DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Direct 17O dynamic nuclear polarization of single-site heterogeneous catalysts

Journal Article · · ChemComm
DOI: https://doi.org/10.1039/C8CC00293B · OSTI ID:1427737

In this work, we utilize direct 17O DNP for the characterization of non-protonated oxygens in heterogeneous catalysts. The optimal sample preparation and population transfer approach for 17O direct DNP experiments performed on silica surfaces is determined and applied to the characterization of Zr- and Y-based mesoporous silica-supported single-site catalysts.

Research Organization:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-07CH11358
OSTI ID:
1427737
Report Number(s):
IS-J--593
Journal Information:
ChemComm, Journal Name: ChemComm Journal Issue: 28 Vol. 54; ISSN 1359-7345
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (55)

Beyond the Silica Surface by Direct Silicon-29 Dynamic Nuclear Polarization journal July 2011
Improved Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy through Controlled Incorporation of Deuterated Functional Groups journal January 2013
Highly Efficient, Water-Soluble Polarizing Agents for Dynamic Nuclear Polarization at High Frequency journal August 2013
Highly Dispersed SiO x /Al 2 O 3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites journal September 2015
Atomistic Description of Reaction Intermediates for Supported Metathesis Catalysts Enabled by DNP SENS journal March 2016
Natural Abundance 17 O DNP NMR Provides Precise O−H Distances and Insights into the Brønsted Acidity of Heterogeneous Catalysts journal June 2017
Beyond the Silica Surface by Direct Silicon-29 Dynamic Nuclear Polarization journal July 2011
Improved Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy through Controlled Incorporation of Deuterated Functional Groups journal January 2013
Highly Efficient, Water-Soluble Polarizing Agents for Dynamic Nuclear Polarization at High Frequency journal August 2013
Atomistic Description of Reaction Intermediates for Supported Metathesis Catalysts Enabled by DNP SENS journal March 2016
Natural Abundance 17 O DNP NMR Provides Precise O−H Distances and Insights into the Brønsted Acidity of Heterogeneous Catalysts journal June 2017
A Well-Defined Pd Hybrid Material for the Z -Selective Semihydrogenation of Alkynes Characterized at the Molecular Level by DNP SENS journal August 2013
Sensitivity enhancement of NMR spectra of half-integer quadrupolar nuclei in the solid state via population transfer journal January 2005
Advantages of double frequency sweeps in static, MAS and MQMAS NMR of spin I=3/2 nuclei journal February 1999
Optimal sample formulations for DNP SENS: The importance of radical-surface interactions journal January 2018
Signal enhancement of NMR spectra of half-integer quadrupolar nuclei in solids using hyperbolic secant pulses journal April 2004
Symmetry-based recoupling of 17O–1H spin pairs in magic-angle spinning NMR journal March 2006
Fast passage dynamic nuclear polarization on rotating solids journal November 2012
Heteronuclear polarization transfer by symmetry-based recoupling sequences in solid-state NMR journal September 2004
Signal enhancement in solid-state NMR of quadrupolar nuclei journal April 2013
Improved strategies for DNP-enhanced 2D 1H-X heteronuclear correlation spectroscopy of surfaces journal October 2017
Probing Surface Hydrogen Bonding and Dynamics by Natural Abundance, Multidimensional, 17 O DNP-NMR Spectroscopy journal May 2016
Measuring Long-Range 13 C– 13 C Correlations on a Surface under Natural Abundance Using Dynamic Nuclear Polarization-Enhanced Solid-State Nuclear Magnetic Resonance journal October 2017
DNP-Enhanced Ultrawideline Solid-State NMR Spectroscopy: Studies of Platinum in Metal–Organic Frameworks journal June 2016
Mesoporous Silica-Supported Amidozirconium-Catalyzed Carbonyl Hydroboration journal November 2015
Dynamic Nuclear Polarization Solid-State NMR in Heterogeneous Catalysis Research journal October 2015
Dynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy journal March 2013
On the Track to Silica-Supported Tungsten Oxo Metathesis Catalysts: Input from 17 O Solid-State NMR journal August 2013
Surface Enhanced NMR Spectroscopy by Dynamic Nuclear Polarization journal November 2010
Fast Characterization of Functionalized Silica Materials by Silicon-29 Surface-Enhanced NMR Spectroscopy Using Dynamic Nuclear Polarization journal February 2011
A Slowly Relaxing Rigid Biradical for Efficient Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy: Expeditious Characterization of Functional Group Manipulation in Hybrid Materials journal January 2012
17 O NMR Gives Unprecedented Insights into the Structure of Supported Catalysts and Their Interaction with the Silica Carrier journal May 2012
Dynamic Nuclear Polarization Enhanced Natural Abundance 17 O Spectroscopy journal February 2013
Large Molecular Weight Nitroxide Biradicals Providing Efficient Dynamic Nuclear Polarization at Temperatures up to 200 K journal August 2013
WMe 6 Tamed by Silica: ≡Si–O–WMe 5 as an Efficient, Well-Defined Species for Alkane Metathesis, Leading to the Observation of a Supported W–Methyl/Methylidyne Species journal January 2014
Untangling the Condensation Network of Organosiloxanes on Nanoparticles using 2D 29 Si– 29 Si Solid-State NMR Enhanced by Dynamic Nuclear Polarization journal September 2014
Natural Abundance 17 O DNP Two-Dimensional and Surface-Enhanced NMR Spectroscopy journal June 2015
Structure of Colloidal Quantum Dots from Dynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy journal October 2015
Three-Dimensional Structure Determination of Surface Sites journal January 2017
Characterizing Substrate–Surface Interactions on Alumina-Supported Metal Catalysts by Dynamic Nuclear Polarization-Enhanced Double-Resonance NMR Spectroscopy journal February 2017
Dynamic Nuclear Polarization of 17 O: Direct Polarization journal November 2013
Factors Controlling the 17 O NMR Chemical Shift in Ionic Mixed Metal Oxides journal January 1996
Dynamic Nuclear Polarization of Oxygen-17 journal July 2012
Unraveling the Core–Shell Structure of Ligand-Capped Sn/SnO x Nanoparticles by Surface-Enhanced Nuclear Magnetic Resonance, Mössbauer, and X-ray Absorption Spectroscopies journal February 2014
A tris(alkyl)yttrium compound containing six β-agostic Si–H interactions journal January 2009
Identifying low-coverage surface species on supported noble metal nanoparticle catalysts by DNP-NMR journal January 2016
Oxygen-17 dynamic nuclear polarisation enhanced solid-state NMR spectroscopy at 18.8 T journal January 2017
Surface-selective direct 17 O DNP NMR of CeO 2 nanoparticles journal January 2017
17 O MAS NMR studies of oxo-based olefin metathesis catalysts: a critical assessment of signal enhancement methods journal January 2016
Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles: a study by conventional and DNP-enhanced 29 Si solid-state NMR journal January 2017
Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy journal January 2017
Analysis of sensitivity enhancement by dynamic nuclear polarization in solid-state NMR: a case study of functionalized mesoporous materials journal January 2013
Mechanism of dynamic nuclear polarization in high magnetic fields journal March 2001
Theory for cross effect dynamic nuclear polarization under magic-angle spinning in solid state nuclear magnetic resonance: The importance of level crossings journal August 2012
High sensitivity and resolution in 43 Ca solid-state NMR experiments journal August 2015

Cited By (3)

Shedding light on the atomic-scale structure of amorphous silica–alumina and its Brønsted acid sites journal January 2019
Optimizing nitroxide biradicals for cross-effect MAS-DNP: the role of g -tensors’ distance journal January 2020
Shedding light on the atomic-scale structure of amorphous silica-alumina and its Brønsted acid sites text January 2019