Filament-based material extrusion additive manufacturing (MEAM) is one of the most commonly used techniques in additive manufacturing (AM). In spite of recent notable development in the MEAM process, there is still a need to develop more materials that can be printed consistently using this technique. Isotactic polypropylene (PP), a popular thermoplastic material, undergoes rapid crystallization and subsequent volume contraction. This can lead to residual stress buildup in PP parts when processed using MEAM, resulting in poor adhesion to the printing platform, poor geometric tolerance, and mechanical performance. In this work, the effects of varying composition of low molecular weight hydrocarbon resins incorporated to PP are investigated. Specifically, the thermal behavior, crystallization, morphology, and printability of the blends are studied. The rapid crystallization of PP has been delayed by the addition of hydrocarbon resins that provided a larger time window for the residual stresses to relax. The addition of the resins to the pure PP matrix lowers the crystallization temperature of PP from 121.8 to 116.0 °C, which further enables additional diffusion during the solidification process. Polarized optical microscopy demonstrates the differences in crystalline morphology, which is expected to impact the structure at the interlayer boundaries between deposited layers. The combination of modifications in crystallization rate, time, and morphology significantly affects the interlayer adhesion and residual stress state, which directly controls the mechanical properties and part warpage of printed parts. Tensile bars of the different blends were printed in two different orientations to analyze the mechanical performance and study part anisotropy. The maximum tensile stress of pure PP (26.8 ± 2.1 MPa) printed at a ±45° raster angle increased with addition of 20 wt % hydrocarbon resin (32.4 ± 3.0 MPa) when printed under the same conditions. The improvement in the tensile strength is due to a combination of changes in crystallinity, morphology, and improved interlayer adhesion during printing. The parts were annealed postprinting to improve polymer chain diffusion across the layers, thereby improving interlayer adhesion and resulting in tensile modulus and strength values in excess of 90% of injection-molded PP parts.

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As additive manufacturing (AM) expands as a processing technology for structurally customizable materials, there is increasing interest in printing with high particle contents. For suspensions with particle contents of over 50 vol%, there are significant formulation and processing challenges due to increased interparticle friction and suspension complexity. We focus on suspensions with bimodal particle distributions and two common binder systems, a high molecular weight polymer in a solvent that solidifies via solvent evaporation and a monomer mixture that cures via ultraviolet irradiation. We examine the interplay between formulation and processing and show that the formulation effects are particularly important at optimal printing parameters, but that they are overcome by processing-related defects at sub-optimal parameters. By understanding the processing and formulation effects specific to direct ink write AM of high solids suspensions, new customized inks can be designed for a wide range of applications, including construction, energetics, and ceramics.

Additive manufacturing of dense pastes, those with greater than 50 vol% particles, via material extrusion direct ink write is a promising method to produce customized structures for high-performance materials, such as energetic materials and pharmaceuticals, as well as to enable the use of waste or other locally available particles. However, the high volume fraction and the large sizes of the particles for these applications lead to significant challenges in developing inks and processing methods to prepare quality parts. In this prospective, we analyze challenges in managing particle characteristics, stabilizing the suspensions, mixing the particles and binder, and 3D printing the pastes. Graphical abstract