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Scientific and Technological Research Program of Chongqing Municipal Education Commission[HZ2021013]
Template-Assisted Synthesis of Porous Manganese Dioxide Hollow Rods as Supercapacitor Electrode Material
We propose a facile template strategy for fabrication of porous delta manganese dioxide (delta-MnO2) hollow rods under mild conditions. First, highly dispersible molybdenum oxide (MoO3) rods were hydrothermally prepared. Next, MoO3/carbon (MoO3/C) composite rods were further synthesized by wrapping a MoO3 substrate with a polypyrrole thin layer through the oxidative polymerization of pyrrole, followed by annealing in an inert atmosphere. Finally, porous delta-MnO2 hollow rods were produced by redox reaction between the carbon component of MoO3/C and potassium permanganate (KMnO4), followed by total dissolution of MoO3 template. Such developed delta-MnO2 hollow rods were systematically characterized and found to show impressive electrochemical properties with the maximum specific capacitance of 171.3 F g(-1), satisfactory rate performance and exceptional cycle stability with capacitance retention as high as 90.5% even after repetitively charging/discharging for over 10,000 cycles. The remarkable supercapacitive behavior of porous delta-MnO2 hollow rods surpass those of many MnO2-based electrode materials, thus featuring the potential for development of advanced energy storage devices
Reactive template-derived interfacial engineering of CoP/CoO heterostructured porous nanotubes towards superior electrocatalytic hydrogen evolution
The development of economical, efficient, and robust electrocatalysts toward the hydrogen evolution reaction (HER) is highly imperative for the rapid advancement of renewable H-2 energy-associated technologies. Extensive utilization of the heterointerface effect can endow the catalysts with remarkably boosted electrocatalytic performance due to the modified electronic state of active sites. Herein, we demonstrate deliberate crafting of CoP/CoO heterojunction porous nanotubes (abbreviated as CoP/CoO PNTs hereafter) using a self-sacrificial template-engaged strategy. Precise control over the Kirkendall diffusion process of the presynthesized cobalt-aspartic acid complex nanowires is indispensable for the formation of CoP/CoO heterostructures. The topochemical transformation strategy of the reactive templates enables uniform and maximized construction of CoP/CoO heterojunctions throughout all the porous nanotubes. The establishment of CoP/CoO heterojunctions could considerably modify the electronic configuration of the active sites and also improve the electric conductivity, which endows the resultant CoP/CoO PNTs with enhanced intrinsic activity. Simultaneously, the hollow and porous nanotube architectures allow sufficient accessibility of exterior/interior surfaces and molecular permeability, drastically promoting the reaction kinetics. Consequently, when used as HER electrocatalysts, the well-designed CoP/CoO PNTs show Pt-like activity, with an overpotential of only 61 mV at 10 mA cm(-2) and excellent stability in 1.0 M KOH medium, exceeding those of the vast majority of the previously reported nonprecious candidates. Density functional theory calculations further substantiate that the construction of CoP/CoO heterojunctions enables optimization of the Gibbs free energies for water adsorption and H adsorption, resulting in boosted HER intrinsic activity. The present study may provide in-depth insights into the fundamental mechanisms of heterojunction-induced electronic regulation, which may pave the way for the rational design of advanced Earth-abundant electrocatalysts in the future
Application of Pt loaded graphite felt in SO2-depolarized electrolyzer
The three-dimensional anodes for SO2 depolarized electrolysis (SDE) cells are prepared by loading Pt/C on high void content graphite felts, with the method of ultrasonic spray and vacuum suction. SEM results confirm the three-dimensional space distribution of Pt in graphite felts, which ensures sufficient contact between Pt/C and SO2 in anolyte. Comparing with the two-dimensional anodic catalyst layer loaded on the proton exchange membrane in a conventional SDE cell, the application of the three-dimensional anode decreases cell impedance greatly and improves the SDE performance significantly. In this study, 0.63 mg/cm(2) Pt loading amount shows the best performance when Pt/C is double-side-sprayed on graphite felt, and the current density reaches 1.24 A/cm(2) at cell voltage of 1.2 V, as operating at 60 ? and anolyte flow rate of 360 mL/min. The effects of the Pt loading amount, operating temperature and anolyte flow rate on the SDE performance are investigated. (C) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved
Comparison of magnetite/reduced graphene oxide nanocomposites and magnetite nanoparticles on enhancing hydrogen production in dark fermentation
Magnetite/reduced graphene oxide nanocomposites (Fe3O4-rGO NCs) and magnetite nanoparticles (Fe3O4 NPs) were added to enhance biohydrogen (bioH(2)) production in dark fermentation. Concentration of supplements from 10 to 100 mg/L was appropriate to enhance bioH(2) production, and inhibition appeared once concentration exceeded 100 mg/L. The best bioH(2) yield was 198.30 mL/g glucose at 100 mg/L Fe3O4 NPs and 225.60 mL/g glucose at 100 mg/L Fe3O4-rGO NCs, which was 42.97% and 62.65% higher than that in the blank group, respectively. Both Fe3O4 NPs and Fe3O4-rGO NCs could intensify butyrate-type fermentation and change the hydrogen-producing microorganism cells morphology, but the enhancement effect of Fe3O4-rGO NCs was superior. Microbial community structure analysis showed that Clostridium-sensu-stricto-1 became more dominant ultimately by Fe3O4-rGO NCs. (C) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved
Abatement of dichloromethane with high selectivity over defect-rich MOF-derived Ru/TiO2 catalysts
The regulation of oxygen vacancies and Ru species using metal-organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO2 and Ru/N-TiO2 catalysts were synthesized by the pyrolysis of MIL-125 and NH2-MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at similar to 290 degrees C over Ru/M-TiO2 and Ru/N-TiO2 catalysts, while Ru/N-TiO2 showed quite less monochloromethane (MCM) and higher CO2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO2, compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO2. Additionally, Ru/N-TiO2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts
Synthesis of poly(1,2-butylene oxide-stat-tetrahydrofuran) by controllable polymerization over Sc(OTf)(3) for use in high-performance lubricating oil
Aliphatic polyethers are synthesized byring-opening polymerization (ROP) of the most common epoxide monomers, such as ethylene oxide (EO) and propylene oxide (PO). 1,2-Butylene oxide (BO) and tetrahydrofuran (THF) are potentially extended ROP monomers, which can give polyether unique properties. In this work, a series of poly(1,2-butylene oxide-stat-tetrahydrofuran)s (PBO-stat-PTHFs) with M-n, of 900-3700 g.mol(-1) were synthesized by cationic ring-opening polymerization (CROP) of BO with THF using strong Lewis acid Rare Earth triflates (RE(OTf)(3)) as catalysts and diols as an initiator at room temperature. PBO-stat-PTHFs product with yield up to 90 %, narrow polydispersity of D = 198) and low pour point (<=-53 degrees C), which can be used as a lubricant base oil and additives. In addition, PBO-stat-PTHFs have excellent miscibility with polyalphaolefin (PAO), which could significantly improve the PAO viscosity index. This study provides a mild mute to construct high-performance copolyether materials through cationic ring-opening controllable polymerization