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Droplet manipulation is crucial for diverse applications ranging from bioassay to medical diagnosis. Current magnetic-field-driven manipulation strategies are mainly based on fixed or partially tunable structures, which limits their flexibility and versatility. Here, a reconfigurable magnetic liquid metal robot (MLMR) is proposed to address these challenges. Diverse droplet manipulation behaviors including steady transport, oscillatory transport, and release can be achieved by the MLMR, and their underlying physical mechanisms are revealed. Moreover, benefiting from the magnetic-field-induced active deformability and temperature-induced phase transition characteristics, its droplet-loading capacity and shape-locking/unlocking switching can be flexibly adjusted. Because of the fluidity-based adaptive deformability, MLMR can manipulate droplets in challenging confined environments. Significantly, MLMR can accomplish cooperative manipulation of multiple droplets efficiently through on-demand self-splitting and merging. The high-performance droplet manipulation using the reconfigurable and multifunctional MLMR unfolds new potential in microfluidics, biochemistry, and other interdisciplinary fields.

Fibrous surfaces in nature have already exhibited excellent functions that are normally ascribed to the synergistic effects of special structures and material properties. The honey bee tongue, foraging liquid food in nature, has a unique segmented surface covered with dense hairs. Since honey bees are capable of using their tongue to adapt to possibly the broadest range of feeding environments to exploit every possible source of liquids, the surface properties of the tongue, especially the covering hairs, would likely represent an evolutionary optimization. In this paper, we show that their tongue hairs are stiff and hydrophobic, the latter of which is highly unexpected as the structure is designed for liquid capturing. We found that such hydrophobicity can prevent those stiff hairs from being adhered to the soft tongue surface, which could significantly enhance the deformability of the tongue when honey bees feed at various surfaces and promote their adaptability to different environments. These findings bridge the relationship between surface wettability and structural characteristics, which may shed new light on designing flexible microstructured fiber systems to transport viscous liquids.

Liquid manipulation on solid surfaces has attracted a lot of attention for liquid collection and droplet-based microfluidics. However, manipulation strategies mainly depend on chemical modification and artificial structures. Here, we demonstrate a feasible and general strategy based on the self-shrinkage of the droplet induced via specific vapors to efficiently collect liquids and flexibly carry out droplet-based reactions. The vapor-induced self-shrinkage is driven by Marangoni flow originating from molecular adsorption and diffusion. Under a specific vapor environment, the self-shrinking droplet exhibits unique features including reversible responsiveness, high mobility, and autocoalescence. Accordingly, by building a specific vapor environment, the thin liquid films and random liquid films on superlyophilic substrates can be recovered with a collection rate of more than 95%. Moreover, the vapor system can be used to construct a high-efficiency chemical reaction device. The findings and profound understandings are significant for the development of the liquid collection and droplet-based microfluidics.

Patterning of water or oil is of great significance in microfluidics and printing; however, it is still a great challenge to achieve the synchronous patterning of water and oil. Here, we report a distinct Domino patterning of water and oil, simultaneously originating from O/W emulsions. The O/W emulsions first form various emulsion patterns on the textured substrates due to local capillary differences. With the evaporation, the emulsion breaking in emulsion patterns propagates from the boundary toward the center along the radial direction, followed by the formation of water droplet arrays like a Domino. Combining patterned substrates with the Domino patterning, a variety of polymer patterns, including circle-dot arrays, quadrangle-dot arrays, and triangle-dot arrays on tens of micrometers, are successfully produced on the substrates. The Domino patterning may provide a new view for phase separation patterning, liquid directional transport, and block polymer patterns.

Elimination of satellite droplets in inkjet printing has long been desired for high-resolution and precision printing of functional materials and tissues. Generally, the strategy to suppress satellite droplets is to control ink properties, such as viscosity or surface tension, to assist ink filaments in retracting into one drop. However, this strategy brings new restrictions to the ink, such as ink viscosity, surface tension, and concentration. Here, we report an alternative strategy that the satellite droplets are eliminated by enhancing Rayleigh instability of filament at the break point to accelerate pinch-off of the droplet from the nozzle. A superhydrophobic and ultralow adhesive nozzle with cone morphology exhibits the capability to eliminate satellite droplets by cutting the ink filament at breakup point effectively. As a result, the nozzles with different sizes (10–80 μm) are able to print more inks (1 < Z< 38), for which the nozzles are super-ink-phobic and ultralow adhesive, without satellite droplets. The finding presents a new way to remove satellite droplets via designing nozzles with super-ink-phobicity and ultralow adhesion rather than restricting the ink, which has promising applications in printing electronics and biotechnologies.

