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.
Transition metal sulfides with a multi‐elemental nature represent a class of promising catalysts for oxygen evolution reaction (OER) owing to their good catalytic activity. However, their synthesis remains a challenge due to the thermodynamic immiscibility of the constituent multimetallic elements in a sulfide structure. Herein, for the first time the synthesis of high‐entropy metal sulfide (HEMS, i.e., (CrMnFeCoNi)Sx) solid solution nanoparticles is reported. Computational and X‐ray photoelectron spectroscopy analysis suggest that the (CrMnFeCoNi)Sx exhibits a synergistic effect among metal atoms that leads to desired electronic states to enhance OER activity. The (CrMnFeCoNi)Sx nanoparticles show one of the best activities (low overpotential 295 mV at 100 mA cm−2 in 1 m KOH solution) and good durability (only slight polarization after 10 h by chronopotentiometry) compared with their unary, binary, ternary, and quaternary sulfide counterparts. This work opens up a new synthesis paradigm for high‐entropy compound nanoparticles for highly efficient electrocatalysis applications.
Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm−2), in which Cu0.9Ni0.1 shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm−2. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties.
Among all the plastic pollution, straws have brought particularly intricate problems since they are single use, consumed in a large volume, cannot be recycled in most places, and can never be fully degraded. To solve this problem, replacements for plastic straws are being developed following with the global trend of plastic straw bans. Nevertheless, none of the available degradable alternatives are satisfactory due to drawbacks including poor natural degradability, high cost, low mechanical performance, and poor water stability. Here, all-natural degradable straws are designed by hybridizing cellulose nanofibers and microfibers in a binder-free manner. Straws are fabricated by rolling up the wet hybrid film and sealed by the internal hydrogen bonding formed among the cellulose fibers after drying. The cellulose hybrid straws show exceptional behaviors including 1) excellent mechanical performance (high tensile strength of ≈70 MPa and high ductility with a fracture strain of 12.7%), 2) sufficient hydrostability (10× wet mechanical strength compared to commercial paper straw), 3) low cost, and 4) high natural degradability. Given the low-cost raw materials, the binder-free hybrid design based on cellulose structure can potentially be a suitable solution to solve the environmental challenges brought by the enormous usage of plastics straws.
One of the challenges in the use of energetic nanoparticles within a polymer matrix is the difficulty in processing by traditional mixing methods. In this paper, electrospray deposition is employed to create high loadings of aluminum nanoparticles (Al-NPs) in polyvinylidene fluoride (PVDF) reactive composite films. The deposited films containing up to 50 wt% Al are found to be crack free and mechanically flexible. Thermochemical behavior characterized by thermogravimetric (TG) and differential scanning calorimetry (DSC) analysis shows that the addition of Al-NPs sharply reduces the onset decomposition temperature due to a pre-ignition reaction occurring in the film. The combustion propagation velocity in air at three different mass loading of Al-NPs shows burning rates of 5, 16, and 23 cm s À 1 for loadings of 16.7,30, The results suggest electrospray deposition as a direct approach to make bulk polymer composites containing high metal particle mass loading and may be a prelude to 3D printing of rocket motors.
Mixing multimetallic elements in hollow‐structured nanoparticles is a promising strategy for the synthesis of highly efficient and cost‐effective catalysts. However, the synthesis of multimetallic hollow nanoparticles is limited to two or three elements due to the difficulties in morphology control under the harsh alloying conditions. Herein, the rapid and continuous synthesis of hollow high‐entropy‐alloy (HEA) nanoparticles using a continuous “droplet‐to‐particle” method is reported. The formation of these hollow HEA nanoparticles is enabled through the decomposition of a gas‐blowing agent in which a large amount of gas is produced in situ to “puff” the droplet during heating, followed by decomposition of the metal salt precursors and nucleation/growth of multimetallic particles. The high active sites per mass ratio of such hollow HEA nanoparticles makes them promising candidates for energy and electrocatalysis applications. As a proof‐of‐concept, it is demonstrated that these materials can be applied as the cathode catalyst for Li–O2 battery operations with a record‐high current density per catalyst mass loading of 2000 mA gcat.−1, as well as good stability and durable catalytic activity. This work offers a viable strategy for the continuous manufacturing of hollow HEA nanomaterials that can find broad applications in energy and catalysis.
Organophosphorus chemical warfare agents (CWAs) are extremely toxic compounds that are nominally mitigated with gas mask filtration employing metal oxide impregnated activated carbon filtration material. To develop more effective sorbents, it is important to understand the surface chemistry between these organophosphorus compounds and the individual components that make up these filtration materials. In this study, density functional theory (DFT) and Fourier transform infrared spectroscopy (FTIR) were employed to investigate the adsorption and decomposition mechanisms between a sarin simulant molecule, dimethyl methylphosphonate (DMMP), and zinc oxide, which is a component found in current filtration materials. Theoretical calculations show that DMMP readily adsorbs to a pristine and hydroxylated ZnO (101̅0) surface with average adsorption energies of 132 and 65 kJ mol–1, respectively. Experimental diffuse reflectance fourier transform infrared spectroscopy (DRIFTS) reveals that ZnO adsorbs water and readily hydroxylates under ambient conditions, which can facilitate adsorption through hydrogen bonding of the PO to ZnO surface hydroxyls. FTIR gas phase analysis also reveals that DMMP decomposes in the presence of ZnO nanoparticles (NPs) to produce methanol at room temperature. Assuming a fully hydroxylated surface of ZnO, DFT calculations reveal several plausible mechanisms for DMMP decomposition to form methanol with an activation energy barrier of 99.6 kJ mol–1. On the basis of this energy barrier to decompose DMMP, a turnover frequency (TOF) of only 3.5 × 10–7 s–1 is calculated assuming full coverage of DMMP on the ZnO nanoparticles tested. This value is qualitatively consistent with experimental results.
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