Droplets containing ternary mixtures can spontaneously phase-separate into high-order structures upon a change in composition, which provides an alternative strategy to form multiphase droplets. However, existing strategies always involve nonaqueous solvents that limit the potential applications of the resulting multiple droplets, such as encapsulation of biomolecules. Here, a robust approach to achieve high-order emulsion drops with an all-aqueous nature from two aqueous phases by osmosis-induced phase separation on a microfluidic platform is presented. This technique is enabled by the existence of an interface of the two aqueous phases and phase separation caused by an osmolality difference between the two phases. The complexity of emulsion drops induced by phase separation could be controlled by varying the initial concentration of solutes and is systematically illustrated in a state diagram. In particular, this technique is utilized to successfully achieve high-order all-aqueous droplets in a different aqueous two-phase system. The proposed method is simple since it only requires two initial aqueous solutions for generating multilayered, organic-solvent-free all-aqueous emulsion drops, and thus these multiphase emulsion drops can be further tailored to serve as highly biocompatible material templates.

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By imposing vibration to a core-annular flow of an aqueous two-phase system (ATPS) with ultralow interfacial tension, we observe a liquid finger protruding from the interface of an expanding jet. We find that the protruded finger breaks up only when its length-to-width ratio exceeds a threshold value. The breakup follows a constant wavelength-to-width ratio that is consistent with that of breakup under Rayleigh-Plateau instability. The mechanism is applicable to aqueous two-phase systems with a large range of viscosity ratios. The protruded finger can break up into small droplets that are monodisperse in size, controllable in generation frequency under a wide range of flow rates. This work suggests a way to generate small water-water droplets with high monodispersity and production rate from a single nozzle.

In article number https://doi.org/10.1002/smll.201802107, Ho Cheung Shum and co‐workers demonstrate an approach to produce high‐order, up to quadruple, all‐aqueous emulsion drops, which are initiated by osmosis‐induced phase separation from non‐equilibrium aqueous two‐phase systems on a glass‐based microfluidic platform. The complexity of the generated all‐aqueous emulsion drops is well predicted in a phase diagram, providing a strategy to fabricate all‐aqueous emulsions with a tunable high‐order structure.

Power‐free shape retention enables soft pneumatic robots to reduce energy cost and avoid unexpected collapse due to burst or puncture. Existing strategies for pneumatic actuation cannot attain motion locking for trajectories combining extension and bending, one of the most common modes of operation. Here, a design paradigm is introduced for soft pneumatic actuators to enable zero‐power locking for shape retention in both extension and bending. The underpinning mechanism is the integration of a pneumatic transmitter and a multistable guider, which are programmed to interact for balanced load transfer, flexural and extension steering, and progressive snapping leading to state locking. Through theory, simulations, and experiments on proof‐of‐concept actuators, the existence of four distinct regimes of deformation is unveiled, where the constituents first interact during inflation to attain locking in extension and bending, and then cooperate under vacuum to enable fully reversible functionality. Finally, the design paradigm is demonstrated to realize a soft robotic arm capable to lock at desired curvature states at zero‐power, and a gripper that safely operates with puncture resistance to grasp and hold objects of various shapes and consistency. The study promises further development for zero‐power soft robots endowed with multiple deformation modes, sequential deployment, and tunable multistability.