Polyhydroxybutyrate: a review of experimental and simulation studies of the effect of fillers on crystallinity and mechanical properties

Polyhydroxybutyrate (PHB) is a sustainable polymer that is a promising candidate for replacing petroleum-based plastics in food packaging. Fillers are used to improve the mechanical properties of PHB composites, simultaneously changing the crystallinity of the polymer matrix. However, it is not well understood how fillers affect crystallisation and microstructure, and thus the resulting mechanical properties of the composite. This review summarises simulation work on polymer nucleation and crystallisation and how nucleation is influenced by different types of polymer–filler interfaces. Experimental studies of PHB composites with a wide variety of fillers are reviewed to find trends between the filler type, crystallinity and mechanical properties. It is clear that fillers act as nucleants that increase the number of spherulites while reducing spherulite size. This behaviour is apparent for almost all fillers regardless of filler chemistry or topology. However, the data obtained from the literature do not seem to produce strong conclusions about the effect of the degree of crystallinity on the tensile properties of PHB–filler composites, although there are some weak trends that indicate the importance of microstructure. In order to enable prediction and control of PHB composite properties, further systematic studies are required to elucidate the effect of specific filler types and the connection between crystallinity, microstructure and mechanical properties.