Ammonia production using iron nitride and water as hydrogen source under mild temperature and pressure

Ammonia generation was studied in the reaction between water and nitrogen-containing iron at 323 K and atmospheric pressure. Similar to metallic Fe, the interstitial compound Fe₃N reduced water through Fe oxidation to produce hydrogen gas, while the N combined with atomic hydrogen to produce ammonia as a byproduct. The addition of carbon dioxide to this system accelerated the reaction with concomitant consumption of carbon dioxide. The promoted ammonia production upon addition of carbon dioxide can be attributed to the generation of atomic hydrogen from the redox reaction of carbonic acid and Fe, as well as removal of used Fe from the reaction system through the formation of a soluble carbonato complex. When carbonate was added to the reaction system, the production rates of ammonia and hydrogen increased further. The results here confirmed that ammonia can be synthesized from iron nitride under mild conditions by utilizing carbon dioxide.     

Carbon corrosion mechanism on nitrogen-doped carbon support — A density functional theory study

In this work, density functional theory (DFT) calculations were used to investigate the mechanism of carbon corrosion on nitrogen-doped carbon support. Free energy diagrams were generated based on three proposed reaction pathways to evaluate corrosion mechanisms. The most energetically preferred mechanism on nitrogen-doped carbon was determined. The results show that the step of water dissociation to form ^#OH was the rate-determining step for gra-G-1N (graphene doped with graphitic N) and pyrr-G-1N (graphene doped with pyrrolic N). As for graphene doped with pyridinic N, the step of C^#OC^#O formation was critical. It was found that the control of nitrogen concentration was necessary for precisely designing optimized carbon materials. Abundance of nitrogen moieties aggravated the carbon corrosion. When the high potential was applied, specific types of graphitic N and pyridinic N were found to be favorable carbon modifications to improve carbon corrosion resistance. Moreover, the solvent effect was also investigated. The results provide theoretical insights and design guidelines to improve corrosion resistance in carbon support through material modification by inhibiting the adsorption of surface oxides (OH, O, and OOH).     

The dynamic effect of Micro-MHD convection on bubble grown at a horizontal microelectrode

Relatively low efficiency is the biggest obstacle to the popularization of water electrolysis, which is a particularly feasible way to produce super-pure hydrogen. Imposing a magnetic field can increase the hydrogen production efficiency of water electrolysis. However, the enhancement's detailed mechanism still lacks an insightful understanding of the bubbles' micro vicinity. Our recent work aims to understand why the micro-magnetohydrodynamic (MHD) convection hinders single bubbles' detachment on the microelectrode. A water electrolysis experiment by microelectrode is performed under an electrode-normal magnetic field, and dynamic analysis of the single bubble growing on microelectrodes is performed. The variation of bubble diameter with time in the presence or absence of the magnetic field was measured, and the forces acting on the bubble were quantified. The result shows that the micro-MHD convection, induced by Lorentz force, can give rise to a downward hydrodynamic pressure force that will not appear in large-scale MHD convection. This force can be of the same magnitude as the surface tension, so it dramatically hinders bubbles' detachment. Besides, the Kelvin force provides a new potential way for further improving the efficiency of water electrolysis.     

Preparation of high-activity coal char-based catalysts from high metals containing coal gangue and lignite for catalytic decomposition of biomass tar

The potential of using high metals containing coal gangue and lignite to prepare high-activity coal char-based catalysts is investigated for effective biomass tar decomposition. Loose structure and rough surface are formed for these char-based catalysts with heterogeneous distribution of a large number of inorganic particles. In the biomass tar decomposition, the performance of the coal char-based catalysts is significantly influenced by the content of the metals in the raw materials and coal gangue char (GC) with the ash content as high as 50.80% exhibits the highest activity in this work. A high biomass tar conversion efficiency of 93.5% is achieved at 800 °C along with a significant increase in the fuel gas product. During the five-time consecutive tests, the catalytic performance of GC increases a little at the second or third times reuse and remains relatively stable, showing the remarkable stability of the catalyst in biomass tar decomposition applications.     

新时期加强消防装备运行保障能力的思考

改革转制以来,消防救援队伍被赋予了更加多样化的职能职责,各类专业化消防装备的作用愈发凸显,其不但是消防救援队伍及时完成各类灭火救援任务的基本保障,也是日常消防救援训练的物资基础.因而,如何构建消防救援队伍装备运行保障体系,确保关键时刻能充分发挥使用价值,成为了当下的一个重要课题.基于此,文章简单分析加强消防装备运行保障能力的相关知识,希望对相关领域研究有所帮助.     