Droplet impact on solid surfaces is essential both in nature and industry. Precisely regulating the dynamic behavior of droplet impact is of great significance for energy harvesting, anti‐icing, inkjet printing, pesticide spraying, and many other fields. Various rebounding behaviors (deposition, rebounding, rotation, instability control, and so on) and rebounding intrinsic parameters (such as contact time) after droplets impacting on solid surfaces can be regulated by surface engineering. This paper reviews the advances in regulating droplet impact behavior from the perspective of symmetry by modifying solid surfaces from the following aspects: chemical modification and physical structure regulation, in which the symmetry is discussed from mirror symmetry and rotational symmetry. Firstly, the symmetry of the droplet impact dynamics and its influencing factors are introduced. Then the modulation of droplet impact symmetry, using homogeneous and heterogeneous chemically modified solid surfaces, is summarized. The following presents the influence of physical structures, from micro to macro scale compared to the droplet size, on the droplet impact symmetry. Finally, the future challenges and opportunities of the droplet impact behavior regulation are discussed. Droplet impact on solid surfaces is essential both in nature and industry. This paper reviews the advances in regulating droplet impact behavior from the perspective of symmetry by modifying solid surfaces from the following aspects: chemical modification and physical structure regulation, in which the symmetry is discussed from mirror symmetry and rotational symmetry.

The collection and utilization of water power as clean energy have made tremendous progress in recent years, where the droplet-based triboelectric power generation is one of the most studied fields. Current researches mainly focus on the droplet-based single-electrode triboelectric generation mode; however, the low power output greatly limits the practical applications. By contrast, the droplet-based bi-electrode freestanding TENG (DBE-TENG) show great potential for enhancing the output, while the charge transfer mechanism of droplets evolution on the DBE-TENG is still ambiguous. Here we demonstrate that for a DBE-TENG, the maximum current output of the droplet at different droplet impact positions exhibits a sinusoidal-like variation, and the current output can be improved by two orders of magnitude by simply controlling the droplet impacting positions. Furthermore, an asymmetrical-capacitance-induced charge transfer mechanism is proposed, which well elucidates the prominent current output enhancement and the sinusoidal-like variation. In addition, the current output enhancing strategy is applicable under different kinds of dielectric materials and conditions (inclined conditions and different Weber numbers), with the maximum enlargement up to 263 times. The findings deepen the understanding of the charge transfer mechanism for bi-electrode triboelectric nanogenerators, and will be of significance for improving the efficiency of sustainable energy harvesting.

An effective way to improve the electrical conductivity of printed graphene patterns was demonstrated by realizing the assembly of giant graphene oxide sheets during the printing process. The synergetic effect of printing-induced orientation and evaporation-induced interfacial assembly facilitated the formation of laminar-structured patterns. The resulting patterns after chemical reduction showed excellent electrical conductivity in printed graphene electronics. Because of their high conductivity, mechanical flexibility, and advantage in pattern design, printed graphene electrodes were applied in electrical-driven soft actuators, which can realize controllable deformation with low driving voltage. Such achievements will be of great significance for the development of graphene-based flexible and printed electronics.

Self-assembly of colloidal nanoparticles has generated tremendous interest due to its widespread applications in structural colorations, sensors, and optoelectronics. Despite numerous strategies being developed to fabricate sophisticated structures, the heterogeneous self-assembly of a single type of nanoparticle in one step remains challenging. Here, facilitated by spatial confinement induced by a skin layer in a drying droplet, we achieve the heterogeneous self-assembly of a single type of nanoparticle by quickly evaporating a colloid-poly (ethylene glycol) (PEG) droplet. During the drying process, a skin layer forms at the droplet surface. The resultant spatial confinement assembles nanoparticles into face-centered-cubic (FCC) lattices with (111) and (100) plane orientations, generating binary bandgaps and two structural colors. The self-assembly of nanoparticles can be regulated by varying the PEG concentration so that FCC lattices with homo- or heterogeneous orientation planes can be prepared on demand. Besides, the approach is applicable for diverse droplet shapes, various substrates, and different nanoparticles. The one-pot general strategy breaks the requirements for multiple types of building blocks and predesigned substrates, extending the fundamental understanding underlying colloidal self-assembly.

