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Additive manufacturing (AM) of aerogels increases the achievable geometric complexity, and affords fabrication of hierarchically porous structures. In this work, a custom heated material extrusion (MEX) device prints aerogels of poly(phenylene sulfide) (PPS), an engineering thermoplastic, via in situ thermally induced phase separation (TIPS). First, pre‐prepared solid gel inks are dissolved at high temperatures in the heated extruder barrel to form a homogeneous polymer solution. Solutions are then extruded onto a room‐temperature substrate, where printed roads maintain their bead shape and rapidly solidify via TIPS, thus enabling layer‐wise MEX AM. Printed gels are converted to aerogels via postprocessing solvent exchange and freeze‐drying. This work explores the effect of ink composition on printed aerogel morphology and thermomechanical properties. Scanning electron microscopy micrographs reveal complex hierarchical microstructures that are compositionally dependent. Printed aerogels demonstrate tailorable porosities (50.0–74.8%) and densities (0.345–0.684 g cm⁻³), which align well with cast aerogel analogs. Differential scanning calorimetry thermograms indicate printed aerogels are highly crystalline (≈43%), suggesting that printing does not inhibit the solidification process occurring during TIPS (polymer crystallization). Uniaxial compression testing reveals that compositionally dependent microstructure governs aerogel mechanical behavior, with compressive moduli ranging from 33.0 to 106.5 MPa.

 

Vat photopolymerization (VP) and direct ink write (DIW) additive manufacturing (AM) provide complex geometries with precise spatial control employing a vast array of photo‐reactive polymeric systems. Although VP is recognized for superior resolution and surface finish, DIW provides versatility for higher viscosity systems. However, each AM platform presents specific rheological requirements that are essential for successful 3D printing. First, viscosity requirements constrain VP polymeric materials to viscosities below 10 Pa s. Thus, this requirement presents a challenging paradox that must be overcome to attain the physical performance of high molecular weight polymers while maintaining suitable viscosities for VP polymeric materials. Second, the necessary rheological complexity that is required for DIW pastes requires additional rheological measurements to ensure desirable thixotropic behavior. This manuscript describes the importance of rheological measurements when designing polymeric latexes for AM. Latexes effectively decouple the dependency of viscosity on molecular weight, thus enabling high molecular weight polymers with low viscosities. Photo‐crosslinking of water‐soluble monomers and telechelic oligomeric diacrylates in the presence of the latex enables the fabrication of a scaffold, which is restricted to the continuous aqueous phase and effectively surrounds the latex nanoparticles enabling the printing of otherwise inaccessible high molecular weight polymers. Rheological testing, including both steady and oscillatory shear experiments, provides insights into system properties and provides predictability for successful printing. This perspective article aims to provide an understanding of both chemical functionality (photo‐ and thermal‐reactivity) and rheological response and their importance for the successful design and evaluation of VP and DIW processable latex formulations.

 

Unparalleled temporal and spatial control of colloidal chemical processes introduces immense potential for the manufacturing, modification, and manipulation of latex particles. This review highlights major advances in photochemistry, both as stimulus and response, to generate unprecedented functionality in polymer colloids. Light-based chemical modification generates polymer particles with unique structural complexity, and the incorporation of photoactive functionalities transforms inert particles into photoactive nanodevices. Latex photo-functionality, which is reflected in both the colloidal and coalesced states, enables photochromism, photoswitchable aggregation, tunable fluorescence, photoactivated crosslinking and solidification, and photomechanical actuation. Previous literature explores the capacity of photochemistry, which complements the rheological and processing advantages of latex, to expand beyond traditional coatings applications and enable disruptive technologies in critical areas including nanomedicine, data security, and additive manufacturing. 

Steady-state traveling waves in structures have been previously investigated for a variety of purposes including propulsion of objects and agitation of a surrounding medium. In the field of additive manufacturing, powder bed fusion (PBF) is a commonly used process that uses heat to fuse regions of metallic or polymer powders within a loose bed. PBF processes require post-process removal of loose powder, which can be difficult when blind holes or complex internal geometry are present in the fabricated part. Here, a preliminary investigation of a simple part is conducted examining the use of traveling waves for post-process de-powdering of additively manufactured specimens. The generation of steady-state traveling waves in a structure is accomplished through excitation at a frequency between two adjacent resonant frequencies of the structure, resulting in two-mode excitation. This excitation can be generated by bonded piezoceramic elements actuated by a sinusoidal voltage signal. The response of the structure is affected by the parameters of the excitation, such as the particular frequency of the voltage signal, the placement of the piezoceramic actuators, and the phase difference in the signals applied to different actuators. Careful selection of these parameters allows adjustment of the quality, wavelength, and wave speed of the resulting traveling waves. In this work, open-top rectangular box specimens composed of sintered nylon powder and coated with fine sand are used to represent freshly fabricated parts yet-to-be cleaned of un-sintered powder. Steady-state traveling waves are excited in the specimens while variations in the frequency content and phase differences between actuation points of the excitation are used to affect the characteristics of the dynamic response. The effectiveness of several response types for the purpose of moving un-sintered nylon powder within the specimens is investigated.