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Relevant academic research and scientific papers

Adhesive RAFT agents for controlled polymerization of acrylamide: Effect of catechol-end R groups

Synthesizing polyacrylamide (PAM) inorganic nanocomposites with stable tethering and controlled polymer length has been elusive. Herein, we report on the synthesis of trithiocarbonates with several catechol end R groups (as anchors) that differ in their carbonyl α-substituents. These so-called adhesive RAFT agents were subsequently examined in batch RAFT polymerization of the acrylamide (AM) monomer to study their living characteristics. The catechol-end trithocarbonates (Dopa-CTAs) and catechol-end PAM structures (≤46 kDa) were confirmed via 1D (1H and 13C) and 2D (gHSQC, gHMBC) NMR. Subsequent anchoring of the end-functionalized PAM (grafting to) via catechol induced linkage to γ-alumina nanoparticles was successful, giving good correlation based on ATR-FTIR, DLS and TGA analyses. This unique methodology enables PAM-inorganic nanocomposites to be synthesized with stable tethering without significant rate retardation.

Siderophore-inspired nanoparticle-based biosensor for the selective detection of Fe3+

Inspired by nature's exploitation of the 1,2-dihydroxybenzene unit (or catechol) in mammalian and bacterial siderophores, we report the first example of a nanoparticle sensing system that utilises the strong catechol-Fe3+ binding motif to trigger nanoparticle aggregation, promoting a powerful optical response. Gold nanoparticles are functionalised with RAFT polymerisation-prepared water-soluble poly(N-hydroxyethyl acrylamide) containing a catechol moiety at the α-chain-end. A strong red-to-purple colorimetric response occurs in the presence of Fe3+ at serum concentrations (8-25 μM) in saline solution. Sodium chloride is critical in generating a strong optical output, as is the length of polymer used to coat the AuNPs. This behaviour is also demonstrated to be selective for Fe3+ over a host of other biologically relevant ions.

Highly Ordered Nanoporous Films from Supramolecular Diblock Copolymers with Hydrogen-Bonding Junctions

We designed efficient precursors that combine complementary associative groups with exceptional binding affinities and thiocarbonylthio moieties enabling precise RAFT polymerization. Well defined PS and PMMA supramolecular polymers with molecular weights up to 30 kg mol?1are synthesized and shown to form highly stable supramolecular diblock copolymers (BCPs) when mixed, in non-polar solvents or in the bulk. Hierarchical self-assembly of such supramolecular BCPs by thermal annealing affords morphologies with excellent lateral order, comparable to features expected from covalent diblock copolymer analogues. Simple washing of the resulting materials with protic solvents disrupts the supramolecular association and selectively dissolves one polymer, affording a straightforward process for preparing well-ordered nanoporous materials without resorting to crosslinking or invasive chemical degradations.

Synthesis of magnetic microporous organic nanotube networks for adsorption application

In this work, we report a novel synthesis of magnetic microporous organic nanotube networks (Fe3O4-MONNs) by an in situ hyper-cross-linking reaction between magnetic nanoparticles and core-shell bottlebrush copolymers. The resulting Fe3O4-MONNs magnetic hybrid materials display a hierarchically porous structure with nanotube morphology, large surface area (648 m2 g-1) and uniform mesochannels (～4 nm). Due to abundant anionic carboxylate groups produced as end-groups after polylactide (PLA) core degradation in the bottlebrush copolymers, the Fe3O4-MONNs showed a selective adsorption behavior for the cationic dyes. Moreover, the Fe3O4-MONNs possess superparamagnetism and high saturation magnetization (19.8 emu g-1), which allows them to be easily separated by an external magnetic field and subsequently reused. Therefore, this work provides a promising method for the design and synthesis of magnetic microporous organic nanotube networks, which can be used for the practical separation of organic dyes, as well as having other potential applications in the fields of absorption, fast separation and heterogeneous catalysis.

PH-responsive amphiphilic block copolymer prodrug conjugated near infrared fluorescence probe

A novel amphiphilic multi-block copolymer conjugated with both a near infrared fluorescence probe and drug has been designed and prepared by means of ring-opening polymerization (ROP) of N-Carboxy Anhydride (NCA) monomers following a Reversible Addition-F