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CH-? Interaction Driven Macroscopic Property Transition on Smart Polymer Surface.

ABSTRACT: Life systems have evolved to utilize weak noncovalent interactions, particularly CH-? interaction, to achieve various biofunctions, for example cellular communication, immune response, and protein folding. However, for artificial materials, it remains a great challenge to recognize such weak interaction, further transform it into tunable macroscopic properties and realize special functions. Here we integrate monosaccharide-based CH-? receptor capable of recognizing aromatic peptides into a smart polymer with three-component "Recognition-Mediating-Function" design, and report the CH-? interaction driven surface property switching on smart polymer film, including wettability, adhesion, viscoelasticity and stiffness. Detailed studies indicate that, the CH-? interaction induces the complexation between saccharide unit and aromatic peptide, which breaks the initial amphiphilic balance of the polymer network, resulting in contraction-swelling conformational transition for polymer chains and subsequent dramatic switching in surface properties. This work not only presents a new approach to control the surface property of materials, but also points to a broader research prospect on CH-? interaction at a macroscopic level.

SUBMITTER: Li M

PROVIDER: S-EPMC4625179 | biostudies-literature | 2015 Oct

REPOSITORIES: biostudies-literature

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CH-π Interaction Driven Macroscopic Property Transition on Smart Polymer Surface.

Li Minmin M Qing Guangyan G Xiong Yuting Y Lai Yuekun Y Sun Taolei T

Scientific reports 20151029

Life systems have evolved to utilize weak noncovalent interactions, particularly CH-π interaction, to achieve various biofunctions, for example cellular communication, immune response, and protein folding. However, for artificial materials, it remains a great challenge to recognize such weak interaction, further transform it into tunable macroscopic properties and realize special functions. Here we integrate monosaccharide-based CH-π receptor capable of recognizing aromatic peptides into a smart ...[more]

PMID: 26510671

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Project description:Advances in supramolecular assembly have enabled the design and synthesis of functional materials with well-defined structures across multiple length scales. Biopolymer-synthetic hybrid materials can assemble into supramolecular structures with a broad range of structural and functional diversity through precisely controlled noncovalent interactions between subunits. Despite recent progress, there is a need to understand the mechanisms underlying the assembly of biohybrid/synthetic molecular building blocks, which ultimately control the emergent properties of hierarchical assemblies. In this work, we study the concentration-driven self-assembly and gelation of π-conjugated synthetic oligopeptides containing different π-conjugated cores (quaterthiophene and perylene diimide) using a combination of particle tracking microrheology, confocal fluorescence microscopy, optical spectroscopy, and electron microscopy. Our results show that π-conjugated oligopeptides self-assemble into β-sheet-rich fiber-like structures at neutral pH, even in the absence of electrostatic screening of charged residues. A critical fiber formation concentration cfiber and a critical gel concentration cgel are determined for fiber-forming π-conjugated oligopeptides, and the linear viscoelastic moduli (storage modulus G' and loss modulus G″) are determined across a wide range of peptide concentrations. These results suggest that the underlying chemical structure of the synthetic π-conjugated cores greatly influences the self-assembly process, such that oligopeptides appended to π-conjugated cores with greater torsional flexibility tend to form more robust fibers upon increasing peptide concentration compared to oligopeptides with sterically constrained cores. Overall, our work focuses on the molecular assembly of π-conjugated oligopeptides driven by concentration, which is controlled by a combination of enthalpic and entropic interactions between oligopeptide subunits.

Project description:This paper reports a series of photopolymerizable polysiloxane-modified nanogels for regulating surface microstructure and gradient property of polymers, which were synthesized by solution polymerization under different feed ratios of a methacrylate-modified polysiloxane, urethane dimethacrylate (UDMA) and isobornyl methacrylate (IBMA) in the presence of a thiol chain transfer agent. The nanogel structure and composition were characterized by proton nuclear magnetic resonance (1H-NMR), Fourier transform-infrared spectroscopy (FT-IR), transmission electron microscope (TEM), gel permeation chromatography (GPC) and differential scanning calorimetry (DSC). The dispersion of these nanogels in triethylene glycol dimethacrylate (TEGDMA) can reduce the onset and magnitude of shrinkage stress during polymerization without compromise to mechanical properties of the resulting polymers. Most importantly, as demonstrated by elemental analysis and X-ray photoelectron spectroscopy (XPS), the nanogels exhibit good self-floating ability in the monomer/polymer matrix and the increase of polysiloxane content in the nanogel can enhance the self-floating capability due to the lower surface tension and energy associated with the polysiloxane component. As a result, the polysiloxane-modified nanogels can spontaneously form a concentration gradient that can be locked in upon photopolymerization leading to a well-controlled heterogeneous polymer that presents a gradient change in thermal stability. With the increase of polysiloxane content, the thermal stability of the polymer was improved significantly. Furthermore, the enrichment of the nanogel on the surface resulting from the good self-floating ability can reduce the dispersion surface energy of gradient polymer film and generate a more hydrophobic surface with altered surface microstructure. These photopolymerizable polysiloxane-modified nanogels are demonstrated to have potential broad application in the preparation of gradient polymer with controlled surface properties.

Dataset Information

CH-? Interaction Driven Macroscopic Property Transition on Smart Polymer Surface.

Publications

CH-π Interaction Driven Macroscopic Property Transition on Smart Polymer Surface.

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