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]
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 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.
- Authors:
-
[4];
[5];
[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)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1347397
- Report Number(s):
- IS-J-9224
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- DGE-1256259; EEC-0813570
- Resource 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)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
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., and Pruski, Marek. 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]. United States: N. p., 2017.
Web. doi:10.1021/jacs.6b11408.
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. 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]. United States. https://doi.org/10.1021/jacs.6b11408
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., and Pruski, Marek. Mon .
"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]". United States. https://doi.org/10.1021/jacs.6b11408. https://www.osti.gov/servlets/purl/1347397.
@article{osti_1347397,
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]},
author = {Perras, Frederic A. and Padmos, J. Daniel and Johnson, Robert L. and Wang, Lin -Lin and Schwartz, Thomas J. and Kobayashi, Takeshi and Horton, J. Hugh and Dumesic, James A. and Shanks, Brent H. and Johnson, Duane D. and Pruski, Marek},
abstractNote = {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.},
doi = {10.1021/jacs.6b11408},
journal = {Journal of the American Chemical Society},
number = 7,
volume = 139,
place = {United States},
year = {Mon Jan 23 00:00:00 EST 2017},
month = {Mon Jan 23 00:00:00 EST 2017}
}
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Works referenced in this record:
Surface Enhanced NMR Spectroscopy by Dynamic Nuclear Polarization
journal, November 2010
- Lesage, Anne; Lelli, Moreno; Gajan, David
- Journal of the American Chemical Society, Vol. 132, Issue 44
Dynamic Nuclear Polarization Solid-State NMR in Heterogeneous Catalysis Research
journal, October 2015
- Kobayashi, Takeshi; Perras, Frédéric A.; Slowing, Igor I.
- ACS Catalysis, Vol. 5, Issue 12
Fast Characterization of Functionalized Silica Materials by Silicon-29 Surface-Enhanced NMR Spectroscopy Using Dynamic Nuclear Polarization
journal, February 2011
- Lelli, Moreno; Gajan, David; Lesage, Anne
- Journal of the American Chemical Society, Vol. 133, Issue 7
Evidence for Metal–Surface Interactions and Their Role in Stabilizing Well-Defined Immobilized Ru–NHC Alkene Metathesis Catalysts
journal, February 2013
- Samantaray, Manoja K.; Alauzun, Johan; Gajan, David
- Journal of the American Chemical Society, Vol. 135, Issue 8
A Well-Defined Pd Hybrid Material for the Z -Selective Semihydrogenation of Alkynes Characterized at the Molecular Level by DNP SENS
journal, August 2013
- Conley, Matthew P.; Drost, Ruben M.; Baffert, Mathieu
- Chemistry - A European Journal, Vol. 19, Issue 37
Influences of Dilute Organic Adsorbates on the Hydration of Low-Surface-Area Silicates
journal, June 2015
- Sangodkar, Rahul P.; Smith, Benjamin J.; Gajan, David
- Journal of the American Chemical Society, Vol. 137, Issue 25
γ-Alumina as a Support for Catalysts: A Review of Fundamental Aspects
journal, September 2005
- Trueba, Monica; Trasatti, Stefano P.
- European Journal of Inorganic Chemistry, Vol. 2005, Issue 17
A Study of Commercial Nanoparticulate γ-Al 2 O 3 Catalyst Supports
journal, April 2013
- Rozita, Yahaya; Brydson, Rik; Comyn, Tim P.
- ChemCatChem, Vol. 5, Issue 9
Dynamic nuclear polarization of quadrupolar nuclei using cross polarization from protons: surface-enhanced aluminium-27 NMR
journal, January 2012
- Vitzthum, Veronika; Miéville, Pascal; Carnevale, Diego
- Chemical Communications, Vol. 48, Issue 14
Enhanced Solid-State NMR Correlation Spectroscopy of Quadrupolar Nuclei Using Dynamic Nuclear Polarization
journal, October 2012
- Lee, Daniel; Takahashi, Hiroki; Thankamony, Aany S. L.
