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]

Perras, Frederic A.; Padmos, J. Daniel; Johnson, Robert L.; Wang, Lin -Lin; Schwartz, Thomas J.; Kobayashi, Takeshi; Horton, J. Hugh; Dumesic, James A.; Shanks, Brent H.; Johnson, Duane D.; Pruski, Marek

doi:10.1021/jacs.6b11408

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]

Journal Article · Mon Jan 23 00:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b11408· OSTI ID:1347397

Perras, Frederic A. ^[1]; Padmos, J. Daniel ^[2]; Johnson, Robert L. ^[3]; Wang, Lin -Lin ^[1];

^[4]; Kobayashi, Takeshi ^[1]; Horton, J. Hugh ^[2];

^[5]; Shanks, Brent H. ^[3]; Johnson, Duane D. ^[6];

^[6]

Ames Lab., Ames, IA (United States)
Queen's Univ. Kingston, ON (Canada)
Iowa State Univ., Ames, IA (United States)
Univ. of Wisconsin, Madison, WI (United States); Univ. of Maine, Orono, ME (United States)
Univ. of Wisconsin, Madison, WI (United States)
Ames Lab. and Iowa State Univ., Ames, IA (United States)

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-Al₂O₃-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–Al₂O₃ interface.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: DGE-1256259; EEC-0813570

OSTI ID:: 1347397

Report Number(s):: IS-J-9224

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 7; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 52 works

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