Cell-Like Capsules with "Smart" Compartments.

Eukaryotic cells have inner compartments (organelles), each with distinct properties and functions. One mimic of this architecture, based on biopolymers, is the multicompartment capsule (MCC). Here, MCCs in which the inner compartments are chemically unique and "smart," i.e., responsive to distinct stimuli in an orthogonal manner are created. Specifically, one compartment alone is induced to degrade when the MCC is contacted with an enzyme while other compartments remain unaffected. Similarly, just one compartment gets degraded upon contact with reactive oxygen species generated from hydrogen peroxide (H2 O2 ). And thirdly, one compartment alone is degraded by an external, physical stimulus, namely, by irradiating the MCC with ultraviolet (UV) light. All these specific responses are achieved without resorting to complicated chemistry to create the compartments: the multivalent cation used to crosslink the biopolymer alginate (Alg) is simply altered. Compartments of Alg crosslinked by Ca2+ are shown to be sensitive to enzymes (alginate lyases) but not to H2 O2 or UV, whereas the reverse is the case with Alg/Fe3+ compartments. These results imply the ability to selectively burst open a compartment in an MCC "on-demand" (i.e., as and when needed) and using biologically relevant stimuli. The results are then extended to a sequential degradation, where compartments in an MCC are degraded one after another, leaving behind an empty MCC lumen. Collectively, this work advances the MCC as a platform that not only emulates key features of cellular architecture, but can also begin to capture rudimentary cell-like behaviors.

Universal Way to "Glue" Capsules and Gels into 3D Structures by Electroadhesion.

We demonstrate the use of electroadhesion (EA), i.e., adhesion induced by an electric field, to connect a variety of soft materials into 3D structures. EA requires a cationic and an anionic material, but these can be of diverse origin, including covalently cross-linked hydrogels made by polymerizing charged monomers or physical gels/capsules formed by the ionic cross-linking of biopolymers (e.g., alginate and chitosan). Between each cationic/anionic pair, EA is induced rapidly (in ∼10 s) by low voltages (∼10 V DC)─and the adhesion is permanent after the field is turned off. The adhesion is strong enough to allow millimeter-scale capsules/gels to be assembled in 3D into robust structures such as capsule-capsule chains, capsule arrays on a base gel, and a 3D cube of capsules. EA-based assembly of spherical building blocks can be done more precisely, rapidly, and easily than by any alternative techniques. Moreover, the adhesion can be reversed (by switching the polarity of the field)─hence any errors during assembly can be undone and fixed. EA can also be used for selective sorting of charged soft matter─for example, a 'finger robot' can selectively 'pick up' capsules of the opposite charge by EA and subsequently 'drop off' these structures by reversing the polarity. Overall, our work shows how electric fields can be used to connect soft matter without the need for an adhesive or glue.

Reversible electroadhesion of hydrogels to animal tissues for suture-less repair of cuts or tears.

Electroadhesion, i.e., adhesion induced by an electric field, occurs between non-sticky cationic and anionic hydrogels. Here, we demonstrate electroadhesion between cationic gels and animal (bovine) tissues. When gel and tissue are placed under an electric field (DC, 10 V) for 20 s, the pair strongly adhere, and the adhesion persists indefinitely thereafter. Applying the DC field with reversed polarity eliminates the adhesion. Electroadhesion works with the aorta, cornea, lung, and cartilage. We demonstrate the use of electroadhesion to seal cuts or tears in tissues or model anionic gels. Electroadhered gel-patches provide a robust seal over openings in bovine aorta, and a gel sleeve is able to rejoin pieces of a severed gel tube. These studies raise the possibility of using electroadhesion in surgery while obviating the need for sutures. Advantages include the ability to achieve adhesion on-command, and moreover the ability to reverse this adhesion in case of error.