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Hydrogenation is an effective way to tune the property of metal oxides. It can conventionally be performed by doping hydrogen into solid materials with noble-metal catalysis, high-temperature/pressure annealing treatment, or high-energy proton implantation in vacuum condition. Acid solution naturally provides a rich proton source, but it should cause corrosion rather than hydrogenation to metal oxides. Here we report a facile approach to hydrogenate monoclinic vanadium dioxide (VO 2 ) in acid solution at ambient condition by placing a small piece of low workfunction metal (Al, Cu, Ag, Zn, or Fe) on VO 2 surface. It is found that the attachment of a tiny metal particle (~1.0 mm) can lead to the complete hydrogenation of an entire wafer-size VO 2 (>2 inch). Moreover, with the right choice of the metal a two-step insulator–metal–insulator phase modulation can even be achieved. An electron–proton co-doping mechanism has been proposed and verified by the first-principles calculations. Hydrogenation is an effective way to tune the property of metal oxides. Here, the authors report a simple approach to hydrogenate VO 2 in acid solution under ambient conditions by placing a small piece of low workfunction metal on VO 2 surface.

HighlightsA bimetallic lanthanum-nickel oxysulfide based on a La2O2S prototype was developed as a precatalyst for the electrochemical alkaline oxygen evolution reaction (OER).The in situ, ex situ, and theoretical investigations demonstrated that the precatalyst underwent a deep OER-driven reconstruction into a porous heterostructure where NiOOH nanodomains were uniformly separated and confined by La(OH)3 barrier.Oxyanion (SO42−) was steadily adsorbed on the surface of this in situ reconstructed NiOOH/La(OH)3 heterostructure, enabling it for enhanced OER activity and durability.Efficient and durable oxygen evolution reaction (OER) requires the electrocatalyst to bear abundant active sites, optimized electronic structure as well as robust component and mechanical stability. Herein, a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La2O2S prototype is fabricated as a binder-free precatalyst for alkaline OER. The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La, Ni, O, and S species during OER, which assures the adsorption and stabilization of the oxyanion SO42- onto the surface of the deeply reconstructed porous heterostructure composed of confining NiOOH nanodomains by La(OH)3 barrier. Such coupling, confinement, porosity and immobilization enable notable improvement in active site accessibility, phase stability, mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates. The optimized electrocatalyst delivers exceptional alkaline OER activity and durability, outperforming most of the Ni-based benchmark OER electrocatalysts.

Vacancy engineering is deemed as one of the powerful protocols to tune the catalytic activity of electrocatalysts. Herein, Se‐vacancy with charge polarization is created in the NiSe2 structure (NiSe2‐VSe) via a sequential phase conversion strategy. By a combined analysis of the Rietveld method, transient photovoltage spectra (TPV), in situ Raman and density functional theory (DFT) calculation, it is unequivocally discovered that the presence of charge‐polarized Se‐vacancy is beneficial for stabilizing the structure, decreasing the electron transfer kinetics, as well as optimizing the free adsorption energy of reaction intermediate during two‐electron oxygen reduction reaction (2e− ORR). Benefiting from these merits, the as‐prepared NiSe2‐VSe delivered the highest selectivity of 96% toward H2O2 in alkaline media, together with a selectivity higher than 90% over the wide potential range from 0.25 to 0.55 V, ranking it in the top level among the previously reported transition metal‐based electrocatalysts. Most notably, it also displayed admirable stability with only a slight selectivity decay after 5000 cycles of accelerated degradation test (ADT). Nickel diselenide with negative charge‐polarized Se vacancy (NiSe2‐Vse) has been developed for the two‐electron oxygen reduction reaction (2e− ORR), which delivered remarkable activity, selectivity, and stability. Furthermore, the presence of negatively charge‐polarized Se vacancy effectively retards the interfacial charge transfer and optimizes the adsorption free energy toward *OOH intermediate.

For first-order phase transitions, the second derivatives of Gibbs free energy (specific heat and compressibility) diverge at the transition point, resulting in an effect known as super-elasticity along the pressure axis, or super-thermicity along the temperature axis. Here we report a chemical analogy of these singularity effects along the atomic doping axis, where the second derivative of Gibbs free energy (chemical susceptibility) diverges at the transition point, leading to an anomalously high energy barrier for dopant diffusion in co-existing phases, an effect we coin as super-susceptibility. The effect is realized in hydrogen diffusion in vanadium dioxide (VO 2 ) with a metal-insulator transition (MIT). We show that hydrogen faces three times higher energy barrier and over one order of magnitude lower diffusivity when it diffuses across a metal-insulator domain wall in VO 2 . The additional energy barrier is attributed to a volumetric energy penalty that the diffusers need to pay for the reduction of latent heat. The super-susceptibility and resultant retarded atomic diffusion are expected to exist universally in all phase transformations where the transformation temperature is coupled to chemical composition, and inspires new ways to engineer dopant diffusion in phase-coexisting material systems. For first-order phase transitions, the second derivatives of Gibbs free energy diverge at the transition point, causing super-elasticity or super-thermicity. Here authors report a chemical analogy of these effects by atomic doping, where the second derivative of Gibbs free energy diverges at the transition point, leading to an anomalously high energy barrier for dopant diffusion in coexisting phases.

