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Liquid metals (LMs) have compelling applications in stretchable electronics, wearable devices, and soft robotics ascribing to the unique combination of room temperature fluidity and metallic electrical/thermal conductivity. Adding metallic elements in gallium‐based LMs can produce heterophasic (i.e., solid and liquid) LMs with altered properties including morphology, surface energy, rheology, electrical/thermal conductivity, and chemical reactivity. Importantly, heterophasic LMs can respond to external stimuli such as magnetic fields, temperature, and force. Thus, heterophasic LMs can broaden the potential applications of LMs. This report reviews the recent progress about heterophasic LMs through metallic elements in the periodic table and discusses their functionalities. The heterophasic LMs are systematically organized into four categories based on their features and applications including electrical/thermal conductivity, magnetic property, catalysis/energy management, and biomedical applications. This comprehensive review is aimed to help summarize the field and identify new opportunities for future studies.

 

Gallium-based liquid metals (LMs) are suitable for many potential applications due to their unique combination of metallic and liquid properties. However, due to their high surface tension and low viscosity, LMs are challenging to apply to substrates in useful shapes, such as dots, wires, and films. These issues are mitigated by mixing the LMs in air with other materials, such as mixing with solid particles to form LM solid pastes or mixing with gases to form LM foams. Underlying these deceivingly simple mixing processes are complex and highly intertwined microscale mechanisms. Air microbubbles are inevitably incorporated while making LM pastes, making them partly foams. On the other hand, for foaming of the LM to occur, a critical volume content of solid particles must be internalized first. Consequently, both LM pastes and foams are multiphase composites containing solid and fluid microcomponents. Here, we systematically study the impact of the mixing procedure, solid particle size, and volume fraction (SiO2) on the air content of the multiphase LM composites. We demonstrate that decreasing the particle size and increasing their volume fraction substantially decrease the composite density (i.e., increases air entrapment). The foaming process can also be enhanced with the use of high-speed mechanical mixing, although leading to the formation of a more disordered internal structure. In contrast, manual mixing with larger microparticles can promote the formation of more paste-like composites with minimal air content. We explain the microscopic mechanisms underlying these trends by correlating macroscopic measurements with cross-sectional electron microscopy of the internal structure. 

Pastes and “foams” containing liquid metal (LM) as the continuous phase (liquid metal foams, LMFs) exhibit metallic properties while displaying paste or putty‐like rheological behavior. These properties enable LMFs to be patterned into soft and stretchable electrical and thermal conductors through processes conducted at room temperature, such as printing. The simplest LMFs, featured in this work, are made by stirring LM in air, thereby entraining oxide‐lined air “pockets” into the LM. Here, it is reported that mixing small amounts of water (as low as 1 wt%) into such LMFs gives rise to significant foaming by harnessing known reactions that evolve hydrogen and produce oxides. The resulting structures can be ≈4–5× their original volume and possess a fascinating combination of attributes: porosity, electrical conductivity, and responsiveness to environmental conditions. This expansion can be utilized for a type of 4D printing in which patterned conductors “grow,” fill cavities, and change shape and density with respect to time. Excessive exposure to water in the long term ultimately consumes the metal in the LMF. However, when exposure to water is controlled, the metallic properties of porous LMFs can be preserved.

 

Soft materials tend to be highly permeable to gases, making it difficult to create stretchable hermetic seals. With the integration of spacers, we demonstrate the use of liquid metals, which show both metallic and fluidic properties, as stretchable hermetic seals. Such soft seals are used in both a stretchable battery and a stretchable heat transfer system that involve volatile fluids, including water and organic fluids. The capacity retention of the battery was ~72.5% after 500 cycles, and the sealed heat transfer system showed an increased thermal conductivity of approximately 309 watts per meter-kelvin while strained and heated. Furthermore, with the incorporation of a signal transmission window, we demonstrated wireless communication through such seals. This work provides a route to create stretchable yet hermetic packaging design solutions for soft devices.

 

Biosensors are analytical tools for monitoring various parameters related to living organisms, such as humans and plants. Liquid metals (LMs) have emerged as a promising new material for biosensing applications in recent years. LMs have attractive physical and chemical properties such as deformability, high thermal and electrical conductivity, low volatility, and low viscosity. LM‐based biosensors represent a new strategy in biosensing particularly for wearable and real‐time sensing. While early demonstrations of LM biosensors focus on monitoring physical parameters such as strain, motion, and temperature, recent examples show LM can be an excellent sensing material for biochemical and biomolecular detection as well. In this review, the recent progress of LM‐based biosensors for personalized healthcare and disease monitoring via both physical and biochemical signaling is survey. It is started with a brief introduction of the fundamentals of biosensors and LMs, followed by a discussion of different mechanisms by which LM can transduce biological or physiological signals. Next, it is reviewed example LM‐based biosensors that have been used in real biological systems, ranging from real‐time on‐skin physiological monitoring to target‐specific biochemical detection. Finally, the challenges and future directions of LM‐integrated biosensor platforms is discussed.