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The measured force during a puncture test is found to increase when the needle tip is near to the vial walls. An experimental method for quantifying this increase in stiffness is developed. 

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. 

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.