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Abstract We report the facile synthesis and 3D printing of a series of triblock copolymers consisting of soft and hard blocks and demonstrate that alkene pendant groups of the hard block can be covalently modified. The polymers are prepared using a salenCo(III)TFA/PPNTFA binary catalyst system and 1,2‐propanediol as a chain transfer agent, providing an efficient one‐pot, two‐step strategy to tailor polymer thermal and mechanical properties. Thixotropic inks suitable for direct ink write printing were formulated by dissolving the block copolymers in organic solvent and dispersing NaCl particles. After printing, porous structures were produced by removing solvent and NaCl with water to give printed structures with surfaces that could be modified via UV‐initiated thiol‐ene click reactions. Alternatively, a tetra‐thiol could be incorporated into the ink and used for cross‐linking to give objects with high solvent resistance and selective degradability. 

In this study, the direct ink write (DIW) additive manufacturing technique is employed to print “self-fitting” shape memory polymer (SMP) scaffolds with requisite porosity from biodegradable poly(ε-caprolactone)-diacrylate (PCL-DA)-based polymers. 

The major challenge to fabricate MXene/polymer composites are the processing conditions and poor control over the distribution of the MXene nanosheets within the polymer matrix. Traditional ways involve the direct mix of fillers and polymers to form a random homogeneous composite, which leads to inefficient use of fillers. To address these challenges, researchers have focused on the development of ordered MXene/polymer composite structures using various fabrication strategies. In this review, we summarize recent advances of structured MXene/polymer composites and their processing-structure-property relationships. Two main forms of MXene/polymer composites (films and foams) are separately discussed with a focus on the detailed fabrication means and corresponding structures. These architected composites complement those in which MXenes nanosheets are isotropically dispersed throughout, such as those formed by aqueous solution mixing approaches. This review culminates in a perspective on the future opportunities for architected MXene/polymer composites. 

3D printing is a versatile technology for creating objects with custom geometries and compositions and is increasingly employed for fabricating hybrid solid–liquid composites (SLCs). These composites, comprising solid matrices with integrated liquid components, showcase unique properties such as enhanced flexibility and improved thermal and electrical conductivities. This review focuses on methods to fabricate SLCs directly by different 3D printing techniques, e.g. without needing to backfill or impregnate a porous matrix. The techniques of extrusion, vat photopolymerization and material jetting combined with microfluidics, inkjet printing, vacuum filling and ultraviolet light curing to produce SLCs are emphasized. We also discuss the development of feedstocks, focusing on emulsions and polymer capsules as fillers, and analyze current literature to highlight their significance. The review culminates in a perspective on new directions, highlighting the potential of bicontinuous interfacially jammed emulsion gels (bijels) to facilitate the printing of continuous liquid pathways, alongside the importance of understanding ink formulation and stability. Concluding with future perspectives, we underline the transformative impact of 3D‐printed SLCs in diverse applications, signaling a significant advancement in the field. 

We report an approach for soft-template encapsulation of PCMs vita organocatalyzed photoredox ATRP using silica surfactants with surface-immobilized initiators. 

Solid–liquid composites (SLCs) combine the properties of solids and liquids, enhancing functionalities and expanding potential applications. Traditional methods for creating SLCs often face challenges such as low mass transfer efficiency, difficulty in controlling separation behavior, and substantial waste production. Herein, we report a new approach to solve these challenges by using disulfide-based responsive polymeric capsule shells to make liquid-filled monoliths for carbon capture. The capsules are prepared through interfacial polymerization and contain either non-polar poly(α-olefin)432 or highly polar 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([HMIM][TFSI]) at 74–82 wt%. Upon gentle heating, the dynamic disulfide bonds of the isolated capsules undergo bond exchange, leading to the fusion of capsule shells into free-standing monoliths that retain >89 wt% of their liquid core and remain stable for at least two weeks. These monoliths demonstrate CO2 absorption rates and capacities comparable to their capsule counterparts; further, in response to radiofrequency (RF), they reach the CO2 desorption temperature in only ∼31 s. This innovative system addresses the limitations of conventional SLC fabrication techniques, offering a versatile and practical approach to fusing polymer capsule shells for applications across separation, energy storage, and carbon capture applications. 

Microencapsulation of pristine core liquids in polymer shells has critical applications in thermal energy storage and management, targeted drug delivery, and carbon capture, among others. Herein, we report a novel encapsulation approach based on a double emulsion soft-template to produce microcapsules comprised of an ionic liquid (IL) core in a degradable polymer shell. We demonstrate the production of [IL-in-oil1]-in-oil2 (IL/O1/O2) double emulsions, in which the oil interphase (O1) contains a CO2-derived polycarbonate bearing vinyl pendant groups, tetrathiol small molecule crosslinker, and photoinitiator; upon irradiation of the double emulsion under low shear, thiol–ene crosslinking of the loaded species results in the formation of a robust shell around the pure IL droplets. The core–shell structures have enhanced physisorption for CO2 uptake compared to the bulk IL, which is consistent with the combined capacity of the IL/shell alone and demonstrates more rapid uptake due to an enhanced gas–liquid interface. This approach to microencapsulation of functional liquids offers researchers a distinct route to fabricate composite architectures with a pristine core for applications in separations, transport of cargo, and gas uptake. 

Silica particles were modified to achieve tailored wettability and interfacial activity at various interfaces, allowing for fabrication of hybrid architectures.