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    Impact of graft architecture of PEGylated copolymers assembly on hydroxyapatite in the differential regulation of initial cell and bacterial adhesion

    Year: 2022

    Journal: Appl. Surf. Sci., Volume 606, DEC 30

    Authors: You, Mingyu; Zhang, Lei; Gmuer, Tobias A.; Zhang, Kaihuan; Zuercher, Stefan; Li, Wen; Yuan, Guangyin; Spencer, Nicholas D.; Pei, Jia

    Organizations: National Key Research and Development Program of China [2021YFE0204900, 2021YFC2400701]; SSSTC international cooperation project [EG 18-122016]; Key project of National Natural Science Foundation of China [52130104]

    Keywords: Hydroxyapatite; Self -assembly layer; PEGylated copolymer; Osteoblast adhesion; Antibacterial adhesion

    Synthetic pure hydroxyapatite (HA), though widely investigated as an artificial orthopedic implant material, has neither anti-infection properties nor innate interfacial bioactivity. Ideally, surface modification of this material needs to be developed with simultaneous anti-microbial capacity and superior cytocompatibility. Herein, graft copolymers of a PAA backbone functionalized with a high density of polyethylene glycol (PEG), and varying grafting densities of cyclic Arg-Gly-Asp-d-Phe-Cys peptides (cRGD) end-grafted onto the PEG chains have been designed and synthesized. Systematic study on the grafted anchoring groups first indicates a synergistic binding mechanism of the copolymer to HA surface, involving electrostatic interaction of the protonated amino (-NH3+) with negatively charged HA, assisted with coordination bonding through the nitrodopamine (ND) group. The PEGylated graft copolymers are demonstrated to firmly adsorb to the HA surface as an ultrathin self-assembly layer from a HEPES buffer solution, showing stability with insignificant desorption and effective inhibition of non-specific protein adsorption evaluated by XPS and QCM-D assays. Direct adhesion assays confirm that HA, modified with the density-optimized cRGD/PEG-functionalized graft polymer, can considerably promote osteoblast attachment, while preventing different strains of bacteria adhesion in the initial phase.
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