Project description:Traditional water-gas shift reaction provides one primary route for industrial production of clean-energy hydrogen. However, this process operates at high temperatures and pressures, and requires additional separation of H2 from products containing CO2, CH4 and residual CO. Herein, we report a room-temperature electrochemical water-gas shift process for direct production of high purity hydrogen (over 99.99%) with a faradaic efficiency of approximately 100%. Through rational design of anode structure to facilitate CO diffusion and PtCu catalyst to optimize CO adsorption, the anodic onset potential is lowered to almost 0 volts versus the reversible hydrogen electrode at room temperature and atmospheric pressure. The optimized PtCu catalyst achieves a current density of 70.0 mA cm-2 at 0.6 volts which is over 12 times that of commercial Pt/C (40 wt.%) catalyst, and remains stable for even more than 475 h. This study opens a new and promising route of producing high purity hydrogen.
Project description:Aqueous aluminum ion batteries (AAIBs) have received growing attention because of their low cost, safe operation, eco-friendliness, and high theoretical capacity. However, one of the biggest challenges for AAIBs is the poor reversibility due to the presence of an oxide layer and the accompanying hydrogen evolution reaction. Herein, we develop a strongly hydrolyzed/polymerized aluminum-iron hybrid electrolyte to improve the electrochemical behavior of AAIBs. On the one hand, the designed electrolyte enables aluminum ion intercalation/deintercalation on the cathode while stable deposition/stripping of aluminium occurs on the anode. On the other hand, the electrolyte contributes to the electrochemical energy storage through an iron redox reaction. These two reactions are parallel and coupled through an Fe-Al alloy on the anode, thus enhancing the reversibility and energy density of AAIBs. As a result, this hybrid-ion battery delivers a specific volumetric capacity of 35 A h L-1 at the current density of 1.0 mA cm-2, and remarkable stability with a capacity retention of 90% over 500 cycles. Furthermore, the hybrid-ion battery achieves a high energy density of approximately 42 W h L-1 with an average operating voltage of 1.1 V. This green electrolyte for high-energy AAIBs holds promises for large-scale energy storage applications.
Project description:Aluminum single crystal with 99.999% purity was deformed at room temperature by equal channel angular pressing (ECAP) up to 16 passes. Grain size and misorientation of processed samples were quantitatively characterized by TEM and EBSD. The results show that the refinement efficiency of high purity aluminum single crystal was poor in the initial stage. Extrusion by fewer ECAP passes (n ≤ 8) resulted in only elongated grains containing a large number of subgrains and small misorientations between grains. Stable microstructures of nearly equiaxed grains with high misorientations were obtained by 15 passages, indicating that the initial extremely coarse grains and highly uniform grain orientation are not conducive to the accumulation of strain energy. The initial state of high purity aluminum has a significant effect on the refining efficiency of the ECAP process.
Project description:Two-dimensional van der Waals materials have emerged as promising platforms for solid-state quantum information processing devices with unusual potential for heterogeneous assembly. Recently, bright and photostable single photon emitters were reported from atomic defects in layered hexagonal boron nitride (hBN), but controlling inhomogeneous spectral distribution and reducing multi-photon emission presented open challenges. Here, we demonstrate that strain control allows spectral tunability of hBN single photon emitters over 6 meV, and material processing sharply improves the single photon purity. We observe high single photon count rates exceeding 7 × 106 counts per second at saturation, after correcting for uncorrelated photon background. Furthermore, these emitters are stable to material transfer to other substrates. High-purity and photostable single photon emission at room temperature, together with spectral tunability and transferability, opens the door to scalable integration of high-quality quantum emitters in photonic quantum technologies.Inhomogeneous spectral distribution and multi-photon emission are currently hindering the use of defects in layered hBN as reliable single photon emitters. Here, the authors demonstrate strain-controlled wavelength tuning and increased single photon purity through suitable material processing.
Project description:High-temperature sodium-sulfur batteries operating at 300-350 °C have been commercially applied for large-scale energy storage and conversion. However, the safety concerns greatly inhibit their widespread adoption. Herein, we report a room-temperature sodium-sulfur battery with high electrochemical performances and enhanced safety by employing a "cocktail optimized" electrolyte system, containing propylene carbonate and fluoroethylene carbonate as co-solvents, highly concentrated sodium salt, and indium triiodide as an additive. As verified by first-principle calculation and experimental characterization, the fluoroethylene carbonate solvent and high salt concentration not only dramatically reduce the solubility of sodium polysulfides, but also construct a robust solid-electrolyte interface on the sodium anode upon cycling. Indium triiodide as redox mediator simultaneously increases the kinetic transformation of sodium sulfide on the cathode and forms a passivating indium layer on the anode to prevent it from polysulfide corrosion. The as-developed sodium-sulfur batteries deliver high capacity and long cycling stability.
