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1. Kinetics of Fischer–Tropsch Synthesis in a 3-D Printed Stainless Steel Microreactor Using Different Mesoporous Silica Supported Co-Ru Catalysts

   Mohammad, Nafeezuddin; Bepari, Sujoy; Aravamudham, Shyam; Kuila, Debasish (October 2019, Catalysts)

   Fischer–Tropsch (FT) synthesis was carried out in a 3D printed stainless steel (SS) microchannel microreactor using bimetallic Co-Ru catalysts on three different mesoporous silica supports. CoRu-MCM-41, CoRu-SBA-15, and CoRu-KIT-6 were synthesized using a one-pot hydrothermal method and characterized by Brunner–Emmett–Teller (BET), temperature programmed reduction (TPR), SEM-EDX, TEM, and X-ray photoelectron spectroscopy (XPS) techniques. The mesoporous catalysts show the long-range ordered structure as supported by BET and low-angle XRD studies. The TPR profiles of metal oxides with H2 varied significantly depending on the support. These catalysts were coated inside the microchannels using polyvinyl alcohol and kinetic performance was evaluated at three different temperatures, in the low-temperature FT regime (210–270 °C), at different Weight Hourly Space Velocity (WHSV) in the range of 3.15–25.2 kgcat.h/kmol using a syngas ratio of H2/CO = 2. The mesoporous supports have a significant effect on the FT kinetics and stability of the catalyst. The kinetic models (FT-3, FT-6), based on the Langmuir–Hinshelwood mechanism, were found to be statistically and physically relevant for FT synthesis using CoRu-MCM-41 and CoRu-KIT-6. The kinetic model equation (FT-2), derived using Eley–Rideal mechanism, is found to be relevant for CoRu-SBA-15 in the SS microchannel microreactor. CoRu-KIT-6 was found to be 2.5 times more active than Co-Ru-MCM-41 and slightly more active than CoRu-SBA-15, based on activation energy calculations. CoRu-KIT-6 was ~3 and ~1.5 times more stable than CoRu-SBA-15 and CoRu-MCM-41, respectively, based on CO conversion in the deactivation studies. Keywords: Fischer-Tropsch synthesis; mesoporous silica based catalysts; kinetic studies; 3-D printed microchannel microreactor 

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2. Prussian blue-assisted one-pot synthesis of nitrogen-doped mesoporous graphitic carbon spheres for supercapacitors

   https://doi.org/10.1039/C9TA08454A  

   Dassanayake, Arosha C.; Wickramaratne, Nilantha P.; Hossain, Mohammad Akter; Perera, Vindya S.; Jeskey, Jacob; Huang, Songping D.; Shen, Hao; Jaroniec, Mietek (October 2019, Journal of Materials Chemistry A)

   Synthesis of nitrogen doped mesoporous graphitic carbon spheres with dispersed metal oxide nanoparticles using a single temperature treatment step serves as one of the big challenges in materials research. To date only a few reports have been published on the soft-templating synthesis of mesoporous graphitic carbons. The preparation of graphitic carbons with dispersed Fe 2 O 3 using a single carbonization step at relatively low temperatures is yet to be explored. The first phase of this work shows the potential of graphitization of polyvinylpyrrolidine (PVP) stabilized cubic Prussian blue nanoparticles (CPB) in phenolic resin spheres to produce graphitic carbon spheres through a facile Stöber-like method. In the second phase, the Pluronic F127 soft template was used along with PVP stabilized Prussian blue nanoparticles (PB) in carbon spheres to generate mesopores and graphitic domains with uniformly dispersed Fe 2 O 3 nanoparticles in these spheres. Due to the presence of graphitic layers, doped N species and Fe 2 O 3 nanoparticles in the carbon matrix, the yielded carbon spheres feature a high surface area and magnetic properties. Moreover, these graphitic spheres exhibited excellent capacitive behavior with rectangular cyclic voltammetry (CV) profiles and large capacitance up to 247 F g −1 at 1 mV s −1 scan rate in 6 M KOH solution. 

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3. An interpretation for the components of 2p _3/2 core level x-ray photoelectron spectra of the cations in some inverse spinel oxides

   https://doi.org/10.1088/1361-648X/ad3271  

   Subedi, Arjun; Yang, Detian; Chin, Wai Kiat; Tamang, Binny; Sahoo, Sushrisangita; Yancey, Paul; Mahbub, Rifat; Shield, Jeffrey; Lai, Rebecca Y; Xu, Xiaoshan; et al (April 2024, Journal of Physics: Condensed Matter)

   Abstract In an effort to reconcile the various interpretations for the cation components of the 2p_3/2observed in x-ray photoelectron spectroscopy (XPS) of several spinel oxide materials, the XPS spectra of both spinel alloy nanoparticles and crystalline thin films are compared. We observed that different components of the 2p_3/2core level XPS spectra, of these inverse spinel thin films, are distinctly surface and bulk weighted, indicating surface-to-bulk core level shifts in the binding energies. Surface-to-bulk core level shifts in binding energies of Ni and Fe 2p_3/2core levels of NiFe₂O₄thin film are observed in angle-resolved XPS. The ratio between surface-weighted components and bulk-weighted components of the Ni and Fe core levels shows appreciable dependency on photoemission angle, with respect to surface normal. XPS showed that the ferrite nanoparticles Ni_xCo_1−xFe₂O₄(x= 0.2, 0.5, 0.8, 1) resemble the surface of the NiFe₂O₄thin film. Surface-to-bulk core level shifts are also observed in CoFe₂O₄and NiCo₂O₄thin films but not as significantly as in NiFe₂O₄thin film. Estimates of surface stoichiometry of some spinel oxide nanoparticles and thin films suggested that the apportionment between cationic species present could be farther from expectations for thin films as compared to what is seen with nanoparticles. 