Background Chewing side preference (CSP) has been proposed as one etiology of temporomandibular disorders (TMDs) as it can induce the structural changes of the temporomandibular joint. But its association with the inclination of the articular eminence (IAE) is unknown. This study aimed to compare IAE between patients with CSP and without CSP. Methods Cone-beam computed tomography images of 90 patients with TMD (mean age of 45.6 years, 69 with CSP, 21 without CSP) and 20 participants without TMD and CSP (mean age of 41.3 years) were measured to compare IAE and depth of the glenoid fossa (DGF) Results IAE and DGF showed a positive correlation among all the participants. Compared with the participants without TMD and CSP, the TMD patients without CSP presented a similar IAE but with a significantly higher value of DGF ( p  < 0.05); in contrast, the TMD patients with CSP presented a significantly greater IAE and DGF ( p  < 0.05). No bilateral differences in IAE and DGF were observed in all the participants. Except the male patients with CSP had a deeper fossa than did the female, no differences in IAE and DGF according to gender were observed. Conclusions TMD patients with CSP seem to have a deep glenoid fossa with steep eminence which might be considered one characteristic imaging feature.

Microwave-assisted spark ignition (MAI) is a promising way to enhance the ignition performance of engines under lean conditions. To understand the effect of microwave-induced flow during MAI, the development and morphology of spark-ignited methane-air flame kernel under various microwave pulse parameters are experimentally studied. Experiments are conducted in a constant volume combustion chamber, and flame development is recorded through a high-speed shadowgraph method. Flame area and deformation index are adopted to evaluate the flame characteristic. Results show that increasing the microwave pulse energy from 0 to 150 mJ exhibits a threshold process for expanding the flame kernel area under 0.2 MPa ambient pressure. When the pulse energy is below the threshold of 90 mJ, the microwave enhancing efficiency is much lower than that beyond the threshold. Increasing microwave pulse repetition frequency (PRF) changes the flow on flame surface and raises the absorption efficiency for microwave energy, and thus helps to improve the MAI performance under higher pressures. Hence, 1 kHz pulses cause more obvious flame deformation than those with higher PRF pulses under 0.2 MPa, while this tendency is reversed as the ambient pressure increases to 0.6 MPa. Besides, microwave pulses of different repetition frequencies lead to different flame kernel morphology, implying the various regimes behind the interaction between a microwave and spark kernel.

In this paper, mesoporous CuO with a novel architecture was synthesized through a conventional hydrothermal approach followed by a facile sintering procedure. HR-TEM analysis found that mesoporous CuO with an interconnected pore structure has exposed high-energy crystal planes of (002) and (200). Theoretical calculations indicated that the high-energy crystal planes have superior adsorption capacity for H+ ions, which is critical for the excellent adsorption and remarkable photocatalytic activity of the anionic dye. The adsorption capacity of CuO to methyl orange (MO) at 0.4 g/L was approximately 30% under adsorption equilibrium conditions. We propose a state-changing mechanism to analyze the synergy and mutual restraint relation among the catalyst CuO, H+ ions, dye and H2O2. According to this mechanism, the degradation rate of MO can be elevated 3.5 times only by regulating the MO ratio in three states.

Hydrogenation is an effective way to tune the property of metal oxides. It can conventionally be performed by doping hydrogen into solid materials with noble-metal catalysis, high-temperature/pressure annealing treatment, or high-energy proton implantation in vacuum condition. Acid solution naturally provides a rich proton source, but it should cause corrosion rather than hydrogenation to metal oxides. Here we report a facile approach to hydrogenate monoclinic vanadium dioxide (VO ) in acid solution at ambient condition by placing a small piece of low workfunction metal (Al, Cu, Ag, Zn, or Fe) on VO surface. It is found that the attachment of a tiny metal particle (~1.0 mm) can lead to the complete hydrogenation of an entire wafer-size VO (>2 inch). Moreover, with the right choice of the metal a two-step insulator-metal-insulator phase modulation can even be achieved. An electron-proton co-doping mechanism has been proposed and verified by the first-principles calculations.

Combined with first-principles calculations and semiclassical Boltzmann transport theory, Janus {\\alpha}-STe2 and {\\alpha}-SeTe2 monolayers are investigated systematically. Janus {\\alpha}-STe2 and {\\alpha}-SeTe2 monolayers are indirect semiconductors with band gaps of 1.20 and 0.96 eV. It is found they possess ultrahigh figure of merit (ZT) values of 3.9 and 4.4 at 500 K, much higher than that of the pristine {\\alpha}-Te monolayer (2.8). The higher ZT originates from Janus structures reduce lattice thermal conductivities remarkably compared with pristine {\\alpha}-Te monolayer. The much higher phonon anharmonicity in Janus monolayers leads to significant lower lattice thermal conductivity. It is also found electronic thermal conductivity can play an important role in thermoelectric efficiency for the materials with quite low lattice thermal conductivity. This work suggests the potential applications of Janus {\\alpha}-STe2 and {\\alpha}-SeTe2 monolayers as thermoelectric materials and highlights Janus structure as an effective way to enhance thermoelectric performance.

VO2 material is promising for developing energy-saving \"smart window\", owing to its thermochromic property induced by metal-insulator transition (MIT). However, its practical application is greatly limited by the relatively high critical transition temperature (~68oC), low luminous transmittance (<60%) and poor solar energy regulation ability (<15%). Here we developed a reversible and non-volatile electric-field control on the MIT of monoclinic VO2 film. With a solid electrolyte layer assisted gating treatment, we modulated the insertion/extraction of hydrogens into/from VO2 lattice at room temperature, causing tri-state phase transitions accompanied with controllable transmission adjustment. The dramatic increase of visible/infrared transmittance during the phase transition from the metallic (lightly H-doping) to insulating (heavily H-doping) phase leads to an increased solar energy regulation ability up to 26.5%, while keep 70.8% visible-luminous transmittance. These results beat all previous records and even exceeded the theoretical limit for traditional VO2 smart window, removing intrinsic disadvantages of VO2 for energy-saving utilizations. Our findings not only demonstrated an electric-field controlled phase modulation strategy, but also open the door for high-performance VO2-based smart window applications.