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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.

Authors:
ORCiD logo; ; ; ; ; ; ORCiD logo; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Laboratory, Oak Ridge Leadership Computing Facility (OLCF); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Lignocellulose Structure and Formation (CLSF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1394309
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
60 APPLIED LIFE SCIENCES; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

O’Neill, Hugh, Pingali, Sai Venkatesh, Petridis, Loukas, He, Junhong, Mamontov, Eugene, Hong, Liang, Urban, Volker, Evans, Barbara, Langan, Paul, Smith, Jeremy C., and Davison, Brian H. Dynamics of water bound to crystalline cellulose. United States: N. p., 2017. Web. doi:10.1038/s41598-017-12035-w.
O’Neill, Hugh, Pingali, Sai Venkatesh, Petridis, Loukas, He, Junhong, Mamontov, Eugene, Hong, Liang, Urban, Volker, Evans, Barbara, Langan, Paul, Smith, Jeremy C., & Davison, Brian H. Dynamics of water bound to crystalline cellulose. United States. doi:10.1038/s41598-017-12035-w.
O’Neill, Hugh, Pingali, Sai Venkatesh, Petridis, Loukas, He, Junhong, Mamontov, Eugene, Hong, Liang, Urban, Volker, Evans, Barbara, Langan, Paul, Smith, Jeremy C., and Davison, Brian H. Tue . "Dynamics of water bound to crystalline cellulose". United States. doi:10.1038/s41598-017-12035-w.
@article{osti_1394309,
title = {Dynamics of water bound to crystalline cellulose},
author = {O’Neill, Hugh and Pingali, Sai Venkatesh and Petridis, Loukas and He, Junhong and Mamontov, Eugene and Hong, Liang and Urban, Volker and Evans, Barbara and Langan, Paul and Smith, Jeremy C. and Davison, Brian H.},
abstractNote = {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.},
doi = {10.1038/s41598-017-12035-w},
journal = {Scientific Reports},
issn = {2045-2322},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {9}
}

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