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2D transition metal dichalcogenides (TMDs) play increasingly significant roles in research and future optoelectronics. However, the large-scale deposition of 2D TMDs remains challenging due to sparse nucleation and substrate dependency. Liquid metals can offer effective solutions to meet these challenges due to their reactive, non-polarized, and templating properties. Here, self-deposition of 2D molybdenum sulfide is shown by introducing a molybdenum precursor onto the surface of a eutectic alloy of gallium and indium (EGaIn). EGaIn serves as an ultra-smooth template and reducing agent for the precursor to form large-scale planar molybdenum sulfides, which is transferrable to any substrate. The molybdenum sulfides form spontaneously on the surface of EGaIn, which has a sufficient potential to drive the cathodic reactions of the deposition process. A highly crystalline 2H-MoS2 is obtained after a final annealing step. This work demonstrates a fundamentally new capability for the formation of large-scale 2D TMDs.

Liquid–liquid interfaces of liquid alloys with electrolytic solutions present fertile platforms for realizing exciting interfacial phenomena that can be devised to process alloys and produce nanomaterials. Here, such an interface is established by immersing a gallium–bismuth binary liquid alloy into aqueous electrolytes. It is shown that the application of a negative voltage to this interface results in a rapid and complete liberation of bismuth nanostructures from liquid gallium. The set of conditions that govern the chemistry of the interface can be adjusted to control the oxidation state, morphology, and crystal structure of the expelled bismuth. By changing the conditions; nanotubular, atomically thin plates, and sea‐urchin‐shaped bismuth oxide morphologies are obtained. The process can also control the crystal phase of bismuth oxide as monoclinic (α), tetragonal (β), or body‐centered cubic (γ). The addition of ascorbic acid to the electrolyte is observed to prevent the oxidation of the expelled entities, resulting in bismuth metal nanoparticles. Ab initio molecular dynamics and computational fluid dynamics simulations are performed to elucidate this rapid phase separation at the interface. This knowledge will potentially lead to new pathways for using alloys as reaction media to refine metals while simultaneously producing nanomaterials for various applications. [ABSTRACT FROM AUTHOR]

Surface patterning of liquid metals (LMs) is a key processing step for LM‐based functional systems. Current patterning methods are substrate specific and largely suffer from undesired imperfections—restricting their widespread applications. Inspired by the universal catechol adhesion chemistry observed in nature, LM inks stabilized by the assembly of a naturally abundant polyphenol, tannic acid, has been developed. The intrinsic adhesive properties of tannic acid containing multiple catechol/gallol groups, allow the inks to be applied to a variety of substrates ranging from flexible to rigid, metallic to plastics and flat to curved, even using a ballpoint pen. This method can be further extended from hand‐written texts to complex conductive patterns using an automated setup. In addition, capacitive touch and hazardous heavy metal ion sensors have been patterned, leveraging from the synergistic combination of polyphenols and LMs. Overall, this strategy provides a unique platform to manipulate LMs from hand‐written pattern to complex designs onto the substrate of choice, that has remained challenging to achieve otherwise. [ABSTRACT FROM AUTHOR]

Understanding the lattice dynamics and phonon transport from the perspective of chemical bonds is essential for improving and finding high-efficiency thermoelectric materials and for many applications. Here, the coexistence of global and local weak chemical bonds is elucidated as the origin of the intrinsically low lattice thermal conductivity of non-caged structure Nowotny-Juza compound, α-MgAgSb, which is identified as a new type of promising thermoelectric material in the temperature range of 300-550 K. The global weak bonds of the compound lead to a low sound velocity. The unique three-centered MgAgSb bonds in α-MgAgSb vibrate locally and induce low-frequency optical phonons, resulting in 'rattling-like' thermal damping to further reduce the lattice thermal conductivity. The hierarchical chemical bonds originate from the low valence electron count of α-MgAgSb, with the feature shared by Nowotny-Juza compounds. Low lattice thermal conductivities are therefore highly possible in this series of compounds, which is verified by phonon and bulk modulus calculations on some of the compositions. [ABSTRACT FROM AUTHOR]

The beneficial effect of impurity scattering on thermoelectric properties has long been disregarded even though possible improvements in power factor have been suggested by Ioffe more than a half century ago. Here it is theoretically and experimentally demonstrated that proper intensification of ionized impurity scattering to charge carriers can benefit the thermoelectric figure of merit ( ZT) by increasing the Seebeck coefficient and decreasing the electronic thermal conductivity. The optimal strength of ionized impurity scattering for maximum ZT depends on the Fermi level and the density of states effective mass. Cr-doping in Ce yCo4Sb12 progressively increases the strength of ionized impurity scattering, and significantly improves the Seebeck coefficient, resulting in high power factors of 45 μW cm−1 K−2 with relatively low electrical conductivity. This effect, combined with the increased Ce-filling fraction and thus decreased lattice thermal conductivity by charge compensation of Cr-dopant, gives rise to a maximum ZT of 1.3 at 800 K and a large average ZT of 1.1 between 500 and 850 K, ≈30% and ≈20% enhancements as compared with those of Cr-free sample, respectively. Furthermore, this study also reveals that carrier scattering parameter can be another fundamental degree of freedom to optimize electrical properties and improve thermal-to-electricity conversion efficiencies of thermoelectric materials. [ABSTRACT FROM AUTHOR]

