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Characterizing Substrate-Surface Interactions on Alumina-Supported Metal Catalysts by Dynamic Nuclear Polarization Enhanced Double-Resonance NMR Spectroscopy

TitleCharacterizing Substrate-Surface Interactions on Alumina-Supported Metal Catalysts by Dynamic Nuclear Polarization Enhanced Double-Resonance NMR Spectroscopy
Publication TypeJournal Article
Year of Publication2017
AuthorsPerras, FA, Padmos, JD, Johnson, RL, Wang, LL, Schwartz, TJ, Kobayashi, T, Horton, JH, Dumesic, JA, Shanks, BH, Johnson, DD, Pruski, M
JournalJournal of the American Chemical Society
Volume139
Pagination2702-2709
Date Published02
Type of ArticleArticle
ISBN Number0002-7863
Accession NumberWOS:000394829200027
Keywordsau, c-13 nmr, chemical-shifts, chemistry, dft calculations, distance measurement, nanoparticles, quadrupolar nuclei, ray-absorption spectroscopy, solid-state nmr, total-energy calculations, wave basis-set
Abstract

The characterization of nanometer-scale interactions between carbon-containing substrates and alumina surfaces is of paramount importance to industrial and academic catalysis applications, but it is also very challenging. Here, we demonstrate that dynamic nuclear polarization surface-enhanced NMR spectroscopy (DNP SENS) allows the unambiguous description of the coordination geometries and conformations of the substrates at the alumina surface through high-resolution measurements of C-13-(27)A1 distances. We apply this new technique to elucidate the molecular-level geometry of C-13 enriched methionine and natural abundance poly(vinyl alcohol) adsorbed on gamma-Al2O3-supported Pd catalysts, and we support these results with element specific X-ray absorption near-edge measurements. This work clearly demonstrates a surprising bimodal coordination of methionine at the Pd-Al2O3 interface.

DOI10.1021/jacs.6b11408
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3D Catalysis

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LDRD

Alternate JournalJ. Am. Chem. Soc.