Double-resonance 17 O NMR experiments reveal unique configurational information for surface organometallic complexes
Abstract
Obtaining three-dimensional (3D) configurational information of surface organometallic complexes is a persistent challenge due to the low spatial sensitivity of most spectroscopic methods. Here we show that employing 17O-enriched supports enables highly informative multidimensional NMR experiments, including radial and vertical distance measurements, that can be used to elucidate site geometry.
- Authors:
-
- Chemical and Biological Sciences Division, Ames National laboratory, Ames, IA 50011, USA, Department of Chemistry, Iowa State University, Ames, IA, 50011, USA
- Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA
- Chemical and Biological Sciences Division, Ames National laboratory, Ames, IA 50011, USA
- Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853, USA
- Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA, Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, USA
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- OSTI Identifier:
- 1970411
- Alternate Identifier(s):
- OSTI ID: 1963732; OSTI ID: 1964141; OSTI ID: 2310921
- Report Number(s):
- IS-J-11,019
Journal ID: ISSN 1359-7345; CHCOFS
- Grant/Contract Number:
- AC-02-06CH11357; AC-02-07CH11358; AC02-06CH11357
- Resource Type:
- Published Article
- Journal Name:
- ChemComm
- Additional Journal Information:
- Journal Name: ChemComm Journal Volume: 59 Journal Issue: 31; Journal ID: ISSN 1359-7345
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Perras, Frédéric A., Arroyave, Alejandra, Southern, Scott A., Lamb, Jessica V., Li, Yuting, LaPointe, Anne, and Delferro, Massimiliano. Double-resonance 17 O NMR experiments reveal unique configurational information for surface organometallic complexes. United Kingdom: N. p., 2023.
Web. doi:10.1039/D3CC00899A.
Perras, Frédéric A., Arroyave, Alejandra, Southern, Scott A., Lamb, Jessica V., Li, Yuting, LaPointe, Anne, & Delferro, Massimiliano. Double-resonance 17 O NMR experiments reveal unique configurational information for surface organometallic complexes. United Kingdom. https://doi.org/10.1039/D3CC00899A
Perras, Frédéric A., Arroyave, Alejandra, Southern, Scott A., Lamb, Jessica V., Li, Yuting, LaPointe, Anne, and Delferro, Massimiliano. Thu .
"Double-resonance 17 O NMR experiments reveal unique configurational information for surface organometallic complexes". United Kingdom. https://doi.org/10.1039/D3CC00899A.
@article{osti_1970411,
title = {Double-resonance 17 O NMR experiments reveal unique configurational information for surface organometallic complexes},
author = {Perras, Frédéric A. and Arroyave, Alejandra and Southern, Scott A. and Lamb, Jessica V. and Li, Yuting and LaPointe, Anne and Delferro, Massimiliano},
abstractNote = {Obtaining three-dimensional (3D) configurational information of surface organometallic complexes is a persistent challenge due to the low spatial sensitivity of most spectroscopic methods. Here we show that employing 17O-enriched supports enables highly informative multidimensional NMR experiments, including radial and vertical distance measurements, that can be used to elucidate site geometry.},
doi = {10.1039/D3CC00899A},
journal = {ChemComm},
number = 31,
volume = 59,
place = {United Kingdom},
year = {Thu Apr 13 00:00:00 EDT 2023},
month = {Thu Apr 13 00:00:00 EDT 2023}
}
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Works referenced in this record:
Molecular and Electronic Structure of Isolated Platinum Sites Enabled by the Expedient Measurement of 195Pt Chemical Shift Anisotropy
journal, July 2022
- Venkatesh, Amrit; Gioffrè, Domenico; Atterberry, Benjamin A.
- Journal of the American Chemical Society, Vol. 144, Issue 30
β-SiH-Containing Tris(silazido) Rare-Earth Complexes as Homogeneous and Grafted Single-Site Catalyst Precursors for Hydroamination
journal, January 2017
- Eedugurala, Naresh; Wang, Zhuoran; Yan, KaKing
- Organometallics, Vol. 36, Issue 6
Multiple Surface Site Three-Dimensional Structure Determination of a Supported Molecular Catalyst
journal, June 2022
- Jabbour, Ribal; Renom-Carrasco, Marc; Chan, Ka Wing
- Journal of the American Chemical Society, Vol. 144, Issue 23
Solid-state 45 Sc NMR studies of Cp* 2 Sc–X and Cp* 2 ScX(THF)
journal, January 2018
- Huynh, Winn; Culver, Damien B.; Tafazolian, Hosein
- Dalton Transactions, Vol. 47, Issue 37
Highly Active and Recyclable Heterogeneous Iridium Pincer Catalysts for Transfer Dehydrogenation of Alkanes
journal, January 2009
- Huang, Zheng; Brookhart, Maurice; Goldman, Alan S.
