Characterization of the state of two-dimensionally condensed water on hydroxylated chromium(III) oxide surface through ft-ir, quasielastic neutron scattering, and dielectric relaxation measurements

Yasushige Kuroda, Shigeharu Kittaka, Shuichi Takahara, Toshio Yamaguchi, Marie Claire Bellissent-Funel

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Abstract

The dynamic properties of water molecules adsorbed on the hydroxylated chromium(III) oxide surface, whose two-dimensional critical temperature was 303 K, were investigated at around the two-dimensional critical temperature by FT-IR, quasielastic neutron scattering, and dielectric relaxation techniques. The CraOa sample covered with monolayer water gives an IR band having a broad nature at ∼3400 cm-1, due to the mutual hydrogen bonding among the adsorbed water molecules. The quasielastic neutron scattering data have revealed that the motion of the adsorbed water molecules changes across the two-dimensional critical temperature, ranging from the motion of the supercritical fluid to that of a solidified phase with decreasing temperature. The dielectric spectra observed at 298 K and at the coverage of 1.1 monolayers have been interpreted in terms of the presence of two relaxations due to the interfacial and orientational polarizations. The characteristic frequency of the relaxation for the latter polarization was estimated to be ca. 300 Hz. It is concluded from these findings that the two-dimensionally condensed waters adopt the mutually hydrogen-bonded solid state having a commensurate structure with the hydroxylated (001) Cr2O3 surface below the two-dimensional critical temperature of this system. In addition, the interfacial polarization was explained in terms of a hopping model of protons of the adsorbed molecules. The behavior of conductivity arising from this proton hopping also indicates the morphology of the two-dimensionally condensed water below the monolayer coverage: the small clusters of water are formed on the Cr2Q3 surface.

Original languageEnglish
Pages (from-to)11064-11073
Number of pages10
JournalJournal of Physical Chemistry B
Volume103
Issue number50
Publication statusPublished - Dec 16 1999

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Dielectric relaxation
Chromium
Neutron scattering
Oxides
chromium
neutron scattering
oxides
Water
critical temperature
water
Monolayers
Molecules
Polarization
Protons
molecules
polarization
Temperature
Supercritical fluids
protons
supercritical fluids

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Characterization of the state of two-dimensionally condensed water on hydroxylated chromium(III) oxide surface through ft-ir, quasielastic neutron scattering, and dielectric relaxation measurements. / Kuroda, Yasushige; Kittaka, Shigeharu; Takahara, Shuichi; Yamaguchi, Toshio; Bellissent-Funel, Marie Claire.

In: Journal of Physical Chemistry B, Vol. 103, No. 50, 16.12.1999, p. 11064-11073.

Research output: Contribution to journalArticle

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AB - The dynamic properties of water molecules adsorbed on the hydroxylated chromium(III) oxide surface, whose two-dimensional critical temperature was 303 K, were investigated at around the two-dimensional critical temperature by FT-IR, quasielastic neutron scattering, and dielectric relaxation techniques. The CraOa sample covered with monolayer water gives an IR band having a broad nature at ∼3400 cm-1, due to the mutual hydrogen bonding among the adsorbed water molecules. The quasielastic neutron scattering data have revealed that the motion of the adsorbed water molecules changes across the two-dimensional critical temperature, ranging from the motion of the supercritical fluid to that of a solidified phase with decreasing temperature. The dielectric spectra observed at 298 K and at the coverage of 1.1 monolayers have been interpreted in terms of the presence of two relaxations due to the interfacial and orientational polarizations. The characteristic frequency of the relaxation for the latter polarization was estimated to be ca. 300 Hz. It is concluded from these findings that the two-dimensionally condensed waters adopt the mutually hydrogen-bonded solid state having a commensurate structure with the hydroxylated (001) Cr2O3 surface below the two-dimensional critical temperature of this system. In addition, the interfacial polarization was explained in terms of a hopping model of protons of the adsorbed molecules. The behavior of conductivity arising from this proton hopping also indicates the morphology of the two-dimensionally condensed water below the monolayer coverage: the small clusters of water are formed on the Cr2Q3 surface.

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