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Eingeladener Vortrag
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Artificial weathering of LDPE under dry conditions (<10% of relative humidity) by UV radiation was monitored
by dielectric spectroscopy. For an apolar polymer like LDPE, dielectric study yields information
about the change in structure and dynamics of the system. The fluctuations of the polar groups which
are generated as a result of photooxidation such as carbonyl groups can be monitored as characteristic
relaxation processes like the αc or β mode. The dielectric loss characterized by typical dielectric parameters
like the activation energy and dielectric strength are strongly dependent upon changes induced
by photooxidation in the amorphous and crystalline domains. This paper discusses in detail how the foil
reached its mechanical disintegration. It was found that initial stages of weathering induce chain scission
and/or crosslinking in the amorphous domains of the polymer and the motional processes in the crystalline
regions are not affected. After this induction period, an increase in the degree of crystallization was
observed by employing differential calorimetry. The increasing crystallinity is considered as one of the
reasons for embrittlement which finally leads to the complete loss of the structural integrity.
A new concept for molecular interface design in metal-polymer systems is presented. The main features of this concept are the replacement of weak physical interactions by strong covalent bonds, the flexibilization of the interface for compensating different thermal expansions of materials by using long-chain flexible and covalently bonded spacers between the metal and the polymer as well as its design as a moisture-repellent structure for hindering diffusion of water molecules into the interface and hydrolysis of chemical bonds.
For this purpose, the main task was to develop plasmachemical and chemical techniques for equipping polymer surfaces with monotype functional groups of adjustable concentration. The establishing of monotype functional groups allows grafting the functional groups by spacer molecules by applying usual wet-chemical reactions. Four processes were favoured for production of monotype functional groups by highly selective reactions: the plasma bromination, the plasma deposition of plasma polymers, the post-plasma chemical reduction of O-functionalities to OH-groups, and the chemical replacement of bromine groups by NH2-groups. The grafting of flexible organic molecules as spacers between the metal layer and polymer improved the peel strength of the metal. To obtain maximal peel strength of aluminium coatings to polypropylene films and occurrence of cohesive failure in the polypropylene substrate, about 27 OH groups per 100 C-atoms or 6 COOH groups per 100 C-atoms were needed. Introducing C6-11-aliphatic spacers 1 OH or COOH group per 100 C-atoms contributed about 60% of the maximal peel strength of the Al-PP system, i.e. 2 or 3 spacer molecules per 100 C-atoms were sufficient for maximal peel strength.
The peel strength of aluminium to polypropylene and poly(tetrafluoroethylene) was determined in dependence on the type and the concentration of functional groups on the polymer surface. For this purpose the polymer surface was equipped with monotype functional groups. The first method to produce monotype functionalized surfaces was an introduction of O functional groups using an oxygen plasma treatment and converting these groups to OH groups applying a wet chemical reduction. In result of this two-step treatment the hydroxyl group concentration at the polymer surface could be increased from 34 to 1014 OH groups/100 C atoms. The second method consists in the deposition of a 150 nm adhesion-promoting layer of plasmapolymers or copolymers onto the polymer surface using the pulsed plasma technique. For that purpose functional groups carrying monomers as allyl alcohol, allylamine and acrylic acid were used. Applying the plasma-initiated copolymerization and using neutral monomers like ethylene or butadiene the concentration of the functional groups was varied.
A correlation of peel strength with the ability of forming chemical interactions between Al atoms and functional groups was found: COOH > OH >> NH2 > H(CH2CH2).