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Preparation and Characterization of Thermo-Responsive Rod-Coil Diblock Copolymers.

ABSTRACT: In this study, we synthesized amphiphilic poly(2,7⁻(9,9⁻dioctylfluorene))⁻block⁻N,N⁻(diisopropylamino)ethyl methacrylate (POF⁻b⁻PDPMAEMA) rod-coil diblock copolymers by atom transfer radical polymerization (ATRP). The structure and multifunctional sensing properties of these copolymers were also investigated. The POF rod segment length of 10 was fixed and the PDPAEMA coil segment lengths of 90 and 197 were changed, respectively. The micellar aggregates of POF₁₀⁻b⁻PDPAEMA₉₀ rod-coil diblock copolymer in water showed a reversible shape transition from cylinder bundles to spheres when the temperature was changed from 20 to 80 °C or the pH was changed from 11 to 2. The atomic force microscopy (AFM) and transmission electron microscopy (TEM) measurements indicated that the temperature had also an obvious influence on the micelle size. In addition, since POF₁₀⁻b⁻PDPAEMA₉₀ had a lower critical solution temperature, its photoluminescence (PL) intensity in water is thermoreversible. The PL spectra showed that the POF⁻b⁻PDPAEMA copolymer had a reversible on/off profile at elevated temperatures, and thus could be used as an on/off fluorescent indicator for temperature or pH. The fluorescence intensity distribution of pH switched from "off⁻on" to "on⁻off" as the temperature increased. These results showed that the POF⁻b⁻PDPAEMA copolymer has a potential application for temperature and pH sensing materials.

SUBMITTER: Yu YY

PROVIDER: S-EPMC6418999 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:INTRODUCTION:Intracellular delivery is a key step for many applications in medicine and for investigations into cellular function. This is particularly true for immunotherapy, which often requires controlled delivery of antigen and adjuvants to the cytoplasm of immune cells. Due to the complex responses generated by the stimulation of diverse immune cell populations, it is critical to monitor which cells are targeted during treatment. To address this issue, we have engineered an immunotheranostic polymersome delivery system that fluorescently marks immune cells following intracellular delivery. METHODS:N-(3-bromopropyl)phthalimide end-capped poly(ethylene glycol)-bl-poly(propylene sulfide) (PEG-PPS-PI) was synthesized by anionic ring opening polymerization and linked with PEG-PPS-NH2 via a perylene bisimide (PBI) bridge to form a tetrablock copolymer (PEG-PPS-PBI-PPS-PEG). Block copolymers were assembled into polymersomes by thin film hydration in phosphate buffered saline and characterized by dynamic light scattering, cryogenic electron microscopy and fluorescence spectroscopy. Polymersomes were injected subcutaneously into the backs of mice, and draining lymph nodes were extracted for flow cytometric analysis of cellular uptake and disassembly. RESULTS:Modular self-assembly of tetrablock / diblock copolymers in aqueous solutions induced ?-? stacking of the PBI linker that both red-shifted and quenched the PBI fluorescence. Reactive oxygen species within the endosomes of phagocytic immune cell populations oxidized the PPS blocks, which disassembled the polymersomes for dequenching and shifting of the PBI fluorescence from 640 nm to 550 nm emission. Lymph node resident macrophages and dendritic cells were found to increase in 550 nm emission over the course of 3 days by flow cytometry. CONCLUSIONS:Immunotheranostic polymersomes present a versatile platform to probe the contributions of specific cell populations during the elicitation of controlled immune responses. Flanking PBI with two oxidation-sensitive hydrophobic PPS blocks enhanced ? stacking and introduced a mechanism for disrupting ?-? interactions to shift PBI fluorescence in response to oxidative conditions. Shifts from red (640 nm) to green (550 nm) fluorescence occurred in the presence of physiologically relevant concentrations of reactive oxygen species and could be observed within phagocytic cells both in vitro and in vivo.

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Preparation and Characterization of Thermo-Responsive Rod-Coil Diblock Copolymers.

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