- Advanced Synthesis & Catalysis, Vol. 351, Issue 1-2
Observing the three-dimensional dynamics of supported metal complexes
journal, January 2021
- Paterson, Alexander L.; Liu, Da-Jiang; Kanbur, Uddhav
- Inorganic Chemistry Frontiers, Vol. 8, Issue 6
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
Local Structures and Heterogeneity of Silica-Supported M(III) Sites Evidenced by EPR, IR, NMR, and Luminescence Spectroscopies
journal, June 2017
- Delley, Murielle F.; Lapadula, Giuseppe; Núñez-Zarur, Francisco
- Journal of the American Chemical Society, Vol. 139, Issue 26
Analysis of large-anisotropy-spin recoupling pulses for distance measurement under magic-angle spinning NMR shows the superiority and robustness of a phase modulated saturation pulse
journal, March 2017
- Nimerovsky, E.; Makrinich, M.; Goldbourt, A.
- The Journal of Chemical Physics, Vol. 146, Issue 12
Silica-Supported Organolanthanum Catalysts for C–O Bond Cleavage in Epoxides
journal, January 2020
- Wang, Zhuoran; Patnaik, Smita; Eedugurala, Naresh
- Journal of the American Chemical Society, Vol. 142, Issue 6
Observation of proximities between spin-1/2 and quadrupolar nuclei in solids: Improved robustness to chemical shielding using adiabatic symmetry-based recoupling
journal, October 2018
- Nagashima, Hiroki; Lilly Thankamony, Aany Sofia; Trébosc, Julien
- Solid State Nuclear Magnetic Resonance, Vol. 94
17 O NMR Gives Unprecedented Insights into the Structure of Supported Catalysts and Their Interaction with the Silica Carrier
journal, May 2012
- Merle, Nicolas; Trébosc, Julien; Baudouin, Anne
- Journal of the American Chemical Society, Vol. 134, Issue 22
17O Solid-State NMR Studies of ZrO2 Nanoparticles
journal, January 2019
- Shen, Li; Wu, Xin-Ping; Wang, Yang
- The Journal of Physical Chemistry C, Vol. 123, Issue 7
Catalytic Cleavage of the C-H and C-C Bonds of Alkanes by Surface Organometallic Chemistry: An EXAFS and IR Characterization of a Zr-H Catalyst
journal, February 1996
- Corker, J.; Lefebvre, F. d. r.; Evans, J.
- Science, Vol. 271, Issue 5251
Realistic Models of Hydroxylated Amorphous Silica Surfaces and MCM-41 Mesoporous Material Simulated by Large-scale Periodic B3LYP Calculations
journal, December 2008
- Ugliengo, P.; Sodupe, M.; Musso, F.
- Advanced Materials, Vol. 20, Issue 23
Supported Lanthanum Borohydride Catalyzes CH Borylation Inside Zeolite Micropores
journal, February 2022
- Li, Yuting; Kanbur, Uddhav; Cui, Jinlei
- Angewandte Chemie, Vol. 134, Issue 15
Speciation and Structures in Pt Surface Sites Stabilized by N-Heterocyclic Carbene Ligands Revealed by Dynamic Nuclear Polarization Enhanced Indirectly Detected 195Pt NMR Spectroscopic Signatures and Fingerprint Analysis
journal, November 2022
- Wang, Zhuoran; Völker, Laura A.; Robinson, Thomas C.
- Journal of the American Chemical Society, Vol. 144, Issue 47
INTERFACES. A program for determining the 3D structures of surfaces sites using NMR data
journal, December 2022
- Cunningham, James; Perras, Frédéric A.
- Journal of Magnetic Resonance Open, Vol. 12-13
Natural Abundance 17 O DNP NMR Provides Precise O−H Distances and Insights into the Brønsted Acidity of Heterogeneous Catalysts
journal, June 2017
- Perras, Frédéric A.; Wang, Zhuoran; Naik, Pranjali
- Angewandte Chemie International Edition, Vol. 56, Issue 31
Phase-modulated LA-REDOR: A robust, accurate and efficient solid-state NMR technique for distance measurements between a spin-1/2 and a quadrupole spin
journal, July 2014
- Nimerovsky, Evgeny; Gupta, Rupal; Yehl, Jenna
- Journal of Magnetic Resonance, Vol. 244
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
Revealing the Configuration and Conformation of Surface Organometallic Catalysts with DNP-Enhanced NMR
journal, June 2021
- Perras, Frédéric A.; Paterson, Alexander L.; Syed, Zoha H.
- The Journal of Physical Chemistry C, Vol. 125, Issue 24
DNP-Enhanced Ultrawideline Solid-State NMR Spectroscopy: Studies of Platinum in Metal–Organic Frameworks
journal, June 2016
- Kobayashi, Takeshi; Perras, Frédéric A.; Goh, Tian Wei
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
Direct 17 O dynamic nuclear polarization of single-site heterogeneous catalysts
journal, January 2018
- Perras, Frédéric A.; Boteju, Kasuni C.; Slowing, Igor I.
