Department of Chemical Engineering
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Item Steam reforming of ethanol for hydrogen production by low-temperature steam reforming using modified Ni-Sn/CeO2 catalyst(Elsevier, 2023) Roy, Banasri; Srinivas, AppariThis study focuses on the development of Ni-Sn bimetallic catalysts supported on ZrO2 modified CeO2 and their application for low temperature steam reforming of ethanol (LTSRE) at different temperature 200–400 °C. The catalyst powders are prepared by an ultrasonic-assisted solution combustion synthesis method. The ethanol conversion and selectivity of H2, CO2, CO, and CH4 has been studied with feed composition H2O:EtOH = 12: 1 mol ratio, feed flow rate 0.1 cc/min, and reaction time 20 hrs. Fresh and spent catalysts are characterized using XRD, FTIR, Raman, FESEM, XPS, and TGA-DTA. ZrO2 changes the support chemistry and enhances the activity and stability of the catalyst. At 400 °C, 100 % ethanol (EtOH) conversion, 69 % H2 selectivity with least coke deposition is observed for the catalyst with 5 wt% metal (Ni:Sn = 14:1) loading on Ce:Zr 1:2 mol ratio (NiSn5/CZ12) support.Item Tin and lanthanum modified Ni/CeO2 catalyst systems for low temperature steam reforming of ethanol(Elsevier, 2024-01) Roy, BanasriThis work examines the Ni–Sn/Ce–La–O catalyst systems for low-temperature stream reforming of ethanol. Catalysts of 5 and 20 wt% metal loading, and different Ce:La ratios are prepared by ultra-sonication assisted solution combustion synthesis method. Catalysts at total metal loading 5 wt% with 33 and 67 at. % La and optimum Sn (Ni:Sn = 14:1) demonstrate better efficiency compared to the Ni/CeO2 catalysts. At 20 wt% metal loading and Ni:Sn = 1:1 atomic ratio, catalytic activity degrades. The best activity and stability are revealed for the N14S1(5)/CL21 catalyst with 5 wt.% total metal loading, Ni:Sn = 14:1, and Ce:La = 2:1 mol ratio. Physico-chemical characterizations (XRD, H2 -TPR, NH3-TPD, Raman, FESEM, TEM, XPS, N2 adsorption-desorption, DTA/TGA, etc.) are performed to understand the role of the metal loading, Sn, and La in the catalytic activity and coke deposition behavior.Item Study of preparation method and oxidization/reduction effect on the performance of nickel-cerium oxide catalysts for aqueous-phase reforming of ethanol(Elsevier, 2015-12) Roy, BanasriThe effect of preparation method and oxidation state of the active metal on the catalytic activity of Ni–Ce–O catalysts was studied for aqueous phase reforming of ethanol. A sol-gel (SG) route and a solution combustion synthesis (SCS) method were used for the preparation of 10 wt% Ni loaded catalysts. The catalytic activity of three groups of catalysts; reduced at 425 °C (HR, metallic Ni), reduced at 1000 °C (FR, metallic Ni), and not reduced (NR, as NiO) were tested at different operating conditions. The difference in the metal particle sizes, governed by the preparation method, affects the catalytic efficiency most, not the reduced or oxidized state of Ni. The SG samples were superior for ethanol conversion and selectivity for H2 and CO2 compared to the SCS samples. The X-ray photoelectron spectroscopy (XPS) analysis of the samples demonstrated that the relative ratio of Ce2O3 to CeO2 increased inside the reactor. While Ni doping increases oxygen mobility in the Ce–O lattice, Ce3+ converts Ni2+ to metallic Ni inside the reactor. This can explain why the reduction stage for Ni–Ce–O system in APR is irrelevant. Higher oxygen mobility through the support helps oxidation of CO to CO2 leading to improved catalytic performance.Item Effects of metal loading and support modification on the low-temperature steam reforming of ethanol (LTSRE) over the Ni–Sn/CeO2 catalysts(Elsevier, 2023-05) Roy, Banasri; Srinivas, AppariThis article presents the effect of metal loading and support modification with MgO on low-temperature steam reforming of ethanol (LTSRE) over Ni–Sn/CeO2 catalysts prepare by a single-pot solution combustion synthesis (SCS) method. Atmospheric pressure activity study of these catalysts (0.5 g) is performed at different temperatures (200–400 °C), H2O:EtOH = 12: 1 mol ratio, and feed flow rate 0.1 ml/min. After 10 h TOS at 400 °C, NiSn(5)/CM12 catalyst with 5 wt.