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Title: DNP-enhanced ultrawideline solid-state NMR spectroscopy: Studies of platinum in metal–organic frameworks

Abstract

Ultrawideline dynamic nuclear polarization (DNP)-enhanced 195Pt solid-state NMR (SSNMR) spectroscopy and theoretical calculations are used to determine the coordination of atomic Pt species supported within the pores of metal–organic frameworks (MOFs). The 195Pt SSNMR spectra, with breadths reaching 10,000 ppm, were obtained by combining DNP with broadbanded cross-polarization and CPMG acquisition. Although the DNP enhancements in static samples are lower than those typically observed under magic-angle spinning conditions, the presented measurements would be very challenging using the conventional SSNMR methods. The DNP-enhanced ultrawideline NMR spectra served to separate signals from cis- and trans-coordinated atomic Pt2+ species supported on the UiO-66-NH2 MOF. Here, the data revealed a dominance of kinetic effects in the formation of Pt2+ complexes and the thermodynamic effects in their reduction to nanoparticles. A single cis-coordinated Pt2+ complex was confirmed in MOF-253.

Authors:
 [1];  [1];  [2];  [2];  [3];  [3]
  1. Ames Lab., Ames, IA (United States)
  2. Iowa State Univ., Ames, IA (United States)
  3. Ames Lab. and Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1278754
Report Number(s):
IS-J-9007
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 13; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kobayashi, Takeshi, Perras, Frederic A., Goh, Tian Wei, Metz, Tanner L., Huang, Wenyu, and Pruski, Marek. DNP-enhanced ultrawideline solid-state NMR spectroscopy: Studies of platinum in metal–organic frameworks. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b00860.
Kobayashi, Takeshi, Perras, Frederic A., Goh, Tian Wei, Metz, Tanner L., Huang, Wenyu, & Pruski, Marek. DNP-enhanced ultrawideline solid-state NMR spectroscopy: Studies of platinum in metal–organic frameworks. United States. https://doi.org/10.1021/acs.jpclett.6b00860
Kobayashi, Takeshi, Perras, Frederic A., Goh, Tian Wei, Metz, Tanner L., Huang, Wenyu, and Pruski, Marek. Mon . "DNP-enhanced ultrawideline solid-state NMR spectroscopy: Studies of platinum in metal–organic frameworks". United States. https://doi.org/10.1021/acs.jpclett.6b00860. https://www.osti.gov/servlets/purl/1278754.
@article{osti_1278754,
title = {DNP-enhanced ultrawideline solid-state NMR spectroscopy: Studies of platinum in metal–organic frameworks},
author = {Kobayashi, Takeshi and Perras, Frederic A. and Goh, Tian Wei and Metz, Tanner L. and Huang, Wenyu and Pruski, Marek},
abstractNote = {Ultrawideline dynamic nuclear polarization (DNP)-enhanced 195Pt solid-state NMR (SSNMR) spectroscopy and theoretical calculations are used to determine the coordination of atomic Pt species supported within the pores of metal–organic frameworks (MOFs). The 195Pt SSNMR spectra, with breadths reaching 10,000 ppm, were obtained by combining DNP with broadbanded cross-polarization and CPMG acquisition. Although the DNP enhancements in static samples are lower than those typically observed under magic-angle spinning conditions, the presented measurements would be very challenging using the conventional SSNMR methods. The DNP-enhanced ultrawideline NMR spectra served to separate signals from cis- and trans-coordinated atomic Pt2+ species supported on the UiO-66-NH2 MOF. Here, the data revealed a dominance of kinetic effects in the formation of Pt2+ complexes and the thermodynamic effects in their reduction to nanoparticles. A single cis-coordinated Pt2+ complex was confirmed in MOF-253.},
doi = {10.1021/acs.jpclett.6b00860},
journal = {Journal of Physical Chemistry Letters},
number = 13,
volume = 7,
place = {United States},
year = {Mon Jun 06 00:00:00 EDT 2016},
month = {Mon Jun 06 00:00:00 EDT 2016}
}

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