Project description:A computational data-driven approach is applied to the design of liquid electrolyte materials for a complex phenomenon, viz. electrochemical deposition. A protocol for the liquid electrolyte material exploration consists of (i) structure optimization, (ii) reduction mechanism elucidation, and (iii) computational screening. A case study is conducted targeting glyme-based room-temperature aluminum (Al) electroplating solutions, where how to achieve a higher plating speed has been an open issue. The determination of stable Al-Cl-glyme complex structures by density functional theory calculations enables the modeling for molecular dynamics simulations of the bulk electrolytes, namely, aluminum chloride (AlCl3)-diglyme (G2)-cosolvent system. It is shown that a tridentate coordination of diglyme (G2) to [AlCl2]+ is robust against desolvation and one-electron reduction, suggesting that the diffusion coefficients of the [AlCl2]+ cationic complex are an indication of faster plating. Additionally, the calculated diffusion coefficients correlate weakly with the relative permittivity data of cosolvents in their pure state but strongly with viscosity data. This relationship can be used to design Al plating solutions.
Project description:Tracheal intubation constitutes a routine part in the care of critically ill and anaesthetised patients. Prolonged use of endotracheal with inflated cuff is one of the major multifactorial causes of complications. Both under-inflation and over-inflation of cuff are associated with complications. Despite known problems, regular measurement of cuff pressure is not routine, and it is performed on an ad hoc basis.
Project description:The uniform temperature distribution, one of the requirements for long-term durability, is essential for composite heaters. An analytical model for temperature distribution of a tube-type heater was derived, and it revealed that thickness uniformity is one order more important than intrinsic material properties such as density, heat capacity, and electrical conductivity of the heating tube. We introduced a circumferential shearing process to fabricate a flexible, seamless tube-type heating layer of carbon nanotube/silicone rubber composite with outstanding uniform distribution of thickness and temperature, which may be attributed to a shorter characteristic dimension in the circumferential direction than in the axial direction. The temperature uniformity was experimentally verified at various temperatures under heating. The difference in measured thickness and temperature in circumferential direction was within ±1.3~3.0% (for tavg = 352.7 μm) and ±1.1% (for Tavg = 138.8 °C), respectively, all over the heating tube. Therefore, the circumferential shearing process can be effective for cylindrical heaters, like a heating layer of a laser printer, which fuse toners onto papers during printing.
Project description:Highly efficient subtractive tri-color filters of cyan, magenta, and yellow with enhanced color purity and robustness have been proposed and realized, by exploiting a silicon-aluminum (Si-Al) hybrid-nanodisk (ND) metasurface atop a Si substrate. The aspect ratio of the Si-Al hybrid ND is much lower than that of the conventional Si nanowire, which is disadvantageous due to its fragility and low color purity. In response to incident light impinging upon the metasurface, the hybrid-NDs individually play the role in exciting a magnetic dipole (MD) resonance through the mediation of Mie-scattering between the hybrid ND and air. The light stored in the resonance is coupled to the substrate, giving rise to a suppressed reflection. By virtue of the top Al ND, the excited MD resonance is strongly confined by the Si ND. As a consequence, a near-zero resonant dip that exhibits high off-resonance reflection and narrow bandwidth is produced for embodying highly efficient tri-color filters with enhanced color purity. The spectral position can be tuned by a simple adjustment of the hybrid-ND diameter. A full-color palette was successfully created with a high color purity and large color gamut. The proposed devices may be applied for photorealistic high-resolution color printing and holographic displays.
Project description:The development of highly active, reusable catalysts for aqueous-phase reactions is challenging. Herein, metallic nickel is encapsulated in a nitrogen-doped carbon-silica composite (SiO2@Ni@NC) as a catalyst for the selective hydrogenation of vanillin in aqueous media. The constructed catalyst achieved 99.8% vanillin conversion and 100% 4-hydroxymethyl-2-methoxyphenol selectivity at room temperature. Based on combined scanning transmission electron microscopy, X-ray photoelectron spectroscopy, and Raman analyses, the satisfactory catalytic performance is attributed to the composite structure consisting of an active metal, carbon, and silica. The hydrophilic silica core promoted dispersion of the catalyst in aqueous media. Moreover, the external hydrophobic NC layer has multiple functions, including preventing oxidation or leaching of the internal metal, acting as a reducing agent to reduce the internal metal, regulating the active-site microenvironment by enriching the concentrations of H2 and organic reactants, and modifying the electronic structure of the active metal via metal-support interactions. Density functional theory calculations indicated that NC facilitates vanillin adsorption and hydrogen dissociation to promote aqueous-phase hydrogenation. This study provides an efficient strategy for constructing encapsulated Ni-based amphiphilic catalysts to upgrade biomass-derived compounds.