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Probing Surface Hydrogen Bonding and Dynamics by Natural Abundance, Multidimensional, O-17 DNP-NMR Spectroscopy

TitleProbing Surface Hydrogen Bonding and Dynamics by Natural Abundance, Multidimensional, O-17 DNP-NMR Spectroscopy
Publication TypeJournal Article
Year of Publication2016
AuthorsPerras, FA, Chaudhary, U, Slowing, II, Pruski, M
JournalJournal of Physical Chemistry C
Volume120
Pagination11535-11544
Date Published06
Type of ArticleArticle
ISBN Number1932-7447
Accession NumberWOS:000377239000023
Keywordschemical-shift, chemistry, gel surface, Materials Science, Mesoporous silica nanoparticles, nuclear-magnetic-resonance, polarization transfer, pulse sequence, quadrupolar nuclei, rotating solids, sn-beta zeolite, solid-state nmr, Technology - Other Topics
Abstract

Dynamic nuclear polarization (DNP)-enhanced solid-state nuclear magnetic resonance (SSNMR) spectroscopy is increasingly being used as a tool for the atomic-level characterization of surface sites. DNP surface-enhanced SSNMR spectroscopy of materials has, however, been limited to studying relatively receptive nuclei, and the particularly rare O-17 nuclide, which is of great interest for materials science, has not been utilized. We demonstrate that advanced O-17 SSNMR experiments can be performed on surface species at natural isotopic abundance using DNP. We use O-17 DNP surface enhanced 2D SSNMR to measure O-17{H-1} HETCOR spectra as well as dipolar oscillations on a series of thermally treated mesoporous silica nanoparticle samples having different pore diameters. These experiments allow for a nonintrusive unambiguous characterization of hydrogen bonding and dynamics at the surface of the material; no other single experiment can give such details about the interactions at the surface. Our data show that, upon drying, strongly hydrogen-bonded surface silanols, whose motions are greatly restricted by the interaction when compared to lone silanols, are selectively dehydroxylated.

DOI10.1021/acs.jpcc.6b02579
Custom 1

3D Catalysis

Custom 2

LDRD

Alternate JournalJ. Phys. Chem. C