ja9b07737_si_002.mp4 (1.27 MB)
Switching Dual Catalysis without Molecular Switch: Using A Multicomponent Information System for Reversible Reconfiguration of Catalytic Machinery
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posted on 2019-09-19, 18:33 authored by Abir Goswami, Thomas Paululat, Michael SchmittelDifferent from the
current paradigms of chemistry, a switchable
catalytic system is presented that does not rely on a molecular switch
in different toggling states but on a smart seven-component mixture
that manages the reversible ON/OFF regulation of two catalytic processes.
Hereunto, the workflow of two multicomponent rotary catalytic machineries
was interlinked by the simultaneous shuffling of two components (metal
and ligand) requiring perfect signaling in a 13-component system (see
Movie 1). This network underwent reversible switching over three cycles
as demonstrated by 1H NMR, UV–vis, and fluorescence
spectroscopies and electrospray ionization mass spectrometry. Addition
and removal of zinc(II) ions trigger three distinct events in parallel:
the (i) mutually dependent self-assembly of three-component nanorotors
and two-component reservoirs by resorting components, (ii) toggling
between vastly different rotational exchange rates in the self-assembled
rotors that directly affect catalysis, and (iii) toggling between
two diverse catalytic reactions in a fully reproducible manner. Because
of this information system, the concentrations of free aza-crown ether 7 and its complex with copper(I), that is, [Cu(7)]+, which represent the effective catalysts, are up-
and downregulated in a manner to alternately switch ON/OFF a catalytic
conjugate addition and a click reaction.
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Reversible Reconfigurationfluorescence spectroscopiesself-assembled rotorstoggling states1 H NMRMolecular Switchconjugate additionthree-component nanorotorsUVexchange ratesclick reactionCatalytic Machineryseven-component mixturemanner13- component systeminformation systemMulticomponent Information Systemelectrospray ionization mass spectrometryaza-crown ether 7