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• W2891027357 abstract "The development of supramolecular chemistry and the toolbox of the non-covalent bond to assemble discrete host-guest complexes have long been surpassed by the preparation of much larger polymer chains and 2D layers, and more complex 3D networks. The utilization of highly directional supramolecular forces can thus direct the formation and self-assembly into supramolecular polymers in solution and the bulk state. The reversible nature of the monomer-to-polymer transitions provides exciting opportunities to interrogate the mechanistic aspects of supramolecular polymerization, with respect to thermodynamic and kinetic parameters, as well as opportunities in various areas of research that exploit the mechanical, electronic, or biological function of this dynamic and adaptive class of materials. The idea for this thematic special issue on Structure to Function in Supramolecular Polymers and Materials was borne at a recent ACS POLY session organized in San Francisco in 2017. The issue assembles 11 selected contributions, including 9 communications and 2 review articles. Recent advances in the fundamental understanding of non-covalent interactions and supramolecular polymerization mechanisms are highlighted, and the collection of contributions demonstrates the many exciting features of supramolecular polymers in solution and in the bulk, with applications in self-healing, optoelectronic, and biomedical materials, among others. Wolfgang Binder and co-workers discuss the fundamental aspects and the current status of self-healing in supramolecular polymers (DOI: 10.1002/marc.201700739). The authors highlight some basic physicochemical aspects of supramolecular interactions and polymer networks, and discuss the impact of adhesion, phase segregation, as well as kinetics on self-healable supramolecular materials. The authors further differentiate the thermodynamic and kinetic parameters of the healing processes for swollen supramolecular gels and bulk supramolecular polymers. The discussed examples are classified according to the type of non-covalent interactions (hydrogen bonding, ionic interactions, π–π stacking, metal coordination) that form the basis for the supramolecular “sticky” groups responsible for the healing and restructuring process in a damaged synthetic polymer, and the mechanical and rheological properties of a range of bulk materials are presented. Hager, Schubert, and co-workers report an example of self-healing supramolecular polymer networks in the solid state using imidazole functionalised polymethacrylate copolymers that are crosslinked upon coordination with zinc(II) (DOI: 10.1002/marc.201700742). The incorporation of functional side groups was achieved using ring-opening of the polymerized vinyldimethylazlactone comonomer with protected histidine and aspartic acid, allowing for modification of the ratio of imidazole to carboxylic acid ligands for metal coordination in the final copolymers. Their healing kinetics and mechanical properties could thereby be tuned, as investigated by scratch tests and nanoindentation experiments. Fernández, Sánchez, and coworkers report the cooperative supramolecular polymerization of hydrophobic bispyridyldichlorido Pd(II) complexes in solution (DOI: 10.1002/marc.201800191). The pyridyl ligands are equipped with an extended π-surface of oligo(phenylene ethynylene), as well as amide functional groups. The molecular organization of the metallosupramolecular polymers was characterised as a slipped arrangement of the monomer subunits, supported by π–π stacking and N–H···Cl–Pd(II) interactions, and showed a strong tendency to bundle into fibrillar structures. An area of research intensively investigated with respect to the use of weak non-covalent forces in supramolecular materials is self-assembled swollen networks based on low-molecular-weight gelators (LMWGs). Draper, Adams, and co-workers disclose hydrogelators that are based on hydrophobic terthiophene, tetrathiafulvalene, and oligo(phenylene vinylene) p-type π-conjugates equipped with diphenylalanine (DOI: 10.1002/marc.201700746). The free carboxylic acids were utilized to regulate the assemblies into fibre network morphologies using pH protocols, and the conductivity of the resulting hydrogels as well as dried xerogels were characterised. In a collaborative effort, Dankers and co-workers report the use of a pH-responsive supramolecular hydrogel based on ureido-pyrimidinone (UPy)–polyethylene glycol (PEG) amphiphiles as a macroscale drug delivery system (DOI: 10.1002/marc.201800007). The hydrophilic chemotherapeutic agent mitomycin C was conjugated with cholesterol via its aziridine functionality, and the hydrophobic conjugate was able to bind to the hydrophobic compartments in the UPy hydrogel formulation. In vitro experiments showed the sustained release of the modified drug conjugate. Barnes and co-workers describe covalent PEG hydrogels connected using octameric viologen units (DOI: 10.1002/marc.201700781). Using Ru(bpy)32+ as a visible-light-absorbing photoredox catalyst, the viologen units were reduced and the radical cations were able to interact due to reduced electrostatic repulsion. This enabled a contraction and thus actuation of the hydrogel network via reversible redox (photo)chemistry. Gröhn and co-workers report supramolecular nanostructures that respond to light irradiation (DOI: 10.1002/marc.201700860). Using the electrostatic self-assembly of linear cationic polyelectrolytes with anionic azodyes in aqueous solution, micrometer-long cylindrical nanostructures were obtained and converted into smaller ellipsoidal objects upon irradiation with UV light, as determined by light scattering and small-angle neutron scattering (SANS). Lanier and Bermudez utilize DNA as a building block to prepare supramolecular assemblies in water (DOI: 10.1002/marc.201800342). Using a hybridization chain reaction (HCR) route, linear supramolecular polymers of DNA are produced through a cascade of strand-displacement reactions. The authors show that a supramolecular living polymerization is operative, with molecular weights adjusted by the ratio of monomer to initiator. In contrast to the polyaddition-like process of concatemerization, HCR leads to polymers with narrower dispersity values. In a collaborative effort, Besenius and co-workers report the preparation of ABA and ABA′ triblock polyethylene glycol- and polysarcosine-peptide conjugates (DOI: 10.1002/marc.201800459). The pH-switchable, β-sheet-encoded peptides promote the folding and intermolecular self-assembly of the conjugates into core–shell nanorods in water, whereas only the parallel β-sheet-driven folding leads to interstrand crosslinking and hydrogelation. The authors point out that subtle differences in the design of supramolecular interactions has large consequences on the hierarchical structure formation at the nano- and mesoscopic level. Fink and Zha review silk as high-performance biological material (DOI: 10.1002/marc.201700834). The authors describe theories on the in vivo production and self-assembly of silk, its hierarchical structure, and supramolecular assembly, and discuss similarities with synthetic supramolecular systems, such as block copolymers, liquid crystals, thermoplastic elastomers, and self-assembling peptides. The authors focus on the relationship between chemical structure, nanoscale molecular organization, and material properties of silk and silk-like supramolecular materials. In their contribution, Voets and co-workers investigate the ice recrystallization inhibition activity of poly(vinyl alcohol) (PVA) containing micellar structures (DOI: 10.1002/marc.201700814). The complex coacervate core micelles were obtained by co-assembly of a cationic poly(4-vinyl-N-methylpyridinium iodide) homopolymer with a PVA-block-poly(acrylic acid) anionic block copolymer and investigated with light scattering. The authors report ice recrystallization inhibition concentrations of the complex coacervate core micelles, which are similar to linear PVA and PVA bottlebrush polymers. We would like to thank all the contributing authors of this special issue on supramolecular polymers in Macromolecular Rapid Communications. We also would like to thank Editor-in-Chief Kirsten Severing and Deputy Editor David Huesmann not only for the invitation but also for their patience while assembling the special issue. We view this collection of Communications and Reviews as an opportunity to highlight some of the most recent discoveries and achievements in the field. We hope that they will serve as an inspiration to many readers working at the interface of synthetic organic and polymer chemistry within the materials sciences, in order to pave the way for future research directions in the rapidly growing area of functional supramolecular materials." @default.
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• W2891027357 title "Structure to Function in Supramolecular Polymers and Materials" @default.
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