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Title: Characterizing substrate–surface interactions on alumina-supported metal catalysts by dynamic nuclear polarization-enhanced double-resonance NMR spectroscopy [Characterizing substrate-surface interactions on alumina supported metal catalysts by DNP-enhanced double-resonance NMR spectroscopy]

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 13C– 27Al distances. We apply this new technique to elucidate the molecular-level geometry of 13C-enriched methionine and natural abundance poly(vinyl alcohol) adsorbed on γ-Al 2O 3-supported Pd catalysts, and we support these results with element-specific X-ray absorption near-edge measurements. Furthermore, this work clearly demonstrates a surprising bimodal coordination of methionine at the Pd–Al 2O 3 interface.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ; ORCiD logo [4] ;  [1] ;  [2] ; ORCiD logo [5] ;  [3] ;  [6] ; ORCiD logo [6]
  1. Ames Lab., Ames, IA (United States)
  2. Queen's Univ. Kingston, ON (Canada)
  3. Iowa State Univ., Ames, IA (United States)
  4. Univ. of Wisconsin, Madison, WI (United States); Univ. of Maine, Orono, ME (United States)
  5. Univ. of Wisconsin, Madison, WI (United States)
  6. Ames Lab. and Iowa State Univ., Ames, IA (United States)
Publication Date:
Report Number(s):
IS-J-9224
Journal ID: ISSN 0002-7863
Grant/Contract Number:
DGE-1256259; EEC-0813570
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 7; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1347397