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    Biocompatible Graphene Oxide Nanosheets Densely Functionalized with Biologically Active Molecules for Biosensing Applications

    Year: 2021

    Journal: ACS Appl. Nano Mater., Volume 4, AUG 27, page 8334–8342

    Authors: Lehner, Benjamin A. E.; Benz, Dominik; Moshkalev, Stanislav A.; Meyer, Anne S.; Cotta, Monica A.; Janissen, Richard

    Organizations: Netherlands Organization for Scientific Research (NWO/OCW) [2015SYN08]; FAPESP [2010/18107-8, 2010/51748-7, 2012/51580-4, 2013/02300-1, 2015/16611-4]; CNPq [479486/2012-3, 429326/2018-1]

    Keywords: graphene oxide; poly(ethylene glycol); colamine; APTES; DNA biosensor; surface chemistry; bioconjugation

    Graphene oxide (GO) has immense potential for widespread use in diverse in vitro and in vivo biomedical applications owing to its thermal and chemical resistance, excellent electrical properties and solubility, and high surface-to-volume ratio. However, development of GO-based biological nanocomposites and biosensors has been hampered by its poor intrinsic biocompatibility and difficult covalent biofunctionalization across its lattice. Many studies exploit the strategy of chemically modifying GO by noncovalent and reversible attachment of (bio)molecules or sole covalent biofunctionalization of residual moieties at the lattice edges, resulting in a low coating coverage and a largely bioincompatible composite. Here, we address these problems and present a facile yet powerful method for the covalent biofunctionalization of GO using colamine (CA) and the poly(ethylene glycol) cross-linker that results in a vast improvement in the biomolecular coating density and heterogeneity across the entire GO lattice. We further demonstrate that our biofunctionalized GO with CA as the cross-linker provides superior nonspecific biomolecule adhesion suppression with increased biomarker detection sensitivity in a DNA-biosensing assay compared to the (3-aminopropyl)triethoxysilane cross-linker. Our optimized biofunctionalization method will aid the development of GO-based in situ applications including biosensors, tissue nanocomposites, and drug carriers.
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