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Ultra-high molecular weight polyethylene membranes were modified and subsequently polymer coated using the underwater plasma produced by glow discharge electrolysis. This plasma pretreatment generated various O-functional groups among them OH groups have dominated. This modified inner (pore) surface of membranes showed complete wetting and strong adhesion to a hydrogel copolymerized by glow discharge electrolysis also. The deposited hydrogel consists of plasma polymerized acrylic acid crosslinked by copolymerization with the bifunctional N,N'-methylenebis(acrylamide). Tuning the hydrogel hydrophilicity and bio-compatibility poly(ethylene glycol) was chemically inserted into the copolymer. Such saturated polymer could only be inserted on a non-classic way by (partial) fragmentation and recombination thus demonstrating the exotic properties of the underwater plasma. The modification of membrane was achieved by squeezing the reactive plasma solution into the pores by plasma-induced shock waves and supported by intense stirring. The deposited copolymer hydrogel has filled all pores also in the inner of membrane as shown by scanning electron microscopy of cross-sections. The copolymer shows the characteristic units of acrylic acid and ethylene glycol as demonstrated by infrared spectroscopy. A minimum loss in carboxylic groups of acrylic acid during the plasma polymerization process was confirmed by X-ray photoelectron spectroscopy. Additional cell adhesion tests on copolymer coated polyethylene using IEC-6 cells demonstrated the bio-compatibility of the plasma-deposited hydrogel.
Plasma chemical methods are well suited for introducing functional groups to the surfaces of chemically inert polymers such as polyolefins. However, a broad variety of functional groups are often formed. Unfortunately, for further chemical processing such as grafting of molecules for advanced applications a highly dense monotype functionalized polyolefin surface is needed. Therefore, the main task was to develop a selective surface functionalization process, which formed preferably only a single type of functional groups at the surface in high concentration. Amongst the novel plasma methods, the underwater plasma process (UWP) is one of most attractive options to solve the problem of monotype functionalization. Such plasma is an efficient source of ions, electrons, UV-radiation, high-frequency shock waves, radicals such as hydroxyl radical, and reactive neutral molecules such as hydrogen peroxide. In contrast to established gas phase glow discharge processes, the water phase limits the particle and radiation energies and thus the energy input into the polymer. By virtue of the liquid water environment, which moderates highly energetic plasma species, extensive oxidation, degradation, cross-linking and radical formation on the polymer are more limited as compared to gas plasma exposure. The variety of plasma produced species in the water phase is also much smaller because of the limited reaction possibilities of the plasma with water. The possibility to admix a broad variety of chemical additives makes underwater plasma even more attractive. Hydrogen peroxide and the catalyst (Fe-ZSM5) should influence and increase the equilibrium concentration of OH radicals in the underwater plasma process. It was found that these radicals played a very important role in OH functionalization of polyolefin surfaces. Hydrogen peroxide was identified to be the most prominent precursor for OH group formation in the UWP. The catalyst would affect the steady state of OH radical formation and its reaction with the substrate surface and thus accelerates the functionalization process.