Estimating long-term time-resolved indoor PM2.5 of outdoor and indoor origin using easily obtainable inputs

To evaluate the separate impacts on human health and establish effective control strategies, it is crucial to estimate the contribution of outdoor infiltration and indoor emission to indoor PM_2.5 in buildings. This study used an algorithm to automatically estimate the long-term time-resolved indoor PM_2.5 of outdoor and indoor origin in real apartments with natural ventilation. The inputs for the algorithm were only the time-resolved indoor/outdoor PM_2.5 concentrations and occupants’ window actions, which were easily obtained from the low-cost sensors. This study first applied the algorithm in an apartment in Tianjin, China. The indoor/outdoor contribution to the gross indoor exposure and time-resolved infiltration factor were automatically estimated using the algorithm. The influence of outdoor PM_2.5 data source and algorithm parameters on the estimated results was analyzed. The algorithm was then applied in four other apartments located in Chongqing, Shenyang, Xi'an, and Urumqi to further demonstrate its feasibility. The results provided indirect evidence, such as the plausible explanations for seasonal and spatial variation, to partially support the success of the algorithm used in real apartments. Through the analysis, this study also identified several further development directions to facilitate the practical applications of the algorithm, such as robust long-term outdoor PM_2.5 monitoring using low-cost light-scattering sensors.     

Lithiation MXene Derivative Skeletons for Wide-Temperature Lithium Metal Anodes

Lithium (Li) metal, as an appealing candidate for the next-generation of high-energy-density batteries, is plagued by its safety issue mainly caused by uncontrolled dendrite growth and infinite volume expansion. Developing new materials that can improve the performance of Li-metal anode is one of the urgent tasks. Herein, a new MXene derivative containing pure rutile TiO₂ and N-doped carbon prepared by heat-treating MXene under a mixing gas, exhibiting high chemical activity in molten Li, is reported. The lithiation MXene derivative with a hybrid of LiTiO₂-Li₃N-C and Li offers outstanding electrochemical properties. The symmetrical cell assembling lithiation MXene derivative hybrid anode exhibits an ultra-long cycle lifespan of 2000 h with an overpotential of ≈30 mV at 1 mA cm⁻², which overwhelms Li-based anodes reported so far. Additionally, long-term operations of 34, 350, and 500 h at 10 mA cm⁻² can be achieved in symmetrical cells at temperatures of −10, 25, and 50 °C, respectively. Both experimental tests and density functional theory calculations confirm that the LiTiO₂-Li₃N-C skeleton serves as a promising host for Li infusion by alleviating volume variation. Simultaneously, the superlithiophilic interphase of Li₃N guides Li deposition along the LiTiO₂-Li₃N-C skeleton to avoid dendrite growth.     

Facile synthesis of MgO–Mg2SiO4 composite ceramics with high strength and low thermal conductivity

The recycling of solid waste is a win-win solution for humans and nature. For this purpose, magnesite tailings and silicon kerf waste were employed to prepare MgO–Mg₂SiO₄ composite ceramics by solid-state reaction synthesis in the present work. Then, effects of sintering temperature and raw material ratio on as-prepared ceramics were systematically studied. As-prepared ceramics showed improvement in their relative density (from 47.55%–68.12% to 90.96%–95.25%) and cold compressive strength (from 7.34–118.66 MPa to 303.39–546.65 MPa) with the increase in sintering temperature from 1300 to 1600 °C. In addition, it was found that Si promoted synthesis process of Mg₂SiO₄ phase through transient liquid phase sintering and Fe₂O₃ accelerated sintering process through activation sintering. Consequently, the presence of Mg₂SiO₄ phase effectively improved the density and strength of MgO–Mg₂SiO₄ composite ceramic, while reducing its thermal conductivity. This work provides a potential reutilization strategy for magnesite tailings, and as-prepared products are expected to be applied in fields of construction, metallurgy, and chemical industry.     

Ratiometric Detection of Glutathione Based on Disulfide Linkage Rupture between a FRET Coumarin Donor and a Rhodamine Acceptor

Abnormal levels of glutathione, a cellular antioxidant, can lead to a variety of diseases. We have constructed a near-infrared ratiometric fluorescent probe to detect glutathione concentrations in biological samples. The probe consists of a coumarin donor, which is connected through a disulfide-tethered linker to a rhodamine acceptor. Under the excitation of the coumarin donor at 405 nm, the probe shows weak visible fluorescence of the coumarin donor at 470 nm and strong near-infrared fluorescence of the rhodamine acceptor at 652 nm due to efficient Forster resonance energy transfer (FRET) from the donor to the acceptor. Glutathione breaks the disulfide bond through reduction, which results in a dramatic increase in coumarin fluorescence and a corresponding decrease in rhodamine fluorescence. The probe possesses excellent cell permeability, biocompatibility, and good ratiometric fluorescence responses to glutathione and cysteine with a self-calibration capability. The probe was utilized to ratiometrically visualize glutathione concentration alterations in HeLa cells and Drosophila melanogaster larvae.