The beneficial effect of impurity scattering on thermoelectric properties has long been disregarded even though possible improvements in power factor have been suggested by Ioffe more than a half century ago. Here it is theoretically and experimentally demonstrated that proper intensification of ionized impurity scattering to charge carriers can benefit the thermoelectric figure of merit ( ZT) by increasing the Seebeck coefficient and decreasing the electronic thermal conductivity. The optimal strength of ionized impurity scattering for maximum ZT depends on the Fermi level and the density of states effective mass. Cr-doping in Ce yCo4Sb12 progressively increases the strength of ionized impurity scattering, and significantly improves the Seebeck coefficient, resulting in high power factors of 45 μW cm−1 K−2 with relatively low electrical conductivity. This effect, combined with the increased Ce-filling fraction and thus decreased lattice thermal conductivity by charge compensation of Cr-dopant, gives rise to a maximum ZT of 1.3 at 800 K and a large average ZT of 1.1 between 500 and 850 K, ≈30% and ≈20% enhancements as compared with those of Cr-free sample, respectively. Furthermore, this study also reveals that carrier scattering parameter can be another fundamental degree of freedom to optimize electrical properties and improve thermal-to-electricity conversion efficiencies of thermoelectric materials. [ABSTRACT FROM AUTHOR]

Element doping/alloying is a common strategy to tune the electrical and thermal transports of thermoelectric (TE) materials, but the doping/alloying limit of foreign elements in many TE materials is usually very low, bringing a great challenge to improve the TE performance. In this work, beyond the classic principle of “like dissolves like,” it is found that choosing the compound with a severely distorted lattice and diversified chemical bonding as the matrix also facilitates achieving a high doping/alloying limit. Taking ductile semiconductors as an example, this work shows that gold (Au) element is nearly immiscible in Ag2S and Ag2Te, but has a relatively high alloying limit in complex Ag2S0.5Te0.5 meta‐phase. Au in Ag2S0.5Te0.5 significantly decreases the carrier concentration and improves the TE performance, but scarcely changes the mechanical properties. Consequently, Ag1.99Au0.01S0.5Te0.5 demonstrates both a high figure‐or‐merit of 0.95 at 550 K and extraordinary room‐temperature ductility. This work offers an effective and general strategy to develop stabilized doped/alloyed TE materials. [ABSTRACT FROM AUTHOR]

Liquid metals offer unprecedented chemistry. Here it is shown that they can facilitate self‐limiting oxidation processes on their surfaces, which enables the growth of metal oxides that are atomically thin. This claim is exemplified by creating atomically thin hydrated MnO2 using a Galvanic replacement reaction between permanganate ions and a liquid gallium–indium alloy (EGaIn). The "liquid solution"–"liquid metal" process leads to the reduction of the permanganate ions, resulting in the formation of the oxide monolayer at the interface. It is presented that under mechanical agitation liquid metal droplets are established, and simultaneously, hydrated gallium oxides and manganese oxide sheets delaminate themselves from the interfacial boundaries. The produced nanosheets encapsulate a metallic core, which is found to consist of solid indium only, with the full migration of gallium out of the droplets. This process produces core/shell structures, where the shells are made of stacked atomically thin nanosheets. The obtained core/shell structures are found to be an efficient photocatalyst for the degradation of an organic dye under simulated solar irradiation. This study presents a new research direction toward the modification and functionalization of liquid metals through spontaneous interfacial redox reactions, which has implications for many applications beyond photocatalysis. [ABSTRACT FROM AUTHOR]

Bi2Te3‐based compounds and derivatives are milestone materials in the fields of thermoelectrics (TEs) and topological insulators (TIs). They have highly complex band structures and interesting lattice dynamics, which are favorable for high TE performance as well as strong spin orbit and band inversion underlying topological physics. This review presents rational calculations of properties related to TEs and provides theoretical guidance for improving the TE performance of Bi2Te3‐based materials. Although the band structures of these TE materials have been studied theoretically and experimentally for many years, there remain many controversies on band characteristics, especially the locations of band extrema and the exact values of bandgaps. Here, the key factors in the theoretical investigations of Bi2Te3, Bi2Se3, Sb2Te3, and their solid solutions are reviewed. The phonon spectra and lattice thermal conductivities of Bi2Te3‐based materials are discussed. Electronic and phonon structures and TE transport calculations are discussed and reported in the context of better establishing computational parameters for these V2VI3‐based materials. This review provides a useful guidance for analyzing and improving TE performance of Bi2Te3‐based materials. [ABSTRACT FROM AUTHOR]