Programmable heating and quenching for efficient thermochemical synthesis.

Conventional thermochemical syntheses by continuous heating under near-equilibrium conditions face critical challenges in improving the synthesis rate, selectivity, catalyst stability and energy efficiency, owing to the lack of temporal control over the reaction temperature and time, and thus the reaction pathways1-3. As an alternative, we present a non-equilibrium, continuous synthesis technique that uses pulsed heating and quenching (for example, 0.02 s on, 1.08 s off) using a programmable electric current to rapidly switch the reaction between high (for example, up to 2,400 K) and low temperatures. The rapid quenching ensures high selectivity and good catalyst stability, as well as lowers the average temperature to reduce the energy cost. Using CH4 pyrolysis as a model reaction, our programmable heating and quenching technique leads to high selectivity to value-added C2 products (>75% versus <35% by the conventional non-catalytic method and versus <60% by most conventional methods using optimized catalysts). Our technique can be extended to a range of thermochemical reactions, such as NH3 synthesis, for which we achieve a stable and high synthesis rate of about 6,000 µmol gFe-1 h-1 at ambient pressure for >100 h using a non-optimized catalyst. This study establishes a new model towards highly efficient non-equilibrium thermochemical synthesis.

Rapid Pressureless Sintering of Glasses.

Silica glasses have wide applications in industrial fields due to their extraordinary properties, such as high transparency, low thermal expansion coefficient, and high hardness. However, current methods of fabricating silica glass generally require long thermal treatment time (up to hours) and complex setups, leading to high cost and slow manufacturing speed. Herein, to obtain high-quality glasses using a facile and rapid method, an ultrafast high-temperature sintering (UHS) technique is reported that requires no additional pressure. Using UHS, silica precursors can be densified in seconds due to the large heating rate (up to 102 K s-1 ) of closely placed carbon heaters. The typical sintering time is as short as ≈10 s, ≈1-3 orders of magnitude faster than other methods. The sintered glasses exhibit relative densities of > 98% and high visible transmittances of ≈90%. The powder-based sintering process also allows rapid doping of metal ions to fabricate colored glasses. The UHS is further extended to sinter other functional glasses such as indium tin oxide (ITO)-doped silica glass, and other transparent ceramics such as Gd-doped yttrium aluminum garnet. This study demonstrates an UHS proof-of-concept for the rapid fabrication of high-quality glass and opens an avenue toward rapid discovery of transparent materials.

Low Tortuous, Highly Conductive, and High-Areal-Capacity Battery Electrodes Enabled by Through-thickness Aligned Carbon Fiber Framework.

Thick electrode with high-areal-capacity is a practical and promising strategy to increase the energy density of batteries, but development toward thick electrode is limited by the electrochemical performance, mechanical properties, and manufacturing approaches. In this work, we overcome these limitations and report an ultrathick electrode structure, called fiber-aligned thick or FAT electrode, which offers a novel electrode design and a scalable manufacturing strategy for high-areal-capacity battery electrodes. The FAT electrode uses aligned carbon fibers to construct a through-thickness fiber-aligned electrode structure with features of high electrode material loading, low tortuosity, high electrical and thermal conductivity, and good compression property. The low tortuosity of FAT electrode enables fast electrolyte infusion and rapid electron/ion transport, exhibiting a higher capacity retention and lower charge transfer resistance than conventional slurry-casted thick electrode design.

Equilibrium Thermodynamic Properties of Aqueous Solutions of Ionic Liquid 1-Ethyl-3-Methylimidazolium Methanesulfonate [EMIM][MeSO3].

The ionic liquid 1-ethyl-3-methylimidazolium methanesulfonate ([EMIM][MeSO3]) has been considered as a promising alternative desiccant to triethylene glycol and lithium bromide commonly used in the industry. In this paper, the water activity coefficient of this binary system was measured from 303 K to 363 K with water concentration from 18% to 92%. The interaction energies between the ionic liquid molecules ([Formula: see text]) and between the ionic liquid and water molecules ([Formula: see text]) for the [EMIM][MeSO3]/water binary system were determined from the water activity coefficient data using the Non-Random Two-Liquid (NRTL) model. The magnitude of the interaction energy between the [EMIM][MeSO3] and water molecules ([Formula: see text]) was found to be in the range of 45~49 kJ/mol, which was about 20% larger than that between the water molecules ([Formula: see text]) in the [EMIM][MeSO3]/water system. The large ([Formula: see text]) can explain many observed macroscopic thermodynamic properties such as strong hygroscopicity in the ionic liquid [EMIM][MeSO3]. These interaction energies were used to determine the heat of desorption of the [EMIM][MeSO3]/water system, and the obtained heat of desorption was in good agreement with that calculated from the conventional Clausius-Clapeyron Equation.

A general method to synthesize and sinter bulk ceramics in seconds.

Ceramics are an important class of materials with widespread applications because of their high thermal, mechanical, and chemical stability. Computational predictions based on first principles methods can be a valuable tool in accelerating materials discovery to develop improved ceramics. It is essential to experimentally confirm the material properties of such predictions. However, materials screening rates are limited by the long processing times and the poor compositional control from volatile element loss in conventional ceramic sintering techniques. To overcome these limitations, we developed an ultrafast high-temperature sintering (UHS) process for the fabrication of ceramic materials by radiative heating under an inert atmosphere. We provide several examples of the UHS process to demonstrate its potential utility and applications, including advancements in solid-state electrolytes, multicomponent structures, and high-throughput materials screening.