Polyethylene is a very common liner material for type IV pressure vessels due to its good toughness and easy processing. The property profile of the polymer can be improved by cross-linking thereby changing the nature of the polymer from thermoplastic toward more elastomeric. For this purpose, polyethylene is modified either chemically, using peroxide or silane, or physically by radiation. In the present work, a cross-linkable polyethylene grade that can be processed by rotational molding was peroxide cross-linked under variation of temperature and time. Subsequently, the material was characterized by differential scanning calorimetry, tensile tests, notched bar impact tests and permeation measurements. Two of the altogether six parameter combinations investigated did not lead to successful cross-linking resulting in very poor toughness. Stiffness, strength and permeation barrier properties, however, were much better than those of the other series due to higher crystallinity. Mechanical, physical and chemical properties changed significantly by successful cross-linking. The impact strength could be improved by a factor of more than 10. At the same time, significant losses in stiffness, strength and permeation barrier properties had to be accepted. Peroxide induced randomly distributed formation of cross-links above the melting point interfered with formation of crystalline regions upon cooling.
Lightweight pressure vessels of type IV for hydrogen storage consist of a thermoplastic inner liner, commonly from polyethylene or polyamide. The liner is the permeation barrier against the compressed gas and must prevent the formation of cracks, also after temperature changes, for example after refueling processes. In the present work high-density polyethylene, cross-linked polyethylene, polyamide 6 and polyamide 12 were characterized by tensile tests, single notch impact tests and permeations measurements before and after a cyclic thermal aging process. The aging only lead to slight changes of mechanical properties due to post-crystallization, but to a significant decrease of permeation properties. This decrease was contributed to weakened, amorphous regions where chain splitting occurred. Considerable differences in properties resulted from different peroxide cross-linking times of polyethylene at the same temperature. A longer holding time at 200 °C led to an improvement in impact strength by a factor of more than three. However, the permeation properties decreased by about 50 %, indicating that peroxide cross-linking in the melt inhibited the formation of crystalline regions.
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