- Chemical Communications, Vol. 54, Issue 28
Identification of different oxygen species in oxide nanostructures with 17 O solid-state NMR spectroscopy
journal, February 2015
- Wang, Meng; Wu, Xin-Ping; Zheng, Sujuan
- Science Advances, Vol. 1, Issue 1
Surface Organometallic and Coordination Chemistry toward Single-Site Heterogeneous Catalysts: Strategies, Methods, Structures, and Activities
journal, January 2016
- Copéret, Christophe; Comas-Vives, Aleix; Conley, Matthew P.
- Chemical Reviews, Vol. 116, Issue 2
Measuring multiple carbon–nitrogen distances in natural abundant solids using R-RESPDOR NMR
journal, January 2006
- Gan, Zhehong
- Chem. Commun., Issue 45
Continuous-Flow Alkane Dehydrogenation by Supported Pincer-Ligated Iridium Catalysts at Elevated Temperatures
journal, July 2018
- Sheludko, Boris; Cunningham, Molly T.; Goldman, Alan S.
- ACS Catalysis, Vol. 8, Issue 9
Three-Dimensional Structure Determination of Surface Sites
journal, January 2017
- Berruyer, Pierrick; Lelli, Moreno; Conley, Matthew P.
- Journal of the American Chemical Society, Vol. 139, Issue 2
Catalytic carbon-carbon bond cleavage and carbon-element bond formation give new life for polyolefins as biodegradable surfactants
journal, May 2021
- Kanbur, Uddhav; Zang, Guiyan; Paterson, Alexander L.
- Chem, Vol. 7, Issue 5
Accurate First Principles Prediction of 17 O NMR Parameters in SiO 2 : Assignment of the Zeolite Ferrierite Spectrum
journal, January 2003
- Profeta, Mickael; Mauri, Francesco; Pickard, Chris J.
- Journal of the American Chemical Society, Vol. 125, Issue 2
Solid-State 45 Sc NMR Studies of Cp* 2 Sc–OR (R = CMe 2 CF 3 , CMe(CF 3 ) 2 , C(CF 3 ) 3 , SiPh 3 ) and Relationship to the Structure of Cp* 2 Sc-Sites Supported on Partially Dehydroxylated Silica
journal, February 2020
- Culver, Damien B.; Huynh, Winn; Tafazolian, Hosein
- Organometallics, Vol. 39, Issue 7
17O Solid-State NMR Studies of Ta2O5 Nanorods
journal, April 2020
- Xu, Meng; Chen, Junchao; Wen, Yujie
- ACS Omega, Vol. 5, Issue 14
Atomistic Description of Reaction Intermediates for Supported Metathesis Catalysts Enabled by DNP SENS
journal, March 2016
- Ong, Ta-Chung; Liao, Wei-Chih; Mougel, Victor
- Angewandte Chemie International Edition, Vol. 55, Issue 15
Observation of Low-γ Quadrupolar Nuclei by Surface-Enhanced NMR Spectroscopy
journal, May 2020
- Nagashima, Hiroki; Trébosc, Julien; Kon, Yoshihiro
- Journal of the American Chemical Society, Vol. 142, Issue 24
Determining the Three-Dimensional Structures of Silica-Supported Metal Complexes from the Ground Up
journal, December 2021
- Perras, Frédéric A.; Kanbur, Uddhav; Paterson, Alexander L.
- Inorganic Chemistry, Vol. 61, Issue 2
Efficient transfer of DNP‐enhanced
1
H magnetization to half‐integer quadrupolar nuclei in solids at moderate spinning rate
journal, January 2021
- Nagashima, Hiroki; Trébosc, Julien; Kon, Yoshihiro
- Magnetic Resonance in Chemistry, Vol. 59, Issue 9-10
Formamide Adsorption at the Amorphous Silica Surface: A Combined Experimental and Computational Approach
journal, September 2018
- Signorile, Matteo; Salvini, Clara; Zamirri, Lorenzo
- Life, Vol. 8, Issue 4
Surface differences of oxide nanocrystals determined by geometry and exogenously coordinated water molecules
journal, January 2022
- Chen, Junchao; Wu, Xin-Ping; Hope, Michael A.
- Chemical Science, Vol. 13, Issue 37
On the use of solid-state 45 Sc NMR for structural investigations of molecular and silica-supported scandium amide catalysts
journal, January 2017
- Vancompernolle, T.; Trivelli, X.; Delevoye, L.
- Dalton Transactions, Vol. 46, Issue 39
Surface Organometallic Chemistry of Supported Iridium(III) as a Probe for Organotransition Metal–Support Interactions in C–H Activation
journal, May 2018
- Kaphan, David M.; Klet, Rachel C.; Perras, Frédéric A.
- ACS Catalysis, Vol. 8, Issue 6
The PAW/GIPAW approach for computing NMR parameters: A new dimension added to NMR study of solids
journal, July 2011
- Charpentier, Thibault
- Solid State Nuclear Magnetic Resonance, Vol. 40, Issue 1