3D printing of polymers is accomplished easily with thermoplastics as the extruded hot melt solidifies rapidly during the printing process. Printing with liquid polymer precursors is more challenging due to their longer curing times. One curable liquid polymer of specific interest is polydimethylsiloxane (PDMS). This study demonstrates a new efficient technique for 3D printing with PDMS by using a capillary suspension ink containing PDMS in the form of both precured microbeads and uncured liquid precursor, dispersed in water as continuous medium. The PDMS microbeads are held together in thixotropic granular paste by capillary attraction induced by the liquid precursor. These capillary suspensions possess high storage moduli and yield stresses that are needed for direct ink writing. They could be 3D printed and cured both in air and under water. The resulting PDMS structures are remarkably elastic, flexible, and extensible. As the ink is made of porous, biocompatible silicone that can be printed directly inside aqueous medium, it can be used in 3D printed biomedical products, or in applications such as direct printing of bioscaffolds on live tissue. This study demonstrates a number of examples using the high softness, elasticity, and resilience of these 3D printed structures.

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Soft intelligent structures that are programmed to reshape and reconfigure under magnetic field can find applications such as in soft robotics and biomedical devices. Here, a new class of smart elastomeric architectures that undergo complex reconfiguration and shape change in applied magnetic fields, while floating on the surface of water, is reported. These magnetoactive soft actuators are fabricated by 3D printing with homocomposite silicone capillary ink. The ultrasoft actuators easily deform by the magnetic force exerted on carbonyl iron particles embedded in the silicone, as well as lateral capillary forces. The tensile and compressive moduli of the actuators are easily determined by their topological design through 3D printing. As a result, their responses can be engineered by the interplay of the intensity of the magnetic field gradient and the programmable moduli. 3D printing allows us to fabricate soft architectures with different actuation modes, such as isotropic/anisotropic contraction and multiple shape changes, as well as functional reconfiguration. Meshes that reconfigure in magnetic fields and respond to external stimuli by reshaping could serve as active tissue scaffolds for cell cultures and soft robots mimicking creatures that live on the surface of water.

The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel with the nanofibrillar SDC network of the same biopolymer results in a remarkable increase of the HHG’s mechanical properties. The viscoelastic HHGs show >3× larger storage modulus and >4× larger Young’s modulus than either constitutive network at the same concentration. Such synergistically enforced colloidal-molecular HHGs open up numerous opportunities for formulation of biocompatible gels with robust structure-property relationships. Balance of the ratio of their precursors facilitates precise control of the yield stress and rate of self-reinforcement, enabling efficient extrusion 3D printing of HHGs.

AC electric fields cause three-dimensional orientational fluctuations (solitons) to form and rapidly propagate in confined films of liquid crystals (LCs), offering the basis of a new class of active soft matter (e.g., for accelerating mixing and transport processes in microscale chemical systems). How surface chemistry impacts the formation and trajectories of solitons, however, is not understood. Here, we show that self-assembled monolayers (SAMs) formed from alkanethiols on gold, which permit precise control over surface chemistry, are electrochemically stable over voltage and frequency windows (<100 V; 1 kHz) that lead to soliton formation in achiral nematic films of 4′-butyl-4-heptyl-bicyclohexyl-4-carbonitrile (CCN-47). By comparing soliton formation in LC films confined by SAMs formed from hexadecanethiol (C 16 SH) or pentadecanethiol (C 15 SH), we reveal that the electric field required for soliton formation increases with the LC anchoring energy: surfaces patterned with regions of C 16 SH and C 15 SH SAMs thus permit spatially controlled creation and annihilation of solitons necessary to generate a net flux of solitons. We also show that solitons propagate in orthogonal directions when confined by obliquely deposited gold films decorated with SAMs formed from C 16 SH or C 15 SH and that the azimuthal direction of propagation of solitons within achiral LC films possessing surfaceinduced twists is not unique but reflects variation in the spatial location of the solitons across the thickness of the twisted LC film. Finally, discontinuous changes in LC orientation induced by patterned surface anchoring lead to a range of new soliton behaviors including refraction, reflection, and splitting of solitons at the domain boundaries. Overall, our results provide new approaches for the controlled generation and programming of solitons with complex and precise trajectories, principles that inform new designs of chemical soft matter.