- Journal of the American Chemical Society, Vol. 134, Issue 45
Primostrato Solid-State NMR Enhanced by Dynamic Nuclear Polarization: Pentacoordinated Al 3+ Ions Are Only Located at the Surface of Hydrated γ-Alumina
journal, October 2014
- Lee, Daniel; Duong, Nghia Tuan; Lafon, Olivier
- The Journal of Physical Chemistry C, Vol. 118, Issue 43
PRESTO polarization transfer to quadrupolar nuclei: implications for dynamic nuclear polarization
journal, January 2015
- Perras, Frédéric A.; Kobayashi, Takeshi; Pruski, Marek
- Physical Chemistry Chemical Physics, Vol. 17, Issue 35
Identifying low-coverage surface species on supported noble metal nanoparticle catalysts by DNP-NMR
journal, January 2016
- Johnson, Robert L.; Perras, Frédéric A.; Kobayashi, Takeshi
- Chemical Communications, Vol. 52, Issue 9
Methionine bound to Pd/γ-Al2O3 catalysts studied by solid-state 13C NMR
journal, November 2015
- Johnson, Robert L.; Schwartz, Thomas J.; Dumesic, James A.
- Solid State Nuclear Magnetic Resonance, Vol. 72
Engineering Catalyst Microenvironments for Metal-Catalyzed Hydrogenation of Biologically Derived Platform Chemicals
journal, September 2014
- Schwartz, Thomas J.; Johnson, Robert L.; Cardenas, Javier
- Angewandte Chemie International Edition, Vol. 53, Issue 47
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005
- Ravel, B.; Newville, M.
- Journal of Synchrotron Radiation, Vol. 12, Issue 4
Large Molecular Weight Nitroxide Biradicals Providing Efficient Dynamic Nuclear Polarization at Temperatures up to 200 K
journal, August 2013
- Zagdoun, Alexandre; Casano, Gilles; Ouari, Olivier
- Journal of the American Chemical Society, Vol. 135, Issue 34
Heteronuclear polarization transfer by symmetry-based recoupling sequences in solid-state NMR
journal, September 2004
- Zhao, Xin; Hoffbauer, Wilfried; Schmedt auf der Günne, Jörn
- Solid State Nuclear Magnetic Resonance, Vol. 26, Issue 2
Frequency-switched pulse sequences: Homonuclear decoupling and dilute spin NMR in solids
journal, March 1989
- Bielecki, A.; Kolbert, A. C.; Levitt, M. H.
- Chemical Physics Letters, Vol. 155, Issue 4-5
Recoupling of heteronuclear dipolar interactions in solid state magic-angle spinning NMR by simultaneous frequency and amplitude modulation
journal, July 1997
- Fu, Riqiang; Smith, Scott A.; Bodenhausen, Geoffrey
- Chemical Physics Letters, Vol. 272, Issue 5-6
Observation of proximities between spin-1/2 and quadrupolar nuclei: Which heteronuclear dipolar recoupling method is preferable?
journal, October 2012
- Lu, X.; Lafon, O.; Trébosc, J.
- The Journal of Chemical Physics, Vol. 137, Issue 14
Advantages of double frequency sweeps in static, MAS and MQMAS NMR of spin I=3/2 nuclei
journal, February 1999
- Kentgens, A. P. M.; Verhagen, R.
- Chemical Physics Letters, Vol. 300, Issue 3-4
Signal enhancement in solid-state NMR of quadrupolar nuclei
journal, April 2013
- Perras, Frédéric A.; Viger-Gravel, Jasmine; Burgess, Kevin M. N.
- Solid State Nuclear Magnetic Resonance, Vol. 51-52
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
All-electron magnetic response with pseudopotentials: NMR chemical shifts
journal, May 2001
- Pickard, Chris J.; Mauri, Francesco
- Physical Review B, Vol. 63, Issue 24
Calculation of NMR chemical shifts for extended systems using ultrasoft pseudopotentials
journal, July 2007
- Yates, Jonathan R.; Pickard, Chris J.; Mauri, Francesco
- Physical Review B, Vol. 76, Issue 2
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Conformational analysis ofDL-,L- andD-methionine by solid-state13C NMR spectroscopy
journal, February 1986
- Díaz, Luis E.; Morin, Frederick; Mayne, Charles L.
- Magnetic Resonance in Chemistry, Vol. 24, Issue 2
13 C NMR and Infrared Evidence of a Dioctyl−Disulfide Structure on Octanethiol-Protected Palladium Nanoparticle Surfaces
journal, July 2004
- Zelakiewicz, Brian S.; Lica, Georgeta C.; Deacon, Morgan L.
