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Title: Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis

Abstract

The development of multi-dimensional statistical methods has been demonstrated on variable contact time (VCT) 29Si{ 1H} cross-polarization magic angle spinning (CP/MAS) data sets collected using Carr–Purcell–Meiboom–Gill (CPMG) type acquisition. These methods utilize the transformation of the collected 2D VCT data set into a 3D data set and use tensor-rank decomposition to extract the spectral components that vary as a function of transverse relaxation time ( T 2) and CP contact time. The result is a data dense spectral set that can be used to reconstruct CP/MAS spectra at any contact time with a high signal to noise ratio and with an excellent agreement to 29Si{ 1H} CP/MAS spectra collected using conventional acquisition. These CPMG data can be collected in a fraction of time that would be required to collect a conventional VCT data set. Here, we demonstrate the method on samples of functionalized mesoporous silica materials and show that the method can provide valuable surface specific information about their functional chemistry.

Authors:
ORCiD logo [1];  [2];  [3]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  3. Hunter College of City Univ. of New York, New York, NY (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1463021
Alternate Identifier(s):
OSTI ID: 1456294; OSTI ID: 1464198
Report Number(s):
LLNL-JRNL-736456; SAND-2018-8223J
Journal ID: ISSN 1463-9076; PPCPFQ; 888524
Grant/Contract Number:  
AC52-07NA27344; AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 26; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mason, H. E., Uribe, E. C., and Shusterman, J. A. Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis. United States: N. p., 2018. Web. doi:10.1039/C8CP02382D.
Mason, H. E., Uribe, E. C., & Shusterman, J. A. Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis. United States. doi:10.1039/C8CP02382D.
Mason, H. E., Uribe, E. C., and Shusterman, J. A. Wed . "Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis". United States. doi:10.1039/C8CP02382D. https://www.osti.gov/servlets/purl/1463021.
@article{osti_1463021,
title = {Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis},
author = {Mason, H. E. and Uribe, E. C. and Shusterman, J. A.},
abstractNote = {The development of multi-dimensional statistical methods has been demonstrated on variable contact time (VCT) 29Si{1H} cross-polarization magic angle spinning (CP/MAS) data sets collected using Carr–Purcell–Meiboom–Gill (CPMG) type acquisition. These methods utilize the transformation of the collected 2D VCT data set into a 3D data set and use tensor-rank decomposition to extract the spectral components that vary as a function of transverse relaxation time (T2) and CP contact time. The result is a data dense spectral set that can be used to reconstruct CP/MAS spectra at any contact time with a high signal to noise ratio and with an excellent agreement to 29Si{1H} CP/MAS spectra collected using conventional acquisition. These CPMG data can be collected in a fraction of time that would be required to collect a conventional VCT data set. Here, we demonstrate the method on samples of functionalized mesoporous silica materials and show that the method can provide valuable surface specific information about their functional chemistry.},
doi = {10.1039/C8CP02382D},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 26,
volume = 20,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1 Fig. 1: Data derived from the tensor-rank decomposition of variable contact time 29Si{1H} CP/MAS CPMG NMR data sets for the DPTS-SBA sample. Contributions from component 1 are given in blue and those from component 2 are given in red (a) The extracted T2 data points (solid symbols) and their correspondingmore » least-square fits (solid lines). (b) The extracted variable contact time data points (solid symbols) and their corresponding least squares fits to standard CP kinetics equation (solid lines). (c) Extracted FID' s presented in real space as alternating real and imaginary data points. (d). Full echo Fourier transforms of the FID' s presented in (c) and corrected for difference in magnitude using the T2 fits in (a)« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.