Spots with dual structural colors on the skin of some organisms in nature are of tremendous interest due to the unique function of their dye-free colors. However, imitation of them requires complicated manufacturing processes, expensive equipment, and multiple predesigned building blocks. In this work, a one-pot strategy based on the phase-separation-assisted nonuniform self-assembly of monosized silica nanoparticles is developed to construct domes with dual structural colors. In drying poly(ethylene glycol)-dextran-based (PEG-DEX) droplets, monosized nanoparticles distribute nonuniformly in two compartments due to the droplet inner flow and different nanoparticle compatibility with the two phases. The dome colors are derived from the self-assembled nanoparticles and are programmable by regulating the assembly conditions. The one-pot strategy enables the preparation of multicolor using only one type of building block. With the dual-color domes, encrypted patterns with a high volume of contents are designed, showing promising applications in information delivery.

Inkjet printing provides an efficient routine for distributing functional materials into locations with well-designed arrangements. As one of the most critical factors in determining the printing quality, the impacting and depositing behaviors of ink drops largely depend on the wettability of the target surface. In addition to printing on solids with intrinsic wettability, various ink-drop impact dynamics and deposition morphologies have been reported through modifying the surface wettability including both homogeneous and heterogeneous, which opens up possibilities for applications such as advanced optic/electric device fabrication and highly sensitive detection. In this Perspective, we summarize recent progress in the modification methods of solid surface wettability and their capability in modulating the ink-drop impacting and depositing dynamics. The challenges facing ink-drop regulation by chemical modification methodologies are also envisaged at the end of the Perspective.

Heterostructures have attracted enormous interest due to the properties arising from the coupling and synergizing between multiscale structures and the promising applications in electronics, mechanics, and optics. However, it is challenging for current technologies to precisely integrate cross-scale micro/nanomaterials in three dimensions (3D). Herein, we realize the precise spatial allocation of nanoblocks on micromatrices and programmable 3D optical heterostructure patterning via printing-assisted self-assembly. This bottom-up approach fully exploits the advantages of printing in on-demand patterning, low cost, and mass production, as well as the merits of solution-based colloidal assembly for simple structuring and high-precision regulating, which facilitates the patterned integration of multiscale materials. Importantly, the luminescent nanoparticle assembly can be accurately coupled to the dye-doped polymer matrix by regulating the interface wettability, enabling facile multicolor tuning in a single heterostructure. Thus, the heterostructure can be specially encoded for anticounterfeiting and encryption applications due to the morphology-dependent and interface-coupling-induced luminescence. Moreover, with the capability to achieve single-nanoparticle resolution, these findings have great potential for designing photonic superstructures and advanced optical devices.

It is challenging to design complex synthetic life-like systems that can show both autoevolution and fuel-driven transient behaviors. Here, we report a new class of chemical reaction networks (CRNs) to construct life-like polymer hydrogels. The CRNs are constituted of autocatalytic cascade reactions and fuel-driven reaction networks. The reactions start with only two compounds, that is, thiol of 4-arm-PEG-SH and thiuram disulfides, and undergo thiol oxidation (k1), disulfide metathesis (k2), and thionate hydrolysis-coupling reactions (k3) subsequently, leading to a four-state autonomous transition of sol(I) → soft gel → sol(II) → stiff gel. Moreover, thiuram disulfides can be applied as a fuel to drive the repeated occurrence of metathesis and hydrolysis-coupling reactions, generating dissipative stiff gel → sol(II) → stiff gel cycles. Systematic kinetics studies reveal that the event and lifetime of every transient state could be delicately tailored-up by varying the thiuram disulfide concentration, pH of the system, and thiuram structures. Since the consecutive transient behaviors are precisely predictable, we envision the strategy’s potential in guiding the molecular designs of autonomous and adaptive materials for many fields.

Only 0.1% of the acoustic energy can transmit across the water–air interface because of the huge acoustic impedance mismatch. Enhancing acoustic transmission across the water–air interface is of great significance for sonar communications and sensing. However, due to the interface instability and subwavelength characteristics of acoustic metamaterials, wide-angle intermediate-frequency (10 kHz-100 kHz) water–air acoustic transmission remains a great challenge. Here, we demonstrate that the lotus leaf is a natural low-cost acoustic transmission metasurface, namely, the lotus acoustic metasurface (LAM). Experiments demonstrate the LAM can enhance the acoustic transmission across the water–air interface, with an energy transmission coefficient of about 40% at 28 kHz. Furthermore, by fabricating artificial LAMs, the operating frequencies can be flexibly adjusted. Also, the LAM allows a wide-angle water-to-air acoustic transmission. It will enable various promising applications, such as detecting and imaging underwater objects from the air, communicating between ocean and atmosphere, reducing ocean noises, etc.