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Abstract Natural systems, synthetic materials, and devices almost always feature interphases that control the flow of mass and energy or stabilize interfaces between incompatible materials. With technologies transitioning to non‐planar and 3D mesoscale architectures, novel deposition methods for realizing ultrathin coatings and interphases are required. Polymer networks are of particular interest for their tunable chemical and physical properties combined with their structural integrity. Here, the electrodeposition of polymer networks (EPoN) is introduced as a general approach to uniformly coat non‐planar conductive materials. Conceptually, EPoN utilizes electrochemically activated crosslinkers as polymer end groups to confine their network formation exclusively to the material surface upon charge transfer, yielding a passivating and self‐limiting growth of conformal and uniform coatings with tunable submicron thickness on conductive materials. EPoN is found to result in thin functional films of various polymer backbones and side group chemistries as demonstrated for poly(ether) and poly(acrylamide) based polymers as solid electrolyte and thermally responsive interphases, respectively. 

Abstract Liquid metals, such as Gallium‐based alloys, have unique mechanical and electrical properties because they behave like liquid at room temperature. These properties make liquid metals favorable for soft electronics and stretchable conductors. In addition, these metals spontaneously form a thin oxide layer on their surface. Applications made possible by this delicate oxide skin include shape reconfigurable electronics, 3D‐printed structures, and unconventional actuators. This paper introduces a new approach where liquid metal oxide serves as an electrochemical energy source. By mechanically rupturing their surface oxide, liquid metals form a galvanic cell and convert their chemical energy to electrical energy. When dispersing liquid metals into an ionically‐conductive liquid to form emulsions, this composite material can provide ∼500 mV of open‐circuit voltage and up to ∼4 μWof power. Protected by the naturally occurring oxide skin, the passivating oxide layer of the liquid metal shields it from self‐discharge over time. The device is also stable in harsh environments, such as high temperature or aquatic conditions. Future applications of this device are demonstrated by designing a strain‐activated stretchable battery and a pressure‐sensitive self‐powered keypad. These findings may unlock new pathways to design stretchable batteries and harness their inherent energy for self‐powered robust devices. 

Abstract Dynamic microcapsules are reported that exhibit shell membranes with fast and reversible changes in permeability in response to external stimuli. A hydrophobic anhydride monomer is employed in the thiol–ene polymerization as a disguised precursor for the acid‐containing shells; this enables the direct encapsulation of aqueous cargo in the liquid core using microfluidic fabrication of water‐in‐oil‐in‐water double emulsion drops. The poly(anhydride) shells hydrolyze in their aqueous environment without further chemical treatment, yielding cross‐linked poly(acid) microcapsules that exhibit trigger‐responsive and reversible property changes. The microcapsule shell can actively be switched numerous times between impermeable and permeable due to the exceptional mechanical properties of the thiol–ene network that prevent rupture or failure of the membrane, allowing it to withstand the mechanical stresses imposed on the capsule during the dynamic property changes. The permeability and molecular weight cutoff of the microcapsules can dynamically be controlled with triggers such as pH and ionic environment. The reversibly triggered changes in permeability of the shell exhibit a response time of seconds, enabling actively adjustable release profiles, as well as on‐demand capture, trapping, and release of cargo molecules with molecular selectivity and fast on‐off rates.