While electrochemical water splitting is one of the most promising methods to store light/electrical energy in chemical bonds, a key challenge remains in the realization of an efficient oxygen evolution reaction catalyst with large surface area, good electrical conductivity, high catalytic properties, and low fabrication cost. Here, a facile solution reduction method is demonstrated for mesoporous Co3O4 nanowires treated with NaBH4. The high‐surface‐area mesopore feature leads to efficient surface reduction in solution at room temperature, which allows for retention of the nanowire morphology and 1D charge transport behavior, while at the same time substantially increasing the oxygen vacancies on the nanowire surface. Compared to pristine Co3O4 nanowires, the reduced Co3O4 nanowires exhibit a much larger current of 13.1 mA cm‐2 at 1.65 V vs reversible hydrogen electrode (RHE) and a much lower onset potential of 1.52 V vs RHE. Electrochemical supercapacitors based on the reduced Co3O4 nanowires also show a much improved capacitance of 978 F g‐1 and reduced charge transfer resistance. Density‐functional theory calculations reveal that the existence of oxygen vacancies leads to the formation of new gap states in which the electrons previously associated with the Co‐O bonds tend to be delocalized, resulting in the much higher electrical conductivity and electrocatalytic activity.
We study steady-state properties of inelastic gases in two-dimensions in the presence of an energy source. We generalize previous hydrodynamic treatments to situations where high and low density regions coexist. The theoretical predictions compare well with numerical simulations in the nearly elastic limit. It is also seen that the system can achieve a nonequilibrium steady-state with asymmetric velocity distributions, and we discuss the conditions under which such situations occur.
The solar-driven water splitting process is highly attractive for alternative energy utilization, while developing efficient, earth-abundant, bifunctional catalysts for both oxygen evolution reaction and hydrogen evolution reaction has remained as a major challenge. Herein, we develop an ordered CoMnO@CN superlattice structure as an efficient bifunctional water-splitting electrocatalyst, in which uniform Co-Mn oxide (CoMnO) nanoparticles are coated with a thin, continuous nitrogen-doped carbon (CN) framework. The CoMnO nanoparticles enable optimized OER activity with effective electronic structure configuration, and the CN framework serves as an excellent HER catalyst. Importantly, the ordered superlattice structure is beneficial for enhanced reactive sites, efficient charge transfer, and structural stability. This bifunctional superlattice catalyst manifests optimized current densities and electrochemical stability in overall water splitting, outperforming most of the previously reported single- or bifunctional electrocatalysts. Combining with a silicon photovoltaic cell, this CoMnO@CN superlattice bifunctional catalyst enables unassisted solar water splitting continuously for ∼5 days with a solar-to-hydrogen conversion efficiency of ∼8.0%. Our discovery suggests that these transition metal oxide-based superlattices may serve as a unique structure modality for efficient bifunctional water splitting electrocatalysts with scale-up potentials.
Polycrystalline Mo9 cluster chalcogenides AgxMo9Se11 (3.4≤x≤3.9) have been prepared by powder metallurgy techniques, sintered by spark plasma sintering and characterized by x-ray diffraction. Their thermoelectric properties (electrical resistivity, thermopower, thermal conductivity) have been determined in the 300–800 K temperature range. The AgxMo9Se11 compounds show p-type conduction characteristics. The outstanding low lattice thermal conductivities give rise to a rather high value of the dimensionless thermoelectric figure of merit ZT of ∼0.65 at 800 K for x=3.8–3.9, making this family of materials particularly promising for thermoelectric power generation applications.
Polycrystalline samples and single crystals of the new compound Ag 3 In 2 Mo 15 Se 19 were synthesized by solidstate reaction in a sealed molybdenum crucible at 1300 °C. Its crystal structure (space group R3̅ c, a = 9.9755(1) Å, c = 57.2943(9) Å, and Z = 6) was determined from single-crystal X-ray diffraction data and constitutes an Ag-filled variant of the In 2 Mo 15 Se 19 structure-type containing octahedral Mo 6 and bioctahedral Mo 9 clusters in a 1:1 ratio. The increase of the cationic charge transfer due to the Ag insertion induces a modification of the Mo−Mo distances within the Mo clusters that is discussed with regard to the electronic structure. Transport properties were measured in a broad temperature range (2−1000 K) to assess the thermoelectric potential of this compound. The transport data indicate an electrical conduction dominated by electrons below 25 K and by holes above this temperature.The metallic character of the transport properties in this material is consistent with electronic band structure calculations carried out using the linear muffin-tin orbital (LMTO) method. The complex unit cell, together with the cagelike structure of this material, results in very low thermal conductivity values (0.9 W m −1 K −1 at 300 K), leading to a maximum estimated thermoelectric figure of merit (ZT) of 0.45 at 1100 K.
We present a detailed study of the evolution of the electrical, galvanomagnetic, and thermodynamic properties of polycrystalline Ag x Mo 9 Se 11 compounds for 3.4 ≤ x ≤ 3.8 at low temperatures (2−350 K). In agreement with density functional theory calculations, the collected data show an overall gradual variation in the transport properties from metallic to semiconducting behavior on going from x = 3.4 to 3.8. The results evidence subtle variations in the electronic properties with the Ag content, typified by both positive and negative phonon-drag effects together with thermopower and Hall coefficient of opposite signs. Analysis of the data suggests that these features may be due to peculiarities of the dispersion of the valence bands in the vicinity of the chemical potential. A drastic influence of the Ag content on the thermal transport was evidenced by a pronounced change in the temperature dependence of the specific heat below 10 K. Nonlinearities in the C p (T 3 ) data are correlated to the concentration of Ag atoms, with an increase in x resulting in a more pronounced departure from a Debye law. The observed behavior mirrors that of ionic conductors, suggesting that Ag x Mo 9 Se 11 for x ≥ 3.6 might belong to this class of compounds.
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