Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids

Walder, Brennan J.; Alam, Todd M.

doi:10.3390/ijms21113938

Title: Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids

Abstract

Materials often contain minor heterogeneous phases that are difficult to characterize yet nonetheless significantly influence important properties. Here we describe a solid-state NMR strategy for quantifying minor heterogenous sample regions containing dilute, essentially uncoupled nuclei in materials where the remaining nuclei experience heteronuclear dipolar couplings. NMR signals from the coupled nuclei are dephased while NMR signals from the uncoupled nuclei can be amplified by one or two orders of magnitude using Carr-Meiboom-Purcell-Gill (CPMG) acquisition. The signal amplification by CPMG can be estimated allowing the concentration of the uncoupled spin regions to be determined even when direct observation of the uncoupled spin NMR signal in a single pulse experiment would require an impractically long duration of signal averaging. We use this method to quantify residual graphitic carbon using 13 C CPMG NMR in poly(carbon monofluoride) samples synthesized by direct fluorination of carbon from various sources. Our detection limit for graphitic carbon in these materials is better than 0.05 mol%. The accuracy of the method is discussed and comparisons to other methods are drawn.

Authors:

Walder, Brennan J.;

Publication Date:: 2020-05-30

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1631470

Alternate Identifier(s):: OSTI ID: 1634806

Report Number(s):: SAND2020-5728J
Journal ID: ISSN 1422-0067; IJMCFK; PII: ijms21113938

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Published Article

Journal Name:: International Journal of Molecular Sciences (Online)

Additional Journal Information:: Journal Name: International Journal of Molecular Sciences (Online) Journal Volume: 21 Journal Issue: 11; Journal ID: ISSN 1422-0067

Publisher:: MDPI

Country of Publication:: Switzerland

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Walder, Brennan J., and Alam, Todd M. Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids.  Switzerland: N. p., 2020. 
Web.  doi:10.3390/ijms21113938.

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                    Walder, Brennan J., & Alam, Todd M. Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids.  Switzerland.  https://doi.org/10.3390/ijms21113938

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                    Walder, Brennan J., and Alam, Todd M. Sat .  
"Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids".  Switzerland.  https://doi.org/10.3390/ijms21113938.

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@article{osti_1631470,

  title        = {Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids},

  author       = {Walder, Brennan J. and Alam, Todd M.},

  abstractNote = {Materials often contain minor heterogeneous phases that are difficult to characterize yet nonetheless significantly influence important properties. Here we describe a solid-state NMR strategy for quantifying minor heterogenous sample regions containing dilute, essentially uncoupled nuclei in materials where the remaining nuclei experience heteronuclear dipolar couplings. NMR signals from the coupled nuclei are dephased while NMR signals from the uncoupled nuclei can be amplified by one or two orders of magnitude using Carr-Meiboom-Purcell-Gill (CPMG) acquisition. The signal amplification by CPMG can be estimated allowing the concentration of the uncoupled spin regions to be determined even when direct observation of the uncoupled spin NMR signal in a single pulse experiment would require an impractically long duration of signal averaging. We use this method to quantify residual graphitic carbon using 13 C CPMG NMR in poly(carbon monofluoride) samples synthesized by direct fluorination of carbon from various sources. Our detection limit for graphitic carbon in these materials is better than 0.05 mol%. The accuracy of the method is discussed and comparisons to other methods are drawn.},

  doi          = {10.3390/ijms21113938},

  journal      = {International Journal of Molecular Sciences (Online)},

  number       = 11,

  volume       = 21,

  place        = {Switzerland},

  year         = {2020},

  month        = {5}

}

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Figure 1: Characteristics of bulk poly(carbon monofluoride) samples. (a) Photographs of the five samples overlaid by their names and their carbon sources; (b) X-ray diffraction spectra for the samples; (c) SEM/EDS map of (CF)_{n_}gr-PC; (d) photon counts for the EDS mapping shown in (c). The asterisk (*) in (b) ismore »

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Title: Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids

Abstract

Citation Formats

Figures / Tables:

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Modified Spin‐Echo Method for Measuring Nuclear Relaxation Times journal, August 1958

An Improved Broadband Decoupling Sequence for Liquid Crystals and Solids journal, January 2000

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On paramagnetism in fluorinated graphite: EPR and solid state NMR study journal, April 2001

EPR and Solid-State NMR Studies of Poly(dicarbon monofluoride) (C 2 F) n journal, June 2006

Quantitative Characterization of Humic Substances by Solid-State Carbon-13 Nuclear Magnetic Resonance journal, January 2000

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Quantitative solid-state 13C NMR with signal enhancement by multiple cross polarization
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Modified Spin‐Echo Method for Measuring Nuclear Relaxation Times
journal, August 1958

An Improved Broadband Decoupling Sequence for Liquid Crystals and Solids
journal, January 2000

