Flexible polyfluorinated bis-diazirines as molecular adhesives.

Motivated by a desire to develop flexible covalent adhesives that afford some of the same malleability in the adhesive layer as traditional polymer-based adhesives, we designed and synthesized two flexible, highly fluorinated bis-diazirines. Both molecules are shown to function as effective crosslinkers for polymer materials, and to act as strong adhesives when painted between two polymer objects of low surface energy, prior to thermal activation. Data obtained from lap-shear experiments suggests that greater molecular flexibility is correlated with improved mechanical compliance in the adhesive layer.

Nonlinear XFEM Modeling of Mode II Delamination in PPS/Glass Unidirectional Composites with Uncertain Fracture Properties.

Initiation and propagation of cracks in composite materials can severely affect their global mechanical properties. Due to the lower strength of the interlaminar bonding compared to fibers and the matrix, delamination between plies is known to be one of the most common failure modes in these materials. It is therefore deemed necessary to gain more insight into this type of failure to guide the design of composite structures towards ensuring their robustness and reliability during service. In this work, delamination of interlaminar bonding in composite end-notched flexure (ENF) samples was modeled using a newly developed stochastic 3D extended finite element method (XFEM). The proposed numerical scheme, which also incorporates the cohesive zone model, was used to characterize the mode II delamination results obtained from ENF testing on polyphenylene sulfide (PPS)/glass unidirectional (UD) composites. The nonrepeatable material responses, often seen during fracture testing of UD composites, were well captured with the current numerical model, demonstrating its capacity to predict the stochastic fracture properties of composites under mode II loading conditions.

A broadly applicable cross-linker for aliphatic polymers containing C-H bonds.

Addition of molecular cross-links to polymers increases mechanical strength and improves corrosion resistance. However, it remains challenging to install cross-links in low-functionality macromolecules in a well-controlled manner. Typically, high-energy processes are required to generate highly reactive radicals in situ, allowing only limited control over the degree and type of cross-link. We rationally designed a bis-diazirine molecule whose decomposition into carbenes under mild and controllable conditions enables the cross-linking of essentially any organic polymer through double C-H activation. The utility of this molecule as a cross-linker was demonstrated for several diverse polymer substrates (including polypropylene, a low-functionality polymer of long-standing challenge to the field) and in applications including adhesion of low-surface-energy materials and the strengthening of polyethylene fabric.

Hierarchically Enhanced Impact Resistance of Bioinspired Composites.

An order of magnitude tougher than nacre, conch shells are known for being one of the toughest body armors in nature. However, the complexity of the conch shell architecture creates a barrier to emulating its cross-lamellar structure in synthetic materials. Here, a 3D biomimetic conch shell prototype is presented, which can replicate the crack arresting mechanisms embedded in the natural architecture. Through an integrated approach combining simulation, additive manufacturing, and drop tower testing, the function of hierarchy in conch shell's multiscale microarchitectures is explicated. The results show that adding the second level of cross-lamellar hierarchy can boost impact performance by 70% and 85% compared to a single-level hierarchy and the stiff constituent, respectively. The overarching mechanism responsible for the impact resistance of conch shell is the generation of pathways for crack deviation, which can be generalized to the design of future protective apparatus such as helmets and body armor.

Hydraulic hydrogel actuators and robots optically and sonically camouflaged in water.

Sea animals such as leptocephali develop tissues and organs composed of active transparent hydrogels to achieve agile motions and natural camouflage in water. Hydrogel-based actuators that can imitate the capabilities of leptocephali will enable new applications in diverse fields. However, existing hydrogel actuators, mostly osmotic-driven, are intrinsically low-speed and/or low-force; and their camouflage capabilities have not been explored. Here we show that hydraulic actuations of hydrogels with designed structures and properties can give soft actuators and robots that are high-speed, high-force, and optically and sonically camouflaged in water. The hydrogel actuators and robots can maintain their robustness and functionality over multiple cycles of actuations, owing to the anti-fatigue property of the hydrogel under moderate stresses. We further demonstrate that the agile and transparent hydrogel actuators and robots perform extraordinary functions including swimming, kicking rubber-balls and even catching a live fish in water.