An approach for supporting a Pd-NHC complex on a soluble star polymer with nanoscale dimensions is described. The resulting star polymer catalyst exhibits excellent activity in cross-coupling reactions, is stable in air and moisture, and is easily recoverable and recyclable. These properties are distinct and unattainable with the small-molecule version of the same catalyst.
Amphiphilic metallo-supramolecular diblock copolymers containing either a reversible cobalt(III) or nickel(II) heteroleptic bis-terpyridine complex at the junction between a polystyrene and a poly(ethylene oxide) block have been successfully prepared.
This review deals with nanoporous materials made from the self-assembly of block copolymers with a special interest in the chemical functions covering the surface of their nanopores. A detailed overview of the existing methods and strategies to generate well-defined organic functional groups covering the surface of the pore walls is provided. This further enables to finely tune the affinity of the pore walls and to perform well-defined chemical reactions onto them, which is essential for further dedicated applications.
We investigate nanoparticle (NP) dispersion, polymer conformations, entanglements and dynamics in ionic nanocomposites. To this end, we study nanocomposite systems with various spherical NP loadings, three different molecular weights, two different Bjerrum lengths, and two types of charge-sequenced polymers by means of molecular dynamics simulations. NP dispersion can be achieved in either oligomeric or entangled polymeric matrices due to the presence of electrostatic interactions. We show that the overall conformations of ionic oligomer chains, as characterized by their radii of gyration, are affected by the presence and the amount of charged NPs, while the dimensions of charged entangled polymers remain unperturbed. Both the dynamical behavior of polymers and NPs, and the lifetime and amount of temporary crosslinks, are found to depend on the ratio between the Bjerrum length and characteristic distance between charged monomers. Polymer–polymer entanglements start to decrease beyond a certain NP loading. The dynamics of ionic NPs and polymers is very different compared with their non-ionic counterparts. Specifically, ionic NP dynamics is getting enhanced in entangled matrices and also accelerates with the increase of NP loading.
Well-defined polystyrene-block-poly(tert-butylacrylate) diblock copolymers end-functionalized by a terpyridine ligand (PS-b-PtBA-[) were synthesized by nitroxide mediated polymerization (NMP) in the presence of an initiator bearing a terpyridine moiety. These materials were then hierarchically organized over two levels of self-assembly to yield metallo-supramolecular micellar gels. The first level of self-assembly is the formation of micelles in the dilute regime. Spherical or cylindrical micelles were obtained depending on the block copolymer composition as well as the method of preparation. The second level of self-assembly was triggered upon addition of Ni(II) ions to the concentrated micellar solutions. Rotational rheometry was used to probe the impact of the micellar morphology and the presence of a co-solvent on the mechanical properties of the gel.
A number of fluorous amphiphilic star block-copolymers containing a tris(benzyltriazolylmethyl)amine motif have been prepared. These polymers assembled into well-defined nanostructures in water, and their mode of assembly could be controlled by changing the composition of the polymer. The polymers were used for enzyme-inspired catalysis of alcohol oxidation.
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