Abstract
Carbon materials and nanomaterials are of great interest for biological applications such as implantable devices and nanoparticle vectors, however, to realize their potential it is critical to control formation and composition of the protein corona in biological media. In this work, protein adsorption studies were carried out at carbon surfaces functionalized with aryldiazonium layers bearing mono- and di-saccharide glycosides. Surface IR reflectance absorption spectroscopy and quartz crystal microbalance were used to study adsorption of albumin, lysozyme and fibrinogen. Protein adsorption was found to decrease by 30–90% with respect to bare carbon surfaces; notably, enhanced rejection was observed in the case of the tested di-saccharide vs. simple mono-saccharides for near-physiological protein concentration values. ζ-potential measurements revealed that aryldiazonium chemistry results in the immobilization of phenylglycosides without a change in surface charge density, which is known to be important for protein adsorption. Multisolvent contact angle measurements were used to calculate surface free energy and acid-base polar components of bare and modified surfaces based on the van Oss-Chaudhury-Good model: results indicate that protein resistance in these phenylglycoside layers correlates positively with wetting behavior and Lewis basicity.
Highlights
Various forms of carbon find multiple applications as biomaterials; coatings such as pyrocarbon and amorphous carbons (e.g. Amorphous carbon (a-C), a-C:Si, a-C:H, ta-C)[6,7], are promising for biomedical applications because of their frictional and mechanical properties, their corrosion resistance and chemical inertness, and their bio- and hemocompatibility
We have recently shown that immobilized phenylglycosides bearing mono-saccharide groups obtained via aryldiazonium chemistry can reduce the unspecific adsorption of Bovine Serum Albumin (BSA) at carbon surfaces[27]
Amorphous carbon (a-C) films used in our experiments were deposited via magnetron sputtering
Summary
Various forms of carbon find multiple applications as biomaterials; coatings such as pyrocarbon and amorphous carbons (e.g. a-C, a-C:Si, a-C:H, ta-C)[6,7], are promising for biomedical applications because of their frictional and mechanical properties, their corrosion resistance and chemical inertness, and their bio- and hemocompatibility. Aryldiazonium chemistry offers a versatile route for surface immobilization with key advantages for carbon applications: (a) functionalization can be carried out from solution, (b) it occurs under mild conditions without the use of multistep reactions, and (c) it leads to the formation of robust functional layers via formation of strong C—C covalent bonds between R-Ph groups and carbon substrates[28] This is a desirable property that imparts chemical and thermal stability to carbohydrate adlayers under a variety of conditions preventing interfacial exchange between the layer and biomolecules in solution. We have recently shown that immobilized phenylglycosides bearing mono-saccharide groups obtained via aryldiazonium chemistry can reduce the unspecific adsorption of Bovine Serum Albumin (BSA) at carbon surfaces[27] It remains unclear whether antifouling properties can be observed with other proteins and whether specific carbohydrate structural properties are responsible for the antifouling behavior. We investigate the relationship between protein adsorption at phenylglycoside layers and surface free energy, charge and glycoside structure with the aim of improving our current understanding of key properties that result in antifouling activity of aryldiazonium carbohydrate layers
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