Allosterically controlled threading of polymers through macrocyclic dimers

Journal of the American Chemical Society
Seda CantekinRoeland J M Nolte

Abstract

As part of an ongoing study to construct a molecular Turing machine in which a polymer chain is encoded via allosteric information transfer between macrocyclic complexes, we describe the thermodynamic and kinetic characterization of a multicomponent self-assembled system based on a zinc porphyrin macrocyclic compound, a bidentate ligand (1,4-diazabicyclo[2.2.2]octane, DABCO), and a viologen-substituted polymer guest. Initial addition of DABCO to the porphyrin macrocycle in chloroform solution leads to the formation of a stable 2:1 (porphyrin:DABCO) dimeric complex, even under dilute conditions, by means of strong cooperative interactions involving hydrogen and metal-ligand bonds. Further titration of the porphyrin-DABCO mixtures with the polymer gives rise to a complex array of species in the solution. The system is analyzed in detail by a combination of spectroscopic measurements and computational modeling. Each association constant in the binding scheme and the fraction of each individual complex that is formed in solution are determined precisely using a mass-balance model. Kinetic studies revealed that the rates of the polymer threading and dethreading in and out of the dimeric system are remarkably slow, indicating that th...Continue Reading

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Citations

Sep 8, 2016·Chemistry : a European Journal·Zheng MengChuan-Feng Chen
Sep 29, 2015·Physical Chemistry Chemical Physics : PCCP·Cheng ShangDavid J Wales
Oct 7, 2016·Chemical Communications : Chem Comm·Lizhi ZhaoLinqi Shi
Jan 6, 2016·Chemistry : a European Journal·Kenji KobayashiMunechika Nakamura
Jun 9, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Marga C LensenJohannes A A W Elemans
Jul 25, 2019·Chemical Communications : Chem Comm·Johannes A A W Elemans, Roeland J M Nolte
Nov 13, 2015·Chemical Science·Shaji VargheseRoeland J M Nolte
Aug 30, 2018·Chemical Science·T H NgoS M Goldup
Jan 1, 2021·European Journal of Organic Chemistry·Kathleen StoutJohannes A A W Elemans
Mar 9, 2021·European Journal of Organic Chemistry·Jeroen P J BruekersRoeland J M Nolte
Dec 15, 2016·Journal of the American Chemical Society·Chengyuan YuHua Jiang

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