Journal
POLYMERS
Volume 9, Issue 12, Pages -Publisher
MDPI
DOI: 10.3390/polym9120719
Keywords
host-guest chemistry; layer-by-layer self-assembly; pillar[6]arene; pH-responsiveness
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Funding
- Deutsche Forschungsgemeinschaft (DFG)
- National Natural Science Foundation of China (NFSC) as a part of the Sino-German collaborative research center [TRR61]
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A water-soluble, anionic pillar[6]arene derivative (WP6) is applied as monomeric building block for the layer-by-layer self-assembly of thin polyelectrolyte multilayer films, and its pH-dependent host-guest properties are employed for the reversible binding and release of a methylviologen guest molecule. The alternating assembly of anionic WP6 and cationic diazo resin (DAR) is monitored in-situ by a dissipative quartz crystal microbalance (QCM-D). In solution, the formation of a stoichiometric inclusion complex of WP6 and cationic methylviologen (MV) as guest molecule is investigated by isothermal titration calorimetry and UV-vis spectroscopy, respectively, and attributed to electrostatic interactions as primary driving force of the host-guest complexation. Exposure of WP6-containing multilayers to MV solution reveals a significant decrease of the resonance frequency, confirming MV binding. Subsequent release is achieved by pH lowering, decreasing the host-guest interactions. The dissociation of the host-guest complex, release of the guest from the film, as well as full reversibility of the binding event are identified by QCM-D. In addition, UV-vis data quantify the surface coverage of the guest molecule in the film after loading and release, respectively. These findings establish the pH-responsiveness of WP6 as a novel external stimulus for the reversible guest molecule recognition in thin films.
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