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Chain Packing in Linear Phenol−Polycarbonate by 13C{2H} REDOR

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Department of Chemistry, Washington University, St. Louis, Missouri 63130, and Department of Physics, Binghamton University, Binghamton, New York 13902
Cite this: Macromolecules 2002, 35, 7, 2608–2617
Publication Date (Web):February 28, 2002
https://doi.org/10.1021/ma010919i
Copyright © 2002 American Chemical Society

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    Abstract

    Interchain packing in [carbonyl-13C, phenol-2H]phenol-substituted bisphenol A polycarbonate (a totally amorphous polymer by X-ray powder diffraction) has been characterized by 13C{2H} rotational-echo double-resonance (REDOR) NMR measurements on a 10 Å distance scale. Differences in the REDOR dephasing rates of the centerband and spinning sidebands of the carbonyl carbon resonance prove the presence of local orientational order. Approximately 70% of the repeat units are locally ordered. For the most tightly packed pairs of chains, the phenol 2H of one chain is 4−5 Å from the carbonate 13C of the other chain, and the interchain 2H−13C dipolar vector has an orientation of approximately 30° (azimuthal) and 70° (polar) in the carbonyl carbon chemical shift tensor reference frame. The REDOR determination of these packing parameters is model-independent. Both random and chain-pair models were generated to describe the chain packing, but only the chain-pair model was consistent with the REDOR distance and orientation results.

     Washington University.

     Binghamton University.

    §

     Present address:  Bayer Plastics Division, Pittsburgh, PA 15205.

    #

     Present address:  Varian Associates, Palo Alto, CA 94304.

    *

     Corresponding author:  phone 314-935-6844; Fax 314-935-4481; e-mail [email protected].

    Cited By

    This article is cited by 12 publications.

    1. Chi Wai Cheung and Stephen L. Buchwald . Palladium-Catalyzed Hydroxylation of Aryl and Heteroaryl Halides Enabled by the Use of a Palladacycle Precatalyst. The Journal of Organic Chemistry 2014, 79 (11) , 5351-5358. https://doi.org/10.1021/jo500662s
    2. Daniel H. Bolton,, Jon M. Goetz,, Daoji Gan,, Jeffrey A. Byers,, Barbara Poliks,, Karen L. Wooley, and, Jacob Schaefer. Chain Dynamics in Linear and Hyperbranched Phenol−Polycarbonates. Macromolecules 2003, 36 (7) , 2368-2373. https://doi.org/10.1021/ma021648u
    3. Robert D. O'Connor,, Jeffery A. Byers,, William D. Arnold,, Eric Oldfield,, Karen L. Wooley, and, Jacob Schaefer. Chain Packing in Ethoxyphenyl−Polycarbonate by 13C{2H} REDOR. Macromolecules 2002, 35 (7) , 2618-2623. https://doi.org/10.1021/ma010918q
    4. Thomas Weldeghiorghis, Manmilan Singh, Jacob Schaefer. Molecular basis of secondary relaxation in stiff-chain glassy polymers. The Journal of Chemical Physics 2022, 157 (4) https://doi.org/10.1063/5.0087132
    5. Jae-Ho Lee, Moon-Su Kim, Hyo Lee, Ihl-Young Lee, Hyun Kim, Nam Kim, SangGap Lee, Hwajeong Seo, Younkee Paik. The Application of REDOR NMR to Understand the Conformation of Epothilone B. International Journal of Molecular Sciences 2017, 18 (7) , 1472. https://doi.org/10.3390/ijms18071472
    6. Dirk Stueber, Tsyr-Yan Yu, Berk Hess, Kurt Kremer, Robert D. O’Connor, Jacob Schaefer. Chain packing in polycarbonate glasses. The Journal of Chemical Physics 2010, 132 (10) https://doi.org/10.1063/1.3330412
    7. Emil Chibowski, Konrad Terpilowski. Surface free energy of polypropylene and polycarbonate solidifying at different solid surfaces. Applied Surface Science 2009, 256 (5) , 1573-1581. https://doi.org/10.1016/j.apsusc.2009.09.024
    8. Shigeru Matsuoka, Masayuki Inoue. Application of REDOR NMR in natural product chemistry. Chemical Communications 2009, 11 (38) , 5664. https://doi.org/10.1039/b910230b
    9. Dirk Stueber, Anil K. Mehta, Zhiyun Chen, Karen L. Wooley, Jacob Schaefer. Local order in polycarbonate glasses by 13 C{ 19 F} rotational-echo double-resonance NMR. Journal of Polymer Science Part B: Polymer Physics 2006, 44 (19) , 2760-2775. https://doi.org/10.1002/polb.20931
    10. Orsolya Toke, W. Lee Maloy, Sung Joon Kim, Jack Blazyk, Jacob Schaefer. Secondary Structure and Lipid Contact of a Peptide Antibiotic in Phospholipid Bilayers by REDOR. Biophysical Journal 2004, 87 (1) , 662-674. https://doi.org/10.1529/biophysj.103.032706
    11. Orsolya Toke, R.D. O’Connor, Thomas K. Weldeghiorghis, W. Lee Maloy, Ralf W. Glaser, Anne S. Ulrich, Jacob Schaefer. Structure of (KIAGKIA)3 Aggregates in Phospholipid Bilayers by Solid-State NMR. Biophysical Journal 2004, 87 (1) , 675-687. https://doi.org/10.1529/biophysj.103.032714
    12. Stephan L. Grage, Jude A. Watts, Anthony Watts. 2H{19F} REDOR for distance measurements in biological solids using a double resonance spectrometer. Journal of Magnetic Resonance 2004, 166 (1) , 1-10. https://doi.org/10.1016/j.jmr.2003.10.005

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