% total metal loading, optimal Sn (Ni:Sn = 14:1), and Ce:Mg = 1:2 mol ratio shows EtOH conversion 100% and H2 selectivity 70% with low coke deposition. Physicochemical characterizations (XRD, Raman, FESEM, TEM, and N2 adsorption-desorption) reveal that addition of MgO in CeO2 and an optimal amount of Sn decrease both Ni and support particle sizes while oxygen storage capacity (OSC) of the support increases (by XPS). Alkaline characteristics of MgO reduces support's acidity and improves active metal-support interaction, as evaluated by NH3-TPD and H2-TPR.Item Effect of variable conditions on steam reforming and aqueous phase reforming of n-butanol over Ni/CeO2 and Ni/Al2O3 catalysts(Elsiever, 2014-12-01) Roy, BanasriA comparison of aqueous phase reforming (APR) and steam reforming (SR) of n-butanol (n-BuOH) over Ni(20 wt%) loaded Al2O3 and CeO2 catalysts has been discussed in this paper. The BuOH conversion increases as the system pressure decreases in APR and SR. For both catalysts, the H2 and CO2 selectivity increased as the pressure increased in SR, reached a maximum at the bubble point pressure, and then decreased in the APR region. The Ni/CeO2 catalyst demonstrated higher selectivity for H2 and CO2than the Ni/Al2O3 catalyst during SR, which are consistent with the results of our previous publication on APR of n-butanol (n-BuOH) over similar catalysts. Unlike in APR, the Ni/CeO2 catalyst produced CO in SR. For both of the catalysts, the activation energies for H2 and CO2 production and BuOH conversion were lower in SR than that in APR. The proposed primary reaction pathway for reforming of BuOH on both catalysts is the same for APR and SR. The n-BuOH dehydrogenated to butaldehyde followed by decarbonylation to propane. Then the propane is steam reformed to hydrogen and carbon monoxide. The CO converts to CO2 mostly through water gas shift.Item Aqueous-phase reforming of n-BuOH over Ni/Al2O3 and Ni/CeO2 catalysts(Elsiever, 2011-12-15) Roy, BanasriThe aqueous-phase reforming (APR) of n-butanol (n-BuOH) over Ni(20 wt%) loaded Al2O3 and CeO2 catalysts has been studied in this paper. Over 100 h of run time, the Ni/Al2O3 catalyst showed significant deactivation compared to the Ni/CeO2 catalyst, both in terms of production rates and the selectivity to H2 and CO2. The Ni/CeO2 catalyst demonstrated higher selectivity for H2 and CO2, lower selectivity to alkanes, and a lower amount of C in the liquid phase compared to the Ni/Al2O3 sample. For the Ni/Al2O3 catalyst, the selectivity to CO increased with temperature, while the Ni/CeO2 catalyst produced no CO. For the Ni/CeO2 catalyst, the activation energies for H2 and CO2 production were 146 and 169 kJ mol−1, while for the Ni/Al2O3 catalyst these activation energies were 158 and 175 kJ mol−1, respectively. The difference of the active metal dispersion on Al2O3 and CeO2 supports, as measured from H2-pulse chemisorption was not significant. This indicates deposition of carbon on the catalyst as a likely cause of lower activity of the Ni/Al2O3 catalyst. It is unlikely that carbon would build up on the Ni/CeO2 catalyst due to higher oxygen mobility in the Ni doped non-stoichiometric CeO2 lattice. Based on the products formed, the proposed primary reaction pathway is the dehydrogenation of n-BuOH to butaldehyde followed by decarbonylation to propane. The propane then partially breaks down to hydrogen and carbon monoxide through steam reforming, while CO converts to CO2 mostly through water gas shift. Ethane and methane are formed via Fischer–Tropsch reactions of CO/CO2 with H2.