Monitoring Self-Sorting by Electrospray Ionization Mass Spectrometry: Formation Intermediates and Error-Correction during the Self-Assembly of Multiply Threaded Pseudorotaxanes.
Three binary pseudorotaxanes, which are based on two different secondary ammonium/crown ether binding motifs, have been studied by H NMR and H,H EXSY NMR experiments with respect to their thermodynamic stabilities and their axle exchange kinetics. The stability ranking does not follow the order of a...
| Publicado en: | Journal of the American Chemical Society Vol. 132; no. 7; pp. 2309 - 2321 |
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| Autores principales: | , , , |
| Formato: | Artículo |
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American Chemical Society
2/24/2010
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| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=48616436&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 48616436 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 2/24/2010 vid: 132 iid: 7 pid: 997 pub: American Chemical Society artinfo: ui: 48616436 10.1021/ja9101369 ppf: 2309 ppct: 12 formats: tig: atl: Monitoring Self-Sorting by Electrospray Ionization Mass Spectrometry: Formation Intermediates and Error-Correction during the Self-Assembly of Multiply Threaded Pseudorotaxanes. aug: au: Wei Jiang Schafer, Andreas Mohr, Parveen Choudhary Schalley, Christoph A. affil: institut für Chemie und Biochemie, Freie Uniuersität Berlin, Takustrasse 3, 14195 Berlin, Germany su: Electrospray ionization mass spectrometry Ammonium Thermodynamic equilibrium Dynamics Ether (Anesthetic) Rotaxanes sug: subj: Electrospray ionization mass spectrometry Ammonium Thermodynamic equilibrium Dynamics Ether (Anesthetic) Rotaxanes ab: Three binary pseudorotaxanes, which are based on two different secondary ammonium/crown ether binding motifs, have been studied by H NMR and H,H EXSY NMR experiments with respect to their thermodynamic stabilities and their axle exchange kinetics. The stability ranking does not follow the order of axle exchange rates, and the thermodynamically most stable axle-wheel combinations assemble only slowly. On the basis of these binding motifs, a series of self-sorting systems have been studied ranging from simple four-component mixtures through sequence-specific pseudorotaxanes to multiply threaded complexes. Because of the mismatch of kinetic and thermodynamic order, wrongly assembled structures are unavoidable, which require error-correction steps to yield the final thermodynamically controlled selfsorted products. These error-correction steps can easily be monitored by electrospray mass spectrometry, when a mixed-flow microreactor is coupled to the ion source to cover second time scales. Self-assembly intermediates, wrongly assembled structures, and the final thermodynamic products can be simultaneously identified. The determination of preferred assembly pathways as well as the formation of dead-end structures provides a clear picture of a rich kinetic behavior of the self-sorting systems under study. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2010 holdings: @attributes: islocal: N |
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