknowledge the support of the Genomic Science Program, Office of Biological and Environmental Research (OBER), U.S. Department of Energy, under Contract FWP ERKP752, for sample preparation and QENS studies. SANS studies on Bio-SANS by S.V.P. and V.U. were supported by the OBER funded Center for Structural Molecular Biology (CSMB) under Contract FWP ERKP291, using facilities supported by the Office of Basic Energy Sciences, U.S. Department of Energy. MD simulations performed by L.P. were supported by the Center for Lignocellulose Structure and Formation, an Energy Frontier Research Center, funded by DOE Office of Basic Energy Sciences, under Award DE-SC0001090.This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. E.M. acknowledges the support of Oak Ridge National Laboratory’s Spallation Neutron Source funded by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

Funders	Funder number
Center for Lignocellulose Structure
DOE Office of Basic Energy Sciences	DE-SC0001090
DOE Office of Science
E.M.
Energy Frontier Research Center
Genomic Science Program
J.C.S.
National Energy Research Scientific Computing Center
OBER funded Center for Structural Molecular Biology
Office of Biological and Environmental Research
Scientific User Facilities Division
UT-Battelle
V.U.
U.S. Department of Energy	FWP ERKP752
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Oberkotter Foundation
Canadian Society for Molecular Biosciences	FWP ERKP291

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10.1038/s41598-017-12035-w

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title = "Dynamics of water bound to crystalline cellulose",

abstract = "Interactions of water with cellulose are of both fundamental and technological importance. Here, we characterize the properties of water associated with cellulose using deuterium labeling, neutron scattering and molecular dynamics simulation. Quasi-elastic neutron scattering provided quantitative details about the dynamical relaxation processes that occur and was supported by structural characterization using small-angle neutron scattering and X-ray diffraction. We can unambiguously detect two populations of water associated with cellulose. The first is {"}non-freezing bound{"} water that gradually becomes mobile with increasing temperature and can be related to surface water. The second population is consistent with confined water that abruptly becomes mobile at ∼260 K, and can be attributed to water that accumulates in the narrow spaces between the microfibrils. Quantitative analysis of the QENS data showed that, at 250 K, the water diffusion coefficient was 0.85 ± 0.04 × 10-10 m2sec-1 and increased to 1.77 ± 0.09 × 10-10 m2sec-1 at 265 K. MD simulations are in excellent agreement with the experiments and support the interpretation that water associated with cellulose exists in two dynamical populations. Our results provide clarity to previous work investigating the states of bound water and provide a new approach for probing water interactions with lignocellulose materials.",

author = "Hugh O'Neill and Pingali, {Sai Venkatesh} and Loukas Petridis and Junhong He and Eugene Mamontov and Liang Hong and Volker Urban and Barbara Evans and Paul Langan and Smith, {Jeremy C.} and Davison, {Brian H.}",

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AU - Hong, Liang

AU - Urban, Volker

AU - Evans, Barbara

AU - Langan, Paul

AU - Smith, Jeremy C.

AU - Davison, Brian H.

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N2 - Interactions of water with cellulose are of both fundamental and technological importance. Here, we characterize the properties of water associated with cellulose using deuterium labeling, neutron scattering and molecular dynamics simulation. Quasi-elastic neutron scattering provided quantitative details about the dynamical relaxation processes that occur and was supported by structural characterization using small-angle neutron scattering and X-ray diffraction. We can unambiguously detect two populations of water associated with cellulose. The first is "non-freezing bound" water that gradually becomes mobile with increasing temperature and can be related to surface water. The second population is consistent with confined water that abruptly becomes mobile at ∼260 K, and can be attributed to water that accumulates in the narrow spaces between the microfibrils. Quantitative analysis of the QENS data showed that, at 250 K, the water diffusion coefficient was 0.85 ± 0.04 × 10-10 m2sec-1 and increased to 1.77 ± 0.09 × 10-10 m2sec-1 at 265 K. MD simulations are in excellent agreement with the experiments and support the interpretation that water associated with cellulose exists in two dynamical populations. Our results provide clarity to previous work investigating the states of bound water and provide a new approach for probing water interactions with lignocellulose materials.

AB - Interactions of water with cellulose are of both fundamental and technological importance. Here, we characterize the properties of water associated with cellulose using deuterium labeling, neutron scattering and molecular dynamics simulation. Quasi-elastic neutron scattering provided quantitative details about the dynamical relaxation processes that occur and was supported by structural characterization using small-angle neutron scattering and X-ray diffraction. We can unambiguously detect two populations of water associated with cellulose. The first is "non-freezing bound" water that gradually becomes mobile with increasing temperature and can be related to surface water. The second population is consistent with confined water that abruptly becomes mobile at ∼260 K, and can be attributed to water that accumulates in the narrow spaces between the microfibrils. Quantitative analysis of the QENS data showed that, at 250 K, the water diffusion coefficient was 0.85 ± 0.04 × 10-10 m2sec-1 and increased to 1.77 ± 0.09 × 10-10 m2sec-1 at 265 K. MD simulations are in excellent agreement with the experiments and support the interpretation that water associated with cellulose exists in two dynamical populations. Our results provide clarity to previous work investigating the states of bound water and provide a new approach for probing water interactions with lignocellulose materials.

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Dynamics of water bound to crystalline cellulose

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