A living radical polymerization (LRP) is a free radical polymerization that aims at displaying living character, (i.e., does not terminate or transfer and is able to continue polymerization once the initial feed is exhausted by addition of more monomer). However, termination reactions are inherent to a radical process, and modern LRP techniques seek to minimize such reactions, therefore providing control over the molecular weight and the molecular weight distribution of a polymeric material. In addition, the better LRP techniques incorporate many of the desirable features of traditional free radical polymerization, such as compatibility with a wide range of monomers, tolerance of many functionalities, and facile reaction conditions. The control of molecular weight and molecular weight distribution has enabled access to complex architectures and site specific functionality that were previously impossible to achieve via traditional free radical polymerizations. These LRPs are classified in three different subgroups: (1) stable free-radical polymerization such as nitroxide mediated polymerization (NMP),1,2 (2) degenerative transfer polymerization, such as iodine transfer polymerization (ITP and RITP),3,4 single electron transfer-degenerative transfer living radical polymerization(SET-DTLRP),5,6reversibleaddition-fragmentation chain transfer (RAFT),7,8 and macromolecular design via the interchange of xanthates (MADIX)9,10 polymerization, and (3) metal mediated catalyzed polymerization, such as atom transfer radical polymerization (ATRP),11-14 single electron transfer-living radical polymerization (SET-LRP),15 and organotellurium mediated living radical polymrization16-19 Among the existing LRP techniques, RAFT and MADIX are probably the most versatile processes, as they are tolerant * E-mail: T.P.D., T.Davis@UNSW.edu.au; S.P., S.Perrier@ chem.usyd.edu.au. † Centre for Advanced Macromolecular Design (CAMD), School of Chemical Sciences & Engineering, UNSW. ‡ Centre for Advanced Macromolecular Design (CAMD), School of Biotechnology & Biomolecular Sciences, UNSW. § The University of Sydney. Chem. Rev. 2009, 109, 5402–5436 5402

Bioapplications of RAFT polymerization.

A full-spectrum (300-850 nm) responsive donor-acceptor (D-A) supramolecular photocatalyst tetraphenylporphinesulfonate/fullerene (TPPS/C60 ) is successfully constructed. The theoretical spectral efficiency of TPPS/C60 is as high as 70%, offering the possibility of full-solar-spectrum light harvesting. The TPPS/C60 performs a highly efficient photocatalytic H2 evolution rate of 276.55 µmol h-1 (34.57 mmol g-1 h-1 ), surpassing many reported organic photocatalysts. The D-A structure effectively promotes electron transfer from TPPS to C60 , which is beneficial to the photocatalytic reaction. Specifically, a giant internal electric field in the D-A structure is built via the enhanced molecular dipole, which dramatically promotes the charge separation (CS) efficiency by 2.35 times. Transient absorption spectra results show a long-lived CS state TPPS•+ -C60 •- in the D-A structure, which effectively promotes participation of photogenerated electrons in the reduction reaction. Briefly, this work provides a novel approach for designing high-performance photocatalytic materials via enhancing the interfacial electric field.

A Full-Spectrum Porphyrin-Fullerene D-A Supramolecular Photocatalyst with Giant Built-In Electric Field for Efficient Hydrogen Production.

This review article summarizes recent progress in the fabrication methodologies and functional modulations of nanoparticle (NP)–polymer composites. On the basis of the techniques of NP synthesis and surface modification, the fabrication methods of nanocomposites are highlighted; these include surface-initiated polymerization on NPs, in situ formation of NPs in polymer media, and the incorporation through covalent linkages and supramolecular assemblies. In these examples, polymers are foremost hypothesized as inert hosts that stabilize and integrate the functionalities of NPs, thus improving the macroscopic performance of NPs. Furthermore, due to the unique physicochemical properties of polymers, polymer chains are also dynamic under heating, swelling, and stretching. This creates an opportunity for modulating NP functionalities within the preformed nanocomposites, which will undoubtedly promote the developments of optoelectronic devices, optical materials, and intelligent materials.

