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Donor–Acceptor-Type Supramolecular Polymers Derived from Robust yet Responsive Heterodimeric Tweezers
journal contribution
posted on 2016-08-26, 18:33 authored by Yu-Kui Tian, Yi-Fei Han, Zhi-Shuai Yang, Feng WangMolecular
tweezer/guest recognition has emerged as a novel motif
for the construction of supramolecular polymers. However, the overwhelming
majority of ADA- or DAD-type (D = donor, A = acceptor) molecular tweezer/guest
recognition systems suffer from relatively low binding affinities
and inconspicuous variations toward external stimuli. To address this
issue, herein a novel heterodimeric DADA-type complex has been designed
and constructed. By engineering of donor–acceptor and hydrogen-bonding
interactions, it demonstrates 1000 times enhancement for the complexation
strength (Ka = 2.23 × 106 M–1) than the ADA-type counterpart. Moreover,
by modulating the intermolecular hydrogen bonds involved in the system,
its binding affinity exhibits significantly large variations toward
external stimuli (∼102–103-fold
change for Ka). The robust yet adaptive
heterodimeric complex is employed as a tecton for the fabrication
of high-molecular-weight donor–acceptor-type supramolecular
polymers, demonstrating the efficiency and versatility to develop
self-assembled materials via rational engineering of fundamental noncovalent
recognition motifs.
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binding affinitiesnovel motif1000 times enhancementcomplexation strengthsupramolecular polymersbinding affinity exhibitsself-assembled materialsadaptive heterodimericADA-type counterpartnoncovalent recognition motifsnovel heterodimeric DADA-typehydrogen-bonding interactionstweezerdonorhydrogen bondsvariationstimuli
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