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Title: Vibrational Density of States of Strongly H-Bonded Interfacial Water: Insights from Inelastic Neutron Scattering and Theory

Abstract

The vibrational dynamics of water and OH sorbed on SnO2 nanoparticles were probed with inelastic neutron scattering and analyzed with the assistance of ab-initio molecular dynamics. The combined analysis points to the existence of very strong hydrogen bonds at the surface with a formation enthalpy twice the average value for liquid water. This unusually large interaction results in (i) decoupling of the hydrated surface from the water system due to an epitaxially-induced screening layer, resulting in an apparent ice-like INS signal at multilayer coverage, (ii) splitting of OH wagging modes that can be used as an experimental indication of the strength of the surface hydrogen bonds, and (iii) high proton exchange rates and high degree of water dissociation at the interface. Our analysis provides general guidance into the tuning of surface hydrophobicity at the molecular level.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [1];  [2]
  1. ORNL
  2. Pennsylvania State University
Publication Date:
Research Org.:
Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1156714
DOE Contract Number:
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Science; Journal Volume: 118; Journal Issue: 20
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Hsiu-Wen, Dellostritto, Mark J, Kumar, Nitin, Kolesnikov, Alexander I, Kent, Paul R, Kubicki, James D., Wesolowski, David J, and Sofo, Jorge O. Vibrational Density of States of Strongly H-Bonded Interfacial Water: Insights from Inelastic Neutron Scattering and Theory. United States: N. p., 2014. Web. doi:10.1021/jp500954v.
Wang, Hsiu-Wen, Dellostritto, Mark J, Kumar, Nitin, Kolesnikov, Alexander I, Kent, Paul R, Kubicki, James D., Wesolowski, David J, & Sofo, Jorge O. Vibrational Density of States of Strongly H-Bonded Interfacial Water: Insights from Inelastic Neutron Scattering and Theory. United States. doi:10.1021/jp500954v.
Wang, Hsiu-Wen, Dellostritto, Mark J, Kumar, Nitin, Kolesnikov, Alexander I, Kent, Paul R, Kubicki, James D., Wesolowski, David J, and Sofo, Jorge O. Wed . "Vibrational Density of States of Strongly H-Bonded Interfacial Water: Insights from Inelastic Neutron Scattering and Theory". United States. doi:10.1021/jp500954v.
@article{osti_1156714,
title = {Vibrational Density of States of Strongly H-Bonded Interfacial Water: Insights from Inelastic Neutron Scattering and Theory},
author = {Wang, Hsiu-Wen and Dellostritto, Mark J and Kumar, Nitin and Kolesnikov, Alexander I and Kent, Paul R and Kubicki, James D. and Wesolowski, David J and Sofo, Jorge O.},
abstractNote = {The vibrational dynamics of water and OH sorbed on SnO2 nanoparticles were probed with inelastic neutron scattering and analyzed with the assistance of ab-initio molecular dynamics. The combined analysis points to the existence of very strong hydrogen bonds at the surface with a formation enthalpy twice the average value for liquid water. This unusually large interaction results in (i) decoupling of the hydrated surface from the water system due to an epitaxially-induced screening layer, resulting in an apparent ice-like INS signal at multilayer coverage, (ii) splitting of OH wagging modes that can be used as an experimental indication of the strength of the surface hydrogen bonds, and (iii) high proton exchange rates and high degree of water dissociation at the interface. Our analysis provides general guidance into the tuning of surface hydrophobicity at the molecular level.},
doi = {10.1021/jp500954v},
journal = {Science},
number = 20,
volume = 118,
place = {United States},
year = {Wed Jan 01 00:00:00 EST 2014},
month = {Wed Jan 01 00:00:00 EST 2014}
}