Functionalization of biomaterials with biologically active peptides can improve their performance after implantation. By genetic fusion to self-assembling proteins, the functional peptides can easily be presented on different physical formats. Herein, a chemical-free coating method based on self-assembly of the recombinant spider silk protein 4RepCT is described and used to prepare functional coatings on various biomaterial surfaces. The silk assembly was studied in real-time, revealing the occurrence of continuous assembly of silk proteins onto surfaces and the formation of nanofibrillar structures. The adsorbed amounts and viscoelastic properties were evaluated, and the coatings were shown to be stable against wash with hydrogen chloride, sodium hydroxide, and ethanol. Titanium, stainless steel, and hydroxyapatite were coated with silk fused to an antimicrobial peptide or a motif from fibronectin. Human primary cells cultured on the functional silk coatings show good cell viability and proliferation, implying the potential to improve implant performance and acceptance by the body.
Synthetic imidazole ligands are typically substituted at the N(1) ((1)-Im) position while natural imidazole ligands are substituted at the C(4) ((4)-Im) position. To outline the difference in coordination properties, the methyl-substituted imidazoles Me(4)-Im and Me(1)-Im were complexed with CuCl(2) and ZnCl(2) and investigated by NMR relaxometry, electron paramagnetic resonance, far-Fourier transform IR vibrational spectroscopy, and ab initio calculations. Me(4)-Im, Me(1)-Im, and Im in excess form the usual tetragonal D(4h) [CuL(4)X(2)] complexes with CuCl(2) whereas the methylated imidazoles form pseudotetrahedral C(2v) complexes instead of the usual octahedral O(h) [ZnIm(6)](2+) complex. All imidazoles display a high degree of covalence in the M-L σ- and π-bonds and the π-interaction strength affects the relative energies of complexation. Opportunities to tailor complexes by the chemical properties of the substituents are envisaged due to the role of the inductive and hyperconjugative effects, rather than position.
The adsorption behavior of ethyl(hydroxyethyl) cellulose EHEC and hydrophobically modified EHEC (HM-EHEC) at hydrophilic and hydrophobic surfaces has been studied using surface plasmon resonance (SPR) and quartz crystal microbalance with dissipation monitoring (QCM-D) methods. The adsorbed amounts measured with the different methods were different due to large amounts of water in the films. The slow adsorption process made it reasonable to assume a continuous polymer reconfiguration process at the surface. This was mostly seen for HM-EHEC at the hydrophobic surface, where a more flexible structure was adopted during the adsorption process. A cross-linking agent was seen to truly interpolymer cross-link EHEC at the hydrophilic surface and HM-EHEC at the hydrophobic surface. For EHEC at a hydrophobic surface and for HM-EHEC at a hydrophilic surface, the polymers adsorbed in an individually phase-separated manner, making an interpolymer cross-linking reaction unsuccessful.
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