This paper discusses approaches and methods for obtaining highly filled polymer-ceramic materials to be used for additive manufacturing purposes. The key deliverable produced in the course of the project work was the development of polymer-ceramic materials that are suitable for extrusion processing and subsequent manufacture of products via Fused Deposition Modeling (FDM).

Three-dimensional printing of composites reinforced by continuous fiber and based on heat-resistant materials requires a prepreg compatible with these plastics. This kind of a prepreg, in its turn, would necessarily have to be similar to these plastics in terms of its chemistry and operational thermal range. This work was an investigation of factors relevant for the strength of adhesion between carbon fiber and polymeric binder. The authors managed to develop the compounds (coupling agents) facilitating fiber impregnation with polymer and improving fiberbinder adhesion. To obtain a thermoplastic binder various polyimide matrices have been synthesized. The properties of polymers thus created were studied as per the methods of thermogravimetric analysis (TGA) and Differential Scanning Calorimetry (DSC), as well as measurement of limiting wetting angle. Then these materials were subject to solution impregnation so as to obtain prepreg samples suitable for 3D printing. Impregnation quality of these samples was studied by means of scanning electronic microscopy. The most promising prepreg samples were used for 3D printing of try-out product specimens. Composites based on the plastics reinforced by continuous fibers (glass, carbon, polymeric, etc.) are widely used in special fields of today’s technology [1–4]. They have already become indispensable for rocketry or aircraft industries, and they are steadily gaining ground in other industries, too, like machine engineering, shipbuilding, civil engineering, etc. Polymeric composite have become so popular because they are quite strong [5, 6] and light [7] at the same time. Today, manufacturing of fiber-reinforced composites is quite tedious and only allows a limited scope of geometries for final products [8] because fiber impregnation with viscous solutions/melts of polymers is a difficult process. Besides, final product takes time to harden, so until it happens it needs a moulding cast or skeleton to maintain its shape. This tedious process of product manufacturing from the parts reinforced with continuous fiber might proceed much easier and with greater automation thanks to 3D printing as per fused deposition modeling (FDM) technique that uses a filament of preimpregnated fiber [9]. In particular, one of the techniques steadily improving today is 3D printing with continuous carbon fiber and prepregs based on epoxy binders. Final products manufactured as per this technology and reinforced by continuous carbon fiber feature stable size and complex shape. However, prepregs based on epoxy resins will work only with the materials that have good adhesion with them, otherwise final composites will be too weak. Current materials can only be used for the products with low operational temperatures whereas hi-tech applications require strong and heat-resistant materials. To meet this requirement, it is necessary to develop prepregs based on heat-resistant compounds, as well as filaments based on heat-resistant plastics compatible with these prepregs. Polyimides as a class of compounds have long been known to remain stable at high temperatures. Therefore, prepregs based on them, as well as polyimide matrices fit for FDM 3D printing technique will pave way to the products simultaneously featuring high thermal resistance and good strength. The purpose of this work was to develop prepregs based on carbon fiber and polyimides featuring good resistance to high temperatures and aggressive media, as well as to develop thermoplastic polyimide matrices fit for 3D printing.

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This paper describes the production of carbon fiber / high-performance polyimide prepregs and the study of prepreg samples quality by scanning electron microscopy, atomic-force electron microscopy and scanning ion-conductance microscopy. The prepreg samples were produced using a laboratory-designed setup by impregnation of carbon fiber with a polyimide solution. The study of the prepreg structure made it possible to establish the connection between polymer matrix composition and quality of carbon fiber impregnation. Thus, the study shows that the polymer matrix composition containing aliphatic fragment and quaternary carbon atom produces the best performance prepreg suitable for FDM 3D printing.