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      Mass Spectrometry and Gas-Phase Chemistry of Bismuth-Oxido Clusters

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      ChemPlusChem

      Wiley

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          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 (1)H NMR and (1)H,(1)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 self-sorted 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.
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            Room-Temperature CH Bond Activation of Methane by Bare [P4O10].+

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              Activation of methane by oligomeric (Al2O3)x(+) (x = 3,4,5): the role of oxygen-centered radicals in thermal hydrogen-atom abstraction.

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                Author and article information

                Journal
                ChemPlusChem
                ChemPlusChem
                Wiley
                21926506
                September 2013
                September 2013
                June 17 2013
                : 78
                : 9
                : 1005-1014
                Article
                10.1002/cplu.201300122
                © 2013

                http://doi.wiley.com/10.1002/tdm_license_1.1

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