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RAFT Polymerization of an Intrinsically Stretchable Water-Soluble Block Copolymer Scaffold for PEDOT.

ABSTRACT: Despite the common association of ?-conjugated polymers with flexible and stretchable electronics, these materials can be rigid and brittle unless they are designed otherwise. For example, low modulus, high extensibility, and high toughness are treated as prerequisites for integration with soft and biological structures. One of the most successful and commercially available organic electronic materials is the conductive and brittle polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS). To make this material stretchable, additives such as ionic liquids must be used. These additives may render the composite incompatible with biological tissue. In this work, we describe the synthesis of an intrinsically stretchable variant of the conductive polymer PEDOT:PSS that is free of additives. The approach involves the synthesis of a block copolymer comprising soft segments of poly(polyethylene glycol methyl ether acrylate) (PPEGMEA) and hard segments of poly(styrene sulfonate) (PSS) using a reversible addition-fragmentation chain transfer (RAFT) polymerization. Subsequently, we used the newly synthesized ionic elastomer PSS-b-PPEGMEA as a matrix for the oxidative polymerization of EDOT. The resulting polyelectrolyte elastomer, PEDOT:PSS-b-PPEGMEA, can withstand elongations up to 128% and has a toughness up to 10.1 MJ m-3. While the polyelectrolyte elastomer is not as conductive as the commercial material, the toughness and extensibility are each more than an order of magnitude higher. Moreover, the electrical conductivity of the polyelectrolyte elastomer exhibits minimal decrease with strain within the elastic regime. We then compared the block copolymer to physical blends of PEDOT:PSS and PPEGMEA. The blend material had a much lower failure strain of only 38% and a maximum toughness of 4.9 MJ m-3. This approach thus emphasizes the importance of the covalent linking of the PSS and PPEGMEA blocks. Furthermore, we demonstrate that the conductivity of scratched films can be restored upon exposure to water.

SUBMITTER: Kayser LV

PROVIDER: S-EPMC6435338 | biostudies-literature | 2018 Jul

REPOSITORIES: biostudies-literature

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RAFT Polymerization of an Intrinsically Stretchable Water-Soluble Block Copolymer Scaffold for PEDOT.

Kayser Laure V LV Russell Madeleine D MD Rodriquez Daniel D Abuhamdieh Sami N SN Dhong Charles C Khan Salik S Stein Alexander N AN Ramírez Julian J Lipomi Darren J DJ

Chemistry of materials : a publication of the American Chemical Society 20180608 13

Despite the common association of π-conjugated polymers with flexible and stretchable electronics, these materials can be rigid and brittle unless they are designed otherwise. For example, low modulus, high extensibility, and high toughness are treated as prerequisites for integration with soft and biological structures. One of the most successful and commercially available organic electronic materials is the conductive and brittle polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(st ...[more]

PMID: 30930534

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Project description:A poly(2-(dimethylamino)ethyl methacrylate) (PDMA) chain transfer agent (CTA) is used for the reversible addition-fragmentation chain transfer (RAFT) alcoholic dispersion polymerization of benzyl methacrylate (BzMA) in ethanol at 70 °C. THF GPC analysis indicated a well-controlled polymerization with molecular weight increasing linearly with conversion. GPC traces also showed high blocking efficiency with no homopolymer contamination apparent and Mw/Mn values below 1.35 in all cases. 1H NMR studies confirmed greater than 98% BzMA conversion for a target PBzMA degree of polymerization (DP) of up to 600. The PBzMA block becomes insoluble as it grows, leading to the in situ formation of sterically stabilized diblock copolymer nanoparticles via polymerization-induced self-assembly (PISA). Fixing the mean DP of the PDMA stabilizer block at 94 units and systematically varying the DP of the PBzMA block enabled a series of spherical nanoparticles of tunable diameter to be obtained. These nanoparticles were characterized by TEM, DLS, MALLS, and SAXS, with mean diameters ranging from 35 to 100 nm. The latter technique was particularly informative: data fits to a spherical micelle model enabled calculation of the core diameter, surface area occupied per copolymer chain, and the mean aggregation number (Nagg). The scaling exponent derived from a double-logarithmic plot of core diameter vs PBzMA DP suggests that the conformation of the PBzMA chains is intermediate between the collapsed and fully extended state. This is in good agreement with 1H NMR studies, which suggest that only 5-13% of the BzMA residues of the core-forming chains are solvated. The Nagg values calculated from SAXS and MALLS are in good agreement and scale approximately linearly with PBzMA DP. This suggests that spherical micelles grow in size not only as a result of the increase in copolymer molecular weight during the PISA synthesis but also by exchange of individual copolymer chains between micelles and/or by sphere-sphere fusion events.

Dataset Information

RAFT Polymerization of an Intrinsically Stretchable Water-Soluble Block Copolymer Scaffold for PEDOT.

Publications

RAFT Polymerization of an Intrinsically Stretchable Water-Soluble Block Copolymer Scaffold for PEDOT.

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