- Journal of the American Chemical Society, Vol. 126, Issue 32
13C NMR Spectroscopy of 13C1-Labeled Octanethiol-Protected Au Nanoparticles: Shifts, Relaxations, and Particle-Size Effect
journal, December 2002
- Zelakiewicz, Brian S.; de Dios, Angel C.; Tong, YuYe
- Journal of the American Chemical Society, Vol. 125, Issue 1, p. 18-19
How Do Spin-Orbit-Induced Heavy-Atom Effects on NMR Chemical Shifts Function? Validation of a Simple Analogy to Spin-Spin Coupling by Density Functional Theory (DFT) Calculations on Some Iodo Compounds
journal, January 1998
- Kaupp, Martin; Malkina, Olga L.; Malkin, Vladimir G.
- Chemistry - A European Journal, Vol. 4, Issue 1
Relativistic effects and the halogen dependencies in the13C chemical shifts of CH4?nIn, CH4?nBrn, CCl4?nIn, and CBr4?nIn (n=0-4)
journal, January 2001
- Fukawa, Shuhei; Hada, Masahiko; Fukuda, Ryoichi
- Journal of Computational Chemistry, Vol. 22, Issue 5
Ligand K-edge X-ray absorption spectroscopy: covalency of ligand–metal bonds
journal, January 2005
- Solomon, Edward I.; Hedman, Britt; Hodgson, Keith O.
- Coordination Chemistry Reviews, Vol. 249, Issue 1-2
Sulfur: not a “silent” element any more
journal, January 2006
- Jalilehvand, Farideh
- Chem. Soc. Rev., Vol. 35, Issue 12
Surface Structure of Organosulfur Stabilized Silver Nanoparticles Studied with X-ray Absorption Spectroscopy
journal, October 2012
- Padmos, J. Daniel; Zhang, Peng
- The Journal of Physical Chemistry C, Vol. 116, Issue 43
Adsorption of dimethyl sulfide and methanethiolate on Ag and Au surfaces: Surface-enhanced Raman scattering and density functional theory calculation study
journal, November 2006
- Lim, Jong Kuk; Kim, In-Hyun; Kim, Ki-Hyun
- Chemical Physics, Vol. 330, Issue 1-2
Peptides containing methionine and carboxymethylcysteine
book, January 1967
- Harris, J. I.
- Methods in Enzymology
Tuning the electronic behavior of Au nanoparticles with capping molecules
journal, July 2002
- Zhang, P.; Sham, T. K.
- Applied Physics Letters, Vol. 81, Issue 4
X-Ray Studies of the Structure and Electronic Behavior of Alkanethiolate-Capped Gold Nanoparticles: The Interplay of Size and Surface Effects
journal, June 2003
- Zhang, Peng; Sham, T. K.
- Physical Review Letters, Vol. 90, Issue 24
Core-shell model for the magnetic properties of Pd nanoparticles
journal, February 2012
- Seehra, M. S.; Rall, J. D.; Liu, J. C.
- Materials Letters, Vol. 68
Solid-State 1H MAS NMR Characterization of γ-Alumina and Modified γ-Aluminas
journal, July 1994
- Decanio, E. C.; Edwards, J. C.; Bruno, J. W.
- Journal of Catalysis, Vol. 148, Issue 1
Measuring multiple carbon–nitrogen distances in natural abundant solids using R-RESPDOR NMR
journal, January 2006
- Gan, Zhehong
- Chem. Commun., Issue 45
Efficient rotational echo double resonance recoupling of a spin-1/2 and a quadrupolar spin at high spinning rates and weak irradiation fields
journal, September 2010
- Nimerovsky, Evgeny; Goldbourt, Amir
- Journal of Magnetic Resonance, Vol. 206, Issue 1
Measurement of Aluminum-Carbon Distances Using S-RESPDOR NMR Experiments
journal, September 2012
- Pourpoint, Frédérique; Trébosc, Julien; Gauvin, Régis M.
