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Abstract Gallium‐based liquid metal alloys (GaLMAs) have widespread applications ranging from soft electronics, energy devices, and catalysis. GaLMAs can be transformed into liquid metal emulsions (LMEs) to modify their rheology for facile patterning, processing, and material integration for GaLMA‐based device fabrication. One drawback of using LMEs is reduced electrical conductivity owing to the oxides that form on the surface of dispersed liquid metal droplets. LMEs thus need to be activated by coalescing liquid metal droplets into an electrically conductive network, which usually involves techniques that subject the LME to harsh conditions. This study presents a way to coalesce these droplets through a chemical reaction at mild temperatures (T∼ 80 °C). Chemical activation is enabled by adding halide compounds into the emulsion that chemically etch the oxide skin on the surface of dispersed droplets of eutectic gallium indium (eGaIn). LMEs synthesized with halide activators can achieve electrical conductivities close to bulk liquid metal (2.4 × 10⁴S cm⁻¹) after being heated. 3D printable chemically coalescing LME ink formulations are optimized by systematically exploring halide activator type and concentration, along with mixing conditions, while maximizing for electrical conductivity, shape retention, and compatibility with direct ink writing (DIW). The utility of this ink is demonstrated in a hybrid 3D printing process to create a battery‐integrated light emitting diode array, followed by a nondestructive low temperature heat activation that produces a functional device. 

Abstract Layered transition metal hydroxides (LTMHs) with transition metal centers sandwiched between layers of coordinating hydroxide anions have attracted considerable interest for their potential in developing clean energy sources and storage technologies. However, two-dimensional (2D) LTMHs remain largely understudied in terms of physical properties and applications in electronic devices. Here, for the first time we report > 20 μm α-Ni(OH)₂2D crystals, synthesized from hydrothermal reaction. And an edge-on condensation mechanism assisted with the crystal field geometry is proposed to understand the 2D intra-planar growth of the crystals, which is also testified through series of systematic comparative studies. We also report the successful synthesis of 2D Co(OH)₂crystals (> 40 μm) with more irregular shape due to the slightly distorted octahedral geometry of the crystal field. Moreover, the detailed structural characterization of synthesized α-Ni(OH)₂are performed. The optical band gap energy is extrapolated as 2.54 eV from optical absorption measurements and the electronic bandgap is measured as 2.52 eV from reflected electrons energy loss spectroscopy (REELS). We further demonstrate its potential as a wide bandgap (WBG) semiconductor for high voltage operation in 2D electronics with a high breakdown strength, 4.77 MV/cm with 4.9 nm thickness. The successful realization of the 2D LTMHs opens the door for future exploration of more fundamental physical properties and device applications.