Is Scanning Electron Microscopy/Energy Dispersive X-ray Spectrometry (SEM/EDS) Quantitative?: Quantitative SEM/EDS analysis
journal, August 2012

High-Resolution Carbon-13 Nuclear Magnetic Resonance Study of Some Solid, Glassy Polymers
journal, May 1975

NMR a critical tool to study the production of carbon fiber from lignin
journal, February 2013

Cooperation between Active Material, Polymeric Binder and Conductive Carbon Additive in Lithium Ion Battery Cathode
journal, February 2012

Practical guides for x-ray photoelectron spectroscopy: First steps in planning, conducting, and reporting XPS measurements
journal, May 2019

QCPMG-MAS NMR of Half-Integer Quadrupolar Nuclei
journal, March 1998

On paramagnetism in fluorinated graphite: EPR and solid state NMR study
journal, April 2001

EPR and Solid-State NMR Studies of Poly(dicarbon monofluoride) (C ₂ F) _n
journal, June 2006

Quantitative Characterization of Humic Substances by Solid-State Carbon-13 Nuclear Magnetic Resonance
journal, January 2000

NMR in rotating solids
journal, April 1979

29Si and 17O (Q)CPMG-MAS solid-state NMR experiments as an optimum approach for half-integer nuclei having long T1 relaxation times
journal, May 2002

A material science perspective of pharmaceutical solids
journal, July 2007

Spatial heterogeneity as the structure feature for structure–property relationship of metallic glasses
journal, September 2018

Quantitative cross-polarization NMR spectroscopy in uniformly 13C-labeled solids
journal, April 2006

Increased 29Si NMR sensitivity in glasses with a Carr–Purcell–Meiboom–Gill echotrain
journal, September 2008

Further conventions for NMR shielding and chemical shifts IUPAC recommendations 2008
journal, March 2008

High Frequency Dynamic Nuclear Polarization
journal, April 2013

Determination of aromatic hydrocarbon fraction in oil shale by 13C n.m.r. with magic-angle spinning
journal, August 1978

Proton‐enhanced NMR of dilute spins in solids
journal, July 1973

Nuclear magnetic resonance study of fluorine–graphite intercalation compounds and graphite fluorides
journal, April 1999

X-ray diffraction patterns of graphite and turbostratic carbon
journal, July 2007

Application of ¹¹⁹ Sn CPMG MAS NMR for Fast Characterization of Sn Sites in Zeolites with Natural ¹¹⁹ Sn Isotope Abundance
journal, March 2016

Communication: Phase incremented echo train acquisition in NMR spectroscopy
journal, June 2012

Zur Konstitution des Kohlenstoff-Monofluorids
journal, August 1947

Nuclear Spin-Lattice Relaxation Via Paramagnetic Centers Without Spin Diffusion
journal, August 1968

Improved sensitivity and quantification for 29Si NMR experiments on solids using UDEFT (Uniform Driven Equilibrium Fourier Transform)
journal, August 2019

Polarization-Enhanced NMR Spectroscopy of Biomolecules in Frozen Solution
journal, May 1997

Sensitivity-Enhanced Quadrupolar-Echo NMR of Half-Integer Quadrupolar Nuclei. Magnitudes and Relative Orientation of Chemical Shielding and Quadrupolar Coupling Tensors
journal, November 1997

The CPMG Pulse Sequence in Strong Magnetic Field Gradients with Applications to Oil-Well Logging
journal, March 1995

EPR study on petroleum cokes annealed at different temperatures and used in lithium and sodium batteries
journal, January 2002

On the interaction of nuclear spins in a crystalline lattice
journal, May 1949

Axiomatic theories of ideal stretched exponential relaxation (SER)
journal, November 2006

Symmetry pathways in solid-state NMR
journal, August 2011

Study on the Structure of C-S-H Gels of Slag–Cement Hardened Paste by 29Si, 27Al MAS NMR
journal, August 2019

Nuclear Spin-Lattice Relaxation via Paramagnetic Centers
journal, February 1968

Solid State ¹³ C and ¹⁹ F NMR Characterization of Fluorinated Charcoal
journal, March 1998

Categories of Coherence Pathways for the CPMG Sequence
journal, July 2002

29Si NMR in solid state with CPMG acquisition under MAS
journal, August 2008

Solid-State NMR ( ¹⁹ F and ¹³ C) Study of Graphite Monofluoride (CF) _n : ¹⁹ F Spin−Lattice Magnetic Relaxation and ¹⁹ F/ ¹³ C Distance Determination by Hartmann−Hahn Cross Polarization
journal, January 2005

Equivalence of the time-domain matched filter and the spectral-domain matched filter in one-dimensional NMR spectroscopy
journal, September 2010

Correlating structural distributions in silica glass with two-dimensional $J$ -resolved spectroscopy
journal, October 2018

Characterizing Nonexponential Spin-Lattice Relaxation in Solid-State NMR by Fitting to the Stretched Exponential
journal, January 1995