- ChemPhysChem, Vol. 13, Issue 16
Probing 27 Al– 13 C proximities in metal–organic frameworks using dynamic nuclear polarization enhanced NMR spectroscopy
journal, January 2014
- Pourpoint, Frédérique; Thankamony, Aany Sofia Lilly; Volkringer, Christophe
- Chem. Commun., Vol. 50, Issue 8
Direct Detection of Supramolecular Reaction Centers in the Methanol-to-Olefins Conversion over Zeolite H-ZSM-5 by 13 C- 27 Al Solid-State NMR Spectroscopy
journal, January 2016
- Wang, Chao; Wang, Qiang; Xu, Jun
- Angewandte Chemie International Edition, Vol. 55, Issue 7
Insight into the formation of the tert-butyl cation confined inside H-ZSM-5 zeolite from NMR spectroscopy and DFT calculations
journal, January 2016
- Huang, Mengdi; Wang, Qiang; Yi, Xianfeng
- Chemical Communications, Vol. 52, Issue 70
Distance measurement between a spin-1/2 and a half-integer quadrupolar nuclei by solid-state NMR using exact analytical expressions
journal, October 2010
- Chen, Lei; Lu, Xingyu; Wang, Qiang
- Journal of Magnetic Resonance, Vol. 206, Issue 2
Measurement of hetero-nuclear distances using a symmetry-based pulse sequence in solid-state NMR
journal, January 2010
- Chen, Lei; Wang, Qiang; Hu, Bingwen
- Physical Chemistry Chemical Physics, Vol. 12, Issue 32
REDOR Dephasing by Multiple Spins in the Presence of Molecular Motion
journal, August 1997
- Goetz, Jon M.; Schaefer, Jacob
- Journal of Magnetic Resonance, Vol. 127, Issue 2
Detailed analysis of the S-RESPDOR solid-state NMR method for inter-nuclear distance measurement between spin-1/2 and quadrupolar nuclei
journal, February 2012
- Lu, Xingyu; Lafon, Olivier; Trébosc, Julien
- Journal of Magnetic Resonance, Vol. 215
SIMPSON: A General Simulation Program for Solid-State NMR Spectroscopy
journal, December 2000
- Bak, Mads; Rasmussen, Jimmy T.; Nielsen, Niels Chr
- Journal of Magnetic Resonance, Vol. 147, Issue 2
γ-Alumina: a single-crystal X-ray diffraction study
journal, August 2006
- Smrčok, Ľubomír; Langer, Vratislav; Křesťan, Jan
- Acta Crystallographica Section C Crystal Structure Communications, Vol. 62, Issue 9
Synthesis and Stabilization of Supported Metal Catalysts by Atomic Layer Deposition
journal, March 2013
- Lu, Junling; Elam, Jeffrey W.; Stair, Peter C.
- Accounts of Chemical Research, Vol. 46, Issue 8
Interfacial Effects of CeO 2 -Supported Pd Nanorod in Catalytic CO Oxidation: A Theoretical Study
journal, May 2015
- Liu, Bing; Liu, Jian; Li, Teng
- The Journal of Physical Chemistry C, Vol. 119, Issue 23
Modifying the Surface Properties of Heterogeneous Catalysts Using Polymer-Derived Microenvironments
journal, September 2015
- Schwartz, Thomas J.; Wesley, Thejas S.; Dumesic, James A.
- Topics in Catalysis, Vol. 59, Issue 1
Works referencing / citing this record:
Room temperature CO oxidation catalysed by supported Pt nanoparticles revealed by solid-state NMR and DNP spectroscopy
journal, January 2019
- Klimavicius, Vytautas; Neumann, Sarah; Kunz, Sebastian
- Catalysis Science & Technology, Vol. 9, Issue 14
Characterization techniques for nanoparticles: comparison and complementarity upon studying nanoparticle properties
journal, January 2018
- Mourdikoudis, Stefanos; Pallares, Roger M.; Thanh, Nguyen T. K.
- Nanoscale, Vol. 10, Issue 27
Selective Aerobic Oxidation of Alcohols over Gold‐Palladium Alloy Catalysts Using Air at Atmospheric Pressure in Water
journal, February 2019
- Zhang, Wei; Xiao, Ziqiang; Wang, Jiajun
- ChemCatChem, Vol. 11, Issue 6
Shedding light on the atomic-scale structure of amorphous silica-alumina and its Brønsted acid sites
text, January 2019
- Perras, Frédéric A.; Wang, Zichun; Kobayashi, Takeshi
- ETH Zurich