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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:
; ORCiD logo
Publication Date:
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.
Walder, Brennan J., & Alam, Todd M. Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids. Switzerland. doi:https://doi.org/10.3390/ijms21113938
Walder, Brennan J., and Alam, Todd M. Sat . "Quantification of Uncoupled Spin Domains in Spin-Abundant Disordered Solids". Switzerland. doi:https://doi.org/10.3390/ijms21113938.
@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}
}

Journal Article:
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DOI: https://doi.org/10.3390/ijms21113938

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