Interactions
of Oxide Surfaces with Water Revealed
with Solid-State NMR Spectroscopy
Posted on 2020-06-11 - 13:36
Hydrous
materials are ubiquitous in the natural environment and
efforts have previously been made to investigate the structures and
dynamics of hydrated surfaces for their key roles in various chemical
and physical applications, with the help of theoretical modeling and
microscopy techniques. However, an overall atomic-scale understanding
of the water–solid interface, including the effect of water
on surface ions, is still lacking. Herein, we employ ceria nanorods
with different amounts of water as an example and demonstrate a new
approach to explore the water–surface interactions by using
solid-state NMR in combination with density functional theory. NMR
shifts and relaxation time analysis provide detailed information on
the local structure of oxygen ions and the nature of water motion
on the surface: the amount of molecularly adsorbed water decreases
rapidly with increasing temperature (from room temperature to 150
°C), whereas hydroxyl groups are stable up to 150 °C, and
dynamic water molecules are found to instantaneously coordinate to
the surface oxygen ions. The applicability of dynamic nuclear polarization
for selective detection of surface oxygen species is also compared
to conventional NMR with surface selective isotopic-labeling: the
optimal method depends on the feasibility of enrichment and the concentration
of protons in the sample. These results provide new insight into the
interfacial structure of hydrated oxide nanostructures, which is important
to improve performance for various applications.
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Chen, Junchao; Hope, Michael A.; Lin, Zhiye; Wang, Meng; Liu, Tao; Halat, David M.; et al. (2020). Interactions
of Oxide Surfaces with Water Revealed
with Solid-State NMR Spectroscopy. ACS Publications. Collection. https://doi.org/10.1021/jacs.0c03760
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AUTHORS (16)
JC
Junchao Chen
MH
Michael A. Hope
ZL
Zhiye Lin
MW
Meng Wang
TL
Tao Liu
DH
David M. Halat
YW
Yujie Wen
TC
Teng Chen
XK
Xiaokang Ke
PM
Pieter C. M. M. Magusin
WD
Weiping Ding
XX
Xifeng Xia
XW
Xin-Ping Wu
XG
Xue-Qing Gong
CG
Clare P. Grey
LP
Luming Peng
KEYWORDS
oxygen ionswater moleculesceria nanorodsNMR shiftssurface ionsmicroscopy techniquesrelaxation time analysisWater RevealedOxide Surfacesoxide nanostructureshydroxyl groupswater motionwater decreasesatomic-scale understandingSolid-State NMR Spectroscopy Hydrous materialssurface oxygen ionssurface oxygen speciesroom temperature