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One of the holy grails in chemistry is to reconstitute some of life’s functions with or within synthetic materials. In this contribution, we demonstrate that “simple” macromolecular architectures such as dendritic amphiphiles, Janus dendrimers, thermoresponsive and hybrid organic-inorganic (co)polymers enable to mimic some of the functions of proteins for biomineralization, natural bactericides, biological membranes or the stimuli-responsive cytoskeleton.
One of the holy grails in chemistry is to reconstruct some of life’s functions with synthetic materials. In this contribution, we demonstrate that “simple” macromolecular architectures such as dendritic amphiphiles, Janus dendrimers, thermoresponsive and hybrid organic-inorganic (co)polymers enable to mimic some of the functions of proteins for biomineralization, natural bactericides, biological membranes or the stimuli-responsive cytoskeleton.
UCST-type thermoresponsive polymers (i.e. that phase separate from solution upon cooling) present a tremendous potential not only in aqueous media where they can be used in drug delivery, diagnostic and microfluidic applications, but also in water/alcohol mixtures, where they can be used for instance in sensing systems for alcohol-soluble drugs. However, only a few thermoresponsive polymers have been reported that present an UCST in a relevant temperature range and “green” solvents such as water or ethanol.
In this context, acrylamide-based monomers can be very useful building blocks for designing novel non-ionic UCST-type polymers because of their hydrophilic nature (with the appropriate side chain) and propensity to form hydrogen bonds. We will present our latest results on the UCST-type thermoresponsive behaviour of acrylamide- and 2,6-diaminopyridine-based homopolymers and copolymers in water or water/alcohol mixtures, and give some insights about the rational design of UCST polymers relying on H-bonding.
UCST-type thermoresponsive polymers (i.e. that phase separate from solution upon cooling) present a tremendous potential not only in aqueous media where they can be used in drug delivery, diagnostic and microfluidic applications but also in water/alcohol mixtures, where they can be used for instance in sensing systems for alcohol-soluble drugs. However, only a few thermoresponsive polymers have been reported that present an UCST in a relevant temperature range and “green” solvents such as water or ethanol.
In this context, acrylamide-based monomers can be very useful building blocks for designing novel non-ionic UCST-type polymers because of their hydrophilic nature (with the right side chain) and propensity to form hydrogen bonds. We will present our latest results on the UCST-type thermoresponsive behaviour of acrylamide- and 2,6-diaminopyridine-based homopolymers and copolymers in water or water/alcohol mixtures, and give some insights about the rational design of UCST polymers relying on H-bonding.
UCST-type thermoresponsive polymers that phase separate from solution upon cooling present a tremendous potential not only in aqueous media where they can be used in drug delivery, diagnostic and microfluidic applications, but also in water/alcohol mixtures, where they can be used for instance in sensing systems for alcohol-soluble drugs. However, only a few thermoresponsive polymers have been reported that present an UCST in a relevant temperature range and “green” solvents such as water or ethanol. In this context, acrylamide-based monomers can be very useful building blocks for designing novel UCST-type polymers because of their hydrophilic nature (with the right side chain) and propensity to form hydrogen bonds.
We want to present our latest results on the copolymer poly(acrylamide-co-acrylonitrile) (P(AAm-co-AN)) that present a UCST in water as well as on two homopolymers based on an acrylamide derivative of 2,6-diaminopyridine, namely poly(N-(6-aminopyridin-2-yl)acrylamide) (PNAPAAm) and poly(N-(6-acetamidopyridin-2-yl)acrylamide) (PNAcAPAAm) that show UCST-type thermoresponsiveness in water/alcohol mixtures.
Our focus for P(AAm-co-AN)) is its aggregation behaviour above and below its phase transition temperature as the size of thermoresponsive polymeric systems is of prime importance for biomedical applications (as size dependent processes take place in the body) and is linked to the optical properties of a material that matter in materials science.
In the case of PNAPAAm and PNAcAPAAm, we focused on the co-solvency/co-non solvency effect on the phase transition temperature in water/alcohol mixture. Indeed, polymers with UCST behavior below 60°C in water/alcohol mixtures are extremely promising for the preparation of “smart” materials for sensing.
An UCST-type copolymer of acrylamide (AAm) and acrylonitrile (AN) (poly(AAm-co-AN)) was prepared by reversible addition fragmentation chain transfer (RAFT) polymerization and its temperature-induced phase transition and aggregation behaviour studied by turbidimetry, static and dynamic light scattering, small angle neutron scattering (SANS) and cryo-transmission electron microscopy (cryo-TEM) measurements. The phase transition temperature was found to increase with increasing AN content in the copolymer, concentration of the solutions and copolymer chain length. A significant effect was observed onto the phase transition temperature by addition of different electrolytes into the copolymer solution. The copolymer chains were aggregated below the phase transition temperature and disaggregated above it. The size of the aggregates increases with increasing AN contents and concentration of the copolymer solutions below the phase transition temperature. The copolymer chains were expanded and weekly associated in solution above the phase transition temperature. A model is proposed to explain such association–aggregation behaviour of poly(AAm-co-AN) copolymers depending on AN contents and concentration of the copolymer solutions as a function of temperature.
Thermoresponsive polymers have shown great potential in applications such as bioseparation, drug delivery and diagnostic. Only few thermoresponsive polymers that present an upper critical solution temperature (UCST), i.e. phase separate from solution upon cooling, in a relevant temperature range have been reported so far. Moreover, the most studied UCST type polymers namely polybetaines are difficult to use under physiological conditions, which significantly restricts their potential applications. Therefore, UCST polymers with sharp and robust phase transition in physiological conditions (in the presence of salts, etc.) are highly needed in order to extend the range of applications of this class of polymers.
A robust UCST-type copolymer of acrylamide (AAm) and acrylonitrile (AN) (poly(AAm-co-AN)) was prepared by reversible addition fragmentation chain transfer (RAFT) polymerization and its thermo-induced aggregation behavior in aqueous media was studied by turbidimetry, dynamic and static light scattering. At temperature below the UCST, the poly(AAm-co-AN) copolymer chains were aggregated together. The aggregate size was found to be larger with increasing AN contents and became smaller upon dilution of the copolymer solutions. While above the UCST, the poly(AAm-co-AN) copolymer chains were expanded and weekly associated in solution. The association between the copolymer chains formed smaller aggregates with increasing the AN contents or the concentration of the solutions. A model is proposed to explain such association-aggregation behavior of the poly(AAm-co-AN) copolymer depending on the AN contents and concentration of the solutions.