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Aggregation-Induced Expansion of Poly-(N-isopropyl acrylamide) Solutions Observed Directly by the Transient Grating Imaging Technique.

ABSTRACT: The anomalous volume expansion of poly-(N-isopropyl acrylamide) (PNIPAM) solutions was observed during the thermally induced polymer phase transition of aqueous solutions having concentrations in the 3-7 wt % range. The process occurred on a millisecond time scale, and a laser temperature-jump time-resolved technique was used to bring about the process. After heating a solution with a pulse laser exploiting light absorption by dyes added to the solution itself, a phase transition was observed to take place, and the temporal changes associated with it were visualized through the transient grating imaging technique, whereby the solution was heated with a stripe pattern. We found several processes occurring on a millisecond time scale, all of which clearly took place after each PNIPAM molecule had collapsed structurally from a coiled to a globular conformation. During the so-called demixing process, the globular polymers aggregated with each other within 10 ms, and suddenly the polymer phase expanded as aggregation progressed further. After this process, the individual globular polymers reverted to their coiled conformation via hydration during the remixing process. We proposed that solution expansion was caused by the mutual entangling of multiple globular PNIPAM molecules, instead each globule polymer was separated.

SUBMITTER: Kato D

PROVIDER: S-EPMC6645113 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Aggregation-Induced Expansion of Poly-(<i>N</i>-isopropyl acrylamide) Solutions Observed Directly by the Transient Grating Imaging Technique.

Kato Daiki D Sohn Woon Yong WY Katayama Kenji K

ACS omega 20180801 8

The anomalous volume expansion of poly-(<i>N</i>-isopropyl acrylamide) (PNIPAM) solutions was observed during the thermally induced polymer phase transition of aqueous solutions having concentrations in the 3-7 wt % range. The process occurred on a millisecond time scale, and a laser temperature-jump time-resolved technique was used to bring about the process. After heating a solution with a pulse laser exploiting light absorption by dyes added to the solution itself, a phase transition was obse ...[more]

PMID: 31458976

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Project description:Thermoresponsive poly((N,N-dimethyl acrylamide)-co-(N-isopropyl acrylamide)) (P(DMA-co-NIPAM)) copolymers were synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization. The monomer reactivity ratios were determined by the Kelen-Tüdős method to be rNIPAM = 0.83 and rDMA = 1.10. The thermoresponsive properties of these copo-lymers with varying molecular weights were characterized by visual turbidimetry and dynamic light scattering (DLS). The copolymers showed a lower critical solution temperature (LCST) in water with a dependence on the molar fraction of DMA in the copolymer. Chaotropic and kosmotropic salt anions of the Hofmeister series, known to affect the LCST of thermoresponsive polymers, were used as additives in the aqueous copolymer solutions and their influence on the LCST was demonstrated. Further on, in order to investigate the thermoresponsive behavior of P(DMA-co-NIPAM) in a confined state, P(DMA-co-NIPAM)-b-PS diblock copolymers were prepared via polymerization induced self-assembly (PISA) through surfactant-free RAFT mediated emulsion polymerization of styrene using P(DMA-co-NIPAM) as the macromolecular chain transfer agent (mCTA) of the polymerization. As confirmed by cryogenic transmission electron microscopy (cryoTEM), this approach yielded stabilized spherical micelles in aqueous dispersions where the PS block formed the hydrophobic core and the P(DMA-co-NIPAM) block formed the hydrophilic corona of the spherical micelle. The temperature-dependent behavior of the LCST-type diblock copolymers was further studied by examining the collapse of the P(DMA-co-NIPAM) minor block of the P(DMA-co-NIPAM)-b-PS diblock copolymers as a function of temperature in aqueous solution. The nanospheres were found to be thermosensitive by changing their hydrodynamic radii almost linearly as a function of temperature between 25 °C and 45 °C. The addition of kosmotropic salt anions, as a potentially useful tuning feature of micellar assemblies, was found to increase the hydrodynamic radius of the micelles and resulted in a faster collapse of the micelle corona upon heating.

Dataset Information

Aggregation-Induced Expansion of Poly-(N-isopropyl acrylamide) Solutions Observed Directly by the Transient Grating Imaging Technique.

Publications

Aggregation-Induced Expansion of Poly-(<i>N</i>-isopropyl acrylamide) Solutions Observed Directly by the Transient Grating Imaging Technique.

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