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  1. Materials that utilize heterogeneous microstructures to control macroscopic mechanical response are ubiquitous in nature. Yet, translating nature's lessons to create synthetic soft solids has remained challenging. This is largely due to the limited synthetic routes available for creating soft composites, particularly with submicron features, as well as uncertainty surrounding the role of such a microstructured secondary phase in determining material behavior. This work leverages recent advances in the development of photocrosslinkable thermogelling nanoemulsions to produce composite hydrogels with a secondary phase assembled at well controlled length scales ranging from tens of nm to tens of μm. Through analysis of the mechanical response of these fluid-filled composite hydrogels, it is found that the size scale of the secondary phase has a profound impact on the strength when at or above the elastofracture length. Moreover, this work shows that mechanical integrity of fluid–filled soft solids can be sensitive to the size scale of the secondary phase. 
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  2. An important but often overlooked feature of Diels–Alder (DA) cycloadditions is the ability for DA adducts to undergo mechanically induced cycloreversion when placed under force. Herein, we demonstrate that the commonly employed DA cycloaddition between furan and maleimide to crosslink hydrogels results in slow gelation kinetics and “mechanolabile” crosslinks that relate to reduced material strength. Through rational computational design, “mechanoresistant” DA adducts were identified by constrained geometries simulate external force models and employed to enhance failure strength of crosslinked hydrogels. Additionally, utilization of a cyclopentadiene derivative, spiro[2.4]hepta-4,6-diene, provided mechanoresistant DA adducts and rapid gelation in minutes at room temperature. This study illustrates that strategic molecular-level design of DA crosslinks can provide biocompatible materials with improved processing, mechanical durability, lifetime, and utility. 
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  3. Abstract

    Electroadhesion provides a simple route to rapidly and reversibly control adhesion using applied electric potentials, offering promise for a variety of applications including haptics and robotics. Current electroadhesives, however, suffer from key limitations associated with the use of high operating voltages (>kV) and corresponding failure due to dielectric breakdown. Here, a new type of electroadhesion based on heterojunctions between iono‐elastomer of opposite polarity is demonstrated, which can be operated at potentials as low as ≈1 V. The large electric field developed across the molecular‐scale ionic double layer (IDL) when the junction is placed under reverse bias allows for strong adhesion at low voltages. In contrast, under forward bias, the electric field across the IDL is destroyed, substantially lowering the adhesion in a reversible fashion. These ionoelastomer electroadhesives are highly efficient with respect to the force capacity per electrostatic capacitive energy and are robust to defects or damage that typically lead to catastrophic failure of conventional dielectric electroadhesives. The findings provide new fundamental insight into low‐voltage electroadhesion and broaden its possible applications.

     
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