The interfacial gelation of proteins at metallic surfaces was investigated with an electrochemical quartz crystal microbalance (QCM). When Cr electrodes were corroded in proteinaceous solutions, it was found that gels will form at the Cr surfaces if molybdate ions are also present in the solution. Gelation is reversible and can also be controlled with the electrochemical potential at the electrode. Further, a method was developed to characterize the viscoelastic properties of thin films in liquid media using the QCM as a high-frequency rheometer. By measuring the frequency and dissipation at multiple harmonics of the resonance frequency, the viscoelastic phase angle, density-modulus product, and areal mass of a film can be determined. The method was applied to characterize the protein films, demonstrating that they have a phase angle near 55° and a density-modulus product of ≈10(7) Pa·g/cm(3). Data imply that the gels are composed of a weakly cross-linked proteinaceous network with properties similar to albumin solutions with concentrations in the range of ≈40 wt %.
The corrosion of CoCrMo, an alloy
frequently used in orthopedic
implants, was studied with an electrochemical quartz crystal microbalance
(QCM) in three physiologically relevant solutions. Mass changes were
measured during potentiodynamic tests, showing material deposition
in protein solutions at potential levels that caused mass loss when
the proteins were not present. X-ray photoelectron spectroscopy (XPS)
data indicated that the deposited material was primarily organic and
therefore was most likely derived from proteins in the electrolyte.
Material deposition consistently occurred at a critical potential
and was not dependent on the current density or total charge released
into solution. Corrosion studies on pure Co, Cr, and Mo in protein
solutions found material deposition only on Mo. We hypothesize that
organic deposition results from the interaction of Mo(VI) with proteins
in the surrounding solution. The organic layer is reminiscent of tribochemical
reaction layers that form on the surface of CoCrMo hip bearings, suggesting
that these types of layers can be formed by purely electrochemical
means.
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