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4. Experimental Studies of Carbon Electrodes With Various Surface Area for Li–O2 Batteries

   https://doi.org/10.1115/1.4043229  

   Wang, Fangzhou; Kahol, P. K.; Gupta, Ram; Li, Xianglin (April 2019, Journal of Electrochemical Energy Conversion and Storage)

   Li−O2 batteries with carbon electrodes made from three commercial carbons and carbon made from waste tea leaves are investigated in this study. The waste tea leaves are recycled from household tea leaves and activated using KOH. The carbon materials have various specific surface areas, and porous structures are characterized by the N2 adsorption/desorption. Vulcan XC 72 carbon shows a higher specific surface area (264.1 m2/g) than the acetylene black (76.5 m2/g) and Super P (60.9 m2/g). The activated tea leaves have an extremely high specific surface area of 2868.4 m2/g. First, we find that the commercial carbons achieve similar discharge capacities of ∼2.50 Ah/g at 0.5 mA/cm2. The micropores in carbon materials result in a high specific surface area but cannot help to achieve higher discharge capacity because it cannot accommodate the solid discharge product (Li2O2). Mixing the acetylene black and the Vulcan XC 72 improves the discharge capacity due to the optimized porous structure. The discharge capacity increases by 42% (from 2.73 ± 0.46 to 3.88 ± 0.22 Ah/g) at 0.5 mA/cm2 when the mass fraction of Vulcan XC 72 changes from 0 to 0.3. Second, the electrode made from activated tea leaves is demonstrated for the first time in Li−O2 batteries. Mixtures of activated tea leaves and acetylene black confirm that mixtures of carbon material with different specific surface areas can increase the discharge capacity. Moreover, carbon made from recycled tea leaves can reduce the cost of the electrode, making electrodes more economically achievable. This study practically enhances the discharge capacity of Li−O2 batteries using mixed carbons and provides a method for fabricating carbon electrodes with lower cost and better environmental friendliness. 

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5. Cr and CeO2 promoted Ni/SBA-15 framework for hydrogen production by steam reforming of glycerol

   Abrokwah, R; Ntow, E; Jennings, T; Stevens_Boyd, R; Hossain, T; Swain, J; Bepari, S; Hassan, S; Mohammad, N; Kuila, D (November 2023, Steel in translation)

   Ni/SBA-15 meso-structured catalysts modified with chromium and CeO2 (Ni–Cr-CeO2/SBA-15) were utilized to produce hydrogen from glycerol steam reforming (GSR). The catalysts were synthesized by a one-pot hydrothermal process and extensively characterized by analytical techniques such as N2 adsorption–desorption (BET), H2-temperature programmed reduction (H2-TPR), powder X-ray diffraction (PXRD), inductively coupled plasma-optical emission spectrometry (ICP-OES), and transmission electron microscopy (TEM). The low-angle XRD reflections affirmed that the catalysts were crystalline and possessed a 2D-ordered porosity. The BET results depicted that all the catalysts exhibited a good surface area ranging from 633 to 792m2/g, and the pore sizes were consistently in the mesoporous range (between 3 and 5 nm). TEM analysis of both calcined and spent catalysts revealed that the metal active sites were embedded in the hybrid CeO2-SiO2 support. Overall, the Ni-based catalysts exhibited higher glycerol conversion -12Ni-SBA-15–99.9%, 12Ni3CeO2-SBA-15–89.4%, and 8Ni4Cr3CeO2-SBA-15–99.7%. Monometallic 12Ni/SBA-15 performed exceptionally well, while 12Cr/SBA-15 performed poorly with the highest 71.48% CO selectivity. For short-term GSR reactions, CeO2 addition to 12Ni/SBA-15 did not have any effect, whereas Cr addition resulted in a 32% decrease in H2 selectivity. The long-term stability studies of 12Ni-SBA-15 showed H2 selectivity of ~ 64% and ~ 98% glycerol conversion. However, its activity was short-lived. After 20–30 h, the H2 selectivity and conversion dropped precipitously to 40%. The doping of mesoporous Ni/SBA-15 with Cr and CeO2 remarkably enhanced the long-term stability of the catalyst for 12Ni3CeO2-SBA-15, and 8Ni4Cr3CeO2-SBA-15 catalyst which showed ~ 58% H2 selectivity and ~ 100% conversion for the entire 60 h. Interestingly, Cr and CeO2 seem to improve the shelf-life of Ni-SBA-15 via different mechanistic pathways. CeO2 mitigated Ni poisoning through coke oxidation whereas Cr bolstered the catalyst stability via maintaining a well-defined pore size, structural rigidity, and integrity of the heterogeneous framework, thereby restricting structural collapse, and hence retard sintering of the Ni active sites during the long-term 60 h of continuous reaction. Hydrogen generation from renewable biomass like glycerol could potentially serve as a sustainable energy source and could substantially help reduce the carbon footprint of the environment 

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