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Efficient strategy for determining the atomic-resolution structure of micro- and nanocrystalline solids within polymeric microbeads: domain-edited NMR crystallography
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SYSNO ASEP 0491936 Druh ASEP J - Článek v odborném periodiku Zařazení RIV J - Článek v odborném periodiku Poddruh J Článek ve WOS Název Efficient strategy for determining the atomic-resolution structure of micro- and nanocrystalline solids within polymeric microbeads: domain-edited NMR crystallography Tvůrce(i) Brus, Jiří (UMCH-V) RID, ORCID
Czernek, Jiří (UMCH-V) RID
Hrubý, Martin (UMCH-V) RID, ORCID
Švec, Pavel (UMCH-V) RID, ORCID
Kobera, Libor (UMCH-V) RID, ORCID
Abbrent, Sabina (UMCH-V) RID, ORCID
Urbanová, Martina (UMCH-V) RID, ORCIDZdroj.dok. Macromolecules. - : American Chemical Society - ISSN 0024-9297
Roč. 51, č. 14 (2018), s. 5364-5374Poč.str. 11 s. Jazyk dok. eng - angličtina Země vyd. US - Spojené státy americké Klíč. slova NMR crystalography ; polymer microbeads ; solid-state self-assembly Vědní obor RIV CF - Fyzikální chemie a teoretická chemie Obor OECD Physical chemistry CEP GA16-04109S GA ČR - Grantová agentura ČR LO1507 GA MŠMT - Ministerstvo školství, mládeže a tělovýchovy LM2015064 GA MŠMT - Ministerstvo školství, mládeže a tělovýchovy Institucionální podpora UMCH-V - RVO:61389013 UT WOS 000440105200035 EID SCOPUS 85050672452 DOI 10.1021/acs.macromol.8b00392 Anotace Precise structural analysis of multiphase polymeric nanocomposites remains a challenge even in the presence of high-quality X-ray diffraction data. This contribution thus addresses our attempt to formulate a combined analytical strategy for obtaining the atomic-resolution structure of multicomponent polymeric solids with complex nanodomain architecture. In this strategy, through the application of T1-filtered solid-state NMR spectroscopy, the individual components are successively distinguished and selected, and the corresponding 1H, 13C, and 15N isotropic chemical shifts are explicitly assigned. Thereafter, using an automated protocol allowing for processing and statistical analysis of large data sets, the experimentally determined NMR parameters are systematically compared with those DFT-calculated for the representative set of crystal structure predictions. Particular attention is devoted to the analysis of NMR parameters of hydrogen-bonded protons which are responsible for molecular packing. As a result of this search, the structures of micro- and nanosized crystallites dispersed in the polymeric matrix are determined and independently verified by the measurements of through-space dipolar couplings. The potential of this strategy is demonstrated on injectable polyanhydride microbeads consisting of a mixture of microcrystalline decitabine and nanocrystalline sebacic acid, both incorporated in the semicrystalline polymeric matrix of poly(sebacic acid). Through the synergistic interplay between the measurements, calculations, and the statistical analysis, we have developed an integrated approach providing structural information that is challenging to elucidate using conventional diffraction approaches. This combination of experimental and theoretical approaches enables one to determine the structural arrangements of molecules in situations which are not tractable by conventional spectroscopic techniques. Pracoviště Ústav makromolekulární chemie Kontakt Eva Čechová, cechova@imc.cas.cz ; Tel.: 296 809 358 Rok sběru 2019
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