Structural Fabrication and Functional Modulation of Nanoparticle–Polymer Composites

Charge separation efficiency of photocatalysts is still the key scientific issue for solar‐to‐chemical energy conversion. In this work, an electron donor–acceptor (D‐A) interface with high charge separation between TPPS (tetra(4‐sulfonatophenyl)porphyrin) and PDI (perylene diimide) is successfully constructed for boosting photocatalytic H2 evolution. The TPPS/PDI with D‐A interface shows excellent photocatalytic H2 evolution rate of 546.54 µmol h–1 (30.36 mmol h–1 g–1), which is 9.95 and 9.41 times higher than that of pure TPPS and PDI, respectively. The TPPS/PDI has a markedly stronger internal electric field, which is respectively 3.76 and 3.01 times higher than that of pure PDI and TPPS. The D‐A interface with giant internal electric field efficiently facilitates charge separation and urges TPPS/PDI to have a longer excited state lifetime than single component. The work provides entirely new ideas for designing materials with D‐A interface to realize high photocatalytic activity.

Electron Donor–Acceptor Interface of TPPS/PDI Boosting Charge Transfer for Efficient Photocatalytic Hydrogen Evolution

A series of well-defined amphiphilic di- and triblock copolymers have been synthesized, using atom transfer radical polymerization, with poly(ethylene glycol) (PEG) and poly(methacrylisobutyl polyhedral oligomeric silsesquioxane) P(MA-POSS) as the hydrophilic and hydrophobic blocks, respectively The detailed self-assembly behavior of the amphiphilic macromolecules in aqueous media was studied using both static and dynamic light scattering (SLS and DLS) techniques The evolution of block copolymer micelle formation in THF/water mixture (20/80 v/v) was monitored as the THF evaporated from the solvent mixture Initially the block copolymer chains existed as unimers in solution, followed by the formation of smaller aggregates (Rh < 2 nm) after 30 min, eventually growing in size to reach an equilibrium size when all the THF evaporated within 24 h The micelles formed by the block copolymers were found to be kinetically unstable (not frozen); ie, they tended to revert to individual copolymer chains on diluti

Micelle formation and gelation of (PEG-P(MA-POSS)) amphiphilic block copolymers via associative hydrophobic effects.

Reverse micelles of star-block copolymer as nanoreactors for preparation of gold nanoparticles

Complex micelles were obtained from PS-b-PNIPAM-b-PAA micelles and PEG-b-P4VP block copolymers via the strong electrostatic interaction and hydrogen bonding between PAA and P4VP blocks in water. The PS block formed the core and the PAA/P4VP complex shell functioned as a semi-permeable membrane which could control the permeation of small molecules. Between the core and shell, the large fluid-filled space that was formed with the thermoresponsive PNIPAM gel could retain the loaded drug for a long period of time. With increasing temperature, the shrinkage of the PNIPAM coils pumped the drug out of the complex micelles. The complex micelles functioned as a contractive "nanopump", which could potentially be applied as a thermosensitive controlled release system.

/pdf/contractive-polymeric-complex-micelles-as-thermo-sensitive-2x9ktm508h.pdf

Contractive Polymeric Complex Micelles as Thermo‐Sensitive Nanopumps

A chiral polymeric micelle is described, formed from the self-assembly of TPPS and PEG 114 -b-P(4VP) 38 in aqueous media based on their electrostatic interaction. The self-assembly behavior is studied by DLS, SLS, TEM, UV-vis absorption spectroscopy, and CD spectroscopy. The experimental results indicate that the resultant hybrid spherical micelles with a hybrid P(4VP)/TPPS core and a PEG shell show chiral signatures. In addition, the chiral micelles have a large dimension and biphasic segregated structure because of the formation of H-aggregates and J-aggregates in the micellar core.

Chiral Polymeric Micelles From Electrostatic Assembly Between Achiral Porphyrins and Block Copolymers

We report a simple procedure to prepare a novel Au-micelle composite with a core-shell-corona structure. This composite is prepared by reduction of tetrachloroauric acid (HAuCl 4 ·3H 2 O) in dilute aqueous solution containing polystyrene-block-poly(4-vinylpyridine) micelles and poly(ethylene oxide)-block-poly(4-vinylpyridine) copolymers. The micelles with a polystyrene core and a poly(4-vinylpyridine) shell are transformed into Au-micelle composites with a polystyrene core, a swollen hybrid Au/poly(4-vinylpyridine) inner shell, and a poly(ethylene oxide) corona by direct physisorption of gold particles with poly(4-vinylpyridine) chains.

Novel Structured Composites Formed from Gold Nanoparticles and Diblock Copolymers

https://pubs.acs.org/doi/pdf/10.1021/bm9010408

Reply to Comment on J- and H-Aggregates of 5,10,15,20-Tetrakis-(4-sulfonatophenyl)-porphyrin and Interconversion in PEG-b-P4VP Micelles

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