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Title: Mobility of Water on Oxide Surfaces Studied by QENS

Abstract

Although neutron scattering is often considered a bulk probe, we demonstrate that the mobility of surface water on oxide nano-powders can be investigated using quasielastic neutron scattering. We discuss how the reduced number of hydrogen bonds per water molecule associated with surface confinement leads to a qualitative modification of single-particle translational dynamics compared to bulk water. The mobility of surface water in zirconium oxide with two hydration layers present is discussed in detail. The outer hydration layer exhibits translational dynamics on the time scale of tens of picoseconds, and thus can be studied using time-of-flight neutron spectrometry. The translational dynamics of the inner hydration layer in the range of hundreds of picoseconds can be assessed with backscattering neutron spectrometry. Interestingly, despite being slower by two orders of magnitude, the translational motion of the molecules of the inner hydration layer may share more common traits with bulk water compared to the motion of the outer hydration layer, the dynamics of which is slower than that of bulk water by just one order of magnitude. Similar to bulk water, the temperature dependence of the residence time for the water molecules of the inner hydration layer is non-Arrhenius, and can be described bymore » a Vogel-Fulcher-Tammann (VFT) law. On the other hand, the molecules of the outer hydration layer demonstrate Arrhenius-type temperature dependence indicative of thermally activated surface jump diffusion. Our recent study of surface water on cerium oxide, which exhibits faster dynamics compared to water on zirconium oxide, has ventured into the low-temperature region (down to 200 K). Below 215 K, we have found a deviation from the VFT temperature dependence for the residence time indicative of a surprise "fragile"-to-"strong" transition in the surface water. While "fragile"-to-"strong" transition has been predicted in supercooled bulk water, there has been no prediction of such a transition in surface water. We discuss the links between our results and recent work on hydration water in carbon nanotubes and proteins.« less

Authors:
 [1]
  1. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
930776
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Conference
Resource Relation:
Conference: The Eighth International Conference on Quasi-Elastic Neutron Scattering, Bloomington, IN, USA, 20060614, 20060617
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; CERIUM OXIDES; HYDRATION; NEUTRONS; OXIDES; SCATTERING; SURFACE WATERS; TEMPERATURE DEPENDENCE; WATER; ZIRCONIUM OXIDES

Citation Formats

Mamontov, Eugene. Mobility of Water on Oxide Surfaces Studied by QENS. United States: N. p., 2007. Web.
Mamontov, Eugene. Mobility of Water on Oxide Surfaces Studied by QENS. United States.
Mamontov, Eugene. Mon . "Mobility of Water on Oxide Surfaces Studied by QENS". United States. doi:.
@article{osti_930776,
title = {Mobility of Water on Oxide Surfaces Studied by QENS},
author = {Mamontov, Eugene},
abstractNote = {Although neutron scattering is often considered a bulk probe, we demonstrate that the mobility of surface water on oxide nano-powders can be investigated using quasielastic neutron scattering. We discuss how the reduced number of hydrogen bonds per water molecule associated with surface confinement leads to a qualitative modification of single-particle translational dynamics compared to bulk water. The mobility of surface water in zirconium oxide with two hydration layers present is discussed in detail. The outer hydration layer exhibits translational dynamics on the time scale of tens of picoseconds, and thus can be studied using time-of-flight neutron spectrometry. The translational dynamics of the inner hydration layer in the range of hundreds of picoseconds can be assessed with backscattering neutron spectrometry. Interestingly, despite being slower by two orders of magnitude, the translational motion of the molecules of the inner hydration layer may share more common traits with bulk water compared to the motion of the outer hydration layer, the dynamics of which is slower than that of bulk water by just one order of magnitude. Similar to bulk water, the temperature dependence of the residence time for the water molecules of the inner hydration layer is non-Arrhenius, and can be described by a Vogel-Fulcher-Tammann (VFT) law. On the other hand, the molecules of the outer hydration layer demonstrate Arrhenius-type temperature dependence indicative of thermally activated surface jump diffusion. Our recent study of surface water on cerium oxide, which exhibits faster dynamics compared to water on zirconium oxide, has ventured into the low-temperature region (down to 200 K). Below 215 K, we have found a deviation from the VFT temperature dependence for the residence time indicative of a surprise "fragile"-to-"strong" transition in the surface water. While "fragile"-to-"strong" transition has been predicted in supercooled bulk water, there has been no prediction of such a transition in surface water. We discuss the links between our results and recent work on hydration water in carbon nanotubes and proteins.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}

Conference:
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