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Item Dual reforming of model biogas for syngas production on Ni/γ-Al2O3 and Ni-C/ZSM-5 cordierite monolith catalysts(Elsevier, 2023) Roy, Banasri; Srinivas, AppariThis work attempts to convert the model biogas on Ni/γ-Al2O3 and Ni-C/ZSM-5 into syngas using a dual-bed catalytic monolith reactor. The monolith is wash-coated with alumina and ZSM-5, respectively, followed by Ni and glucose-assisted Ni (Ni-C) loading using the wet impregnation technique. These two monoliths are loaded in an Inconel reactor and placed in a two-zone heating furnace. In dual reforming, either Ni/γ-Al2O3 or Ni-C/ZSM-5 monolith is used for dry reforming, and then Ni/γ-Al2O3 is used for steam reforming. A distance of ∼ 10 cm is maintained between these two monoliths. The exhaust gases from the first monolith are combined with steam before passing to the second monolith. The biogas reforming is carried out for a feed ratio (CH4:CO2) 1.5, GHSV of 1440 h−1 and 2880 h−1, at 800℃ and 1 atm pressure. The steam to CH4 ratio (S/C) is optimized to maximize the conversions (greater than80 %) of both CH4 and CO2. It was observed that the CH4 conversions increase with an increased S/C ratio due to the steam reforming in the second monolith. The TGA results show 7.6 % carbon formation on Ni-C/ZSM-5 and 35 % on Ni/γ-Al2O3 in dry reforming on the first monolith bed.Item Investigation of Ba doping in A-site deficient perovskite Ni-exsolved catalysts for biogas dry reforming(Elsevier, 2024-08) Roy, BanasriThis work presents the development of an A-site deficient La0.9−xBaxAl0.85Ni0.15O3 (x = 0, 0.02, 0.04, and 0.06) perovskite oxide catalyst for dry reforming of model biogas. The catalysts are prepared using a citrate sol-gel method and used for biogas dry reforming at 800 °C for feed ratios (CH4/CO2) of 1.5 and 2.0. The fresh and spent catalysts are analyzed using XRD, FTIR, TPD, XPS, FESEM, TEM, TPR, TGA-DTA, and Raman analysis. The XRD analysis exhibits the host perovskite oxide structure and the exsolved Ni phase for all prepared catalysts. The partial doping of Ba improves the metal support interaction and oxygen vacancies that enhance catalytic activity and stability, as revealed by the TPR and XPS analysis. The stability experiment on La0.9−xBaxAl0.85Ni0.15O3, for x = 0 catalyst resulted in reduced activity due to the catalyst deactivation by sintering, as confirmed by XRD and FE-SEM. Among all the catalysts studied, La0.84Ba0.06Al0.85Ni0.15O3 (LB6AN-15) exhibited the highest catalytic stability with CH4, and CO2 conversions are 60% and 93%, respectively, for 40 h time-on-stream due to the strong metal support interactions, high oxygen vacancies, and anti-sintering of exsolved Ni nanoparticles in biogas dry reforming.Item Effect of Calcination Time on the Catalytic Activity of Ni/γ-Al2O3 Cordierite Monolith for Dry Reforming of Biogas(Elsevier, 2021-02) Roy, Banasri; Srinivas, AppariNi/γ-Al2O3 wash coated cordierite monolith catalysts are calcined in air at 800 °C for 4, 10, and 20 h in order to study the effect of calcination time on the activity of the catalysts for dry reforming of model biogas. Catalytic activity studies are performed at 800 °C with three different CH4/CO2 ratios of 1.0, 1.5, and 2.0. The catalyst calcined for the longest time (C-20) displays higher stability and activity in terms of CH4 and CO2 conversion compared to those calcined for 4 h (C-4) and 10 h (C-10). XRD data and TPR analysis detect the maximum amount of NiAl2O4/MgAl2O4 phases and strongest metal-support interaction, respectively, for the C-20 sample. FESEM reveals the particle size of the calcined and reduced C-20 sample to be smaller than that of the C-4 and C-10 samples. Whereas, H2 pulse-chemisorption characterization demonstrates the highest metal surface area, metal dispersion, and smallest Ni particle size for the C-20 catalyst. While, no carbon deposition on any catalyst occurs for the CH4/CO2 ratio of one, lowest amount of carbon nanotubes is formed on the C-20 sample for the CH4/CO2 ratio of 1.5 and 2.0, as observe by DTA-TGA. EDX reveals concentration variation of Mg and Si from the cordierite monolith wall along the thickness of the coating for all the samples. In addition, the maximum amount of these elements is observed for the calcined C-20 catalyst coating. These implies that the diffusion of Mg and Si from the cordierite monolith to the catalyst coating during calcination contribute significantly in controlling the physicochemical properties of the catalysts. As a result, the higher stability and activity of the C-20 could be attributed to the formation of higher amount of the Ni– Mg- alumina spinel complex in the catalyst coating during longer calcination time, which leads to the improved metal-support interaction and higher nickel dispersion over monolith.Item Recent advances and perspectives of perovskite-derived Ni-based catalysts for CO2reforming of biogas(Elsevier, 2022-11) Srinivas, Appari; Roy, BanasriCO2 reforming of biogas (CRBG) is a promising renewable energy source to tackle the global energy demands and environmental challenges. Biogas (BG) is reformed to produce syngas on numerous catalysts, including transitional (Ni, Co, Fe, and Mo) and precious (Pt, Pd, Rh, and Ru) metals over various supports. However, catalyst deactivation due to the carbon deposition and trace amounts of H2S in BG is a significant barrier to commercializing the CRBG. Recently, perovskite oxide catalysts have gained interest due to their unique structural characteristics and articulating properties that favor CRBG for carbon-free operation. This review discusses the perovskite oxide catalysts in CO2 reforming, emphasizing structural stability, activity, and carbon deposition. The exsolved perovskite catalysts are reviewed as potential alternatives to the conventional LaNiO3, which suffers the structure break-down during the dry reforming. The exsolution of the catalysts offers numerous benefits such as structural stability, strong metal support interaction, oxygen storage capacity, and active small particle size with good dispersion, thus leading to better catalyst stability without deactivation in CRBG. However, catalyst reduction conditions dictate the particle size and activity of the catalysts. This review extensively covers the studies on different Ni-derived perovskites, the effect of partial doping of various metals (Ni, Co, Fe, Pt, Pd, and Rh), and mechanisms and related mixed-oxide systems.Item Effect of Calcination Time on the Catalytic Activity of Ni/γ-Al2O3 Cordierite Monolith for Dry Reforming of Biogas(Elsiever, 2020) Srinivas, Appari; Roy, BanasriNi/γ-Al2O3 wash coated cordierite monolith catalysts are calcined in air at 800 °C for 4, 10, and 20 h in order to study the effect of calcination time on the activity of the catalysts for dry reforming of model biogas. Catalytic activity studies are performed at 800 °C with three different CH4/CO2 ratios of 1.0, 1.5, and 2.0. The catalyst calcined for the longest time (C-20) displays higher stability and activity in terms of CH4 and CO2 conversion compared to those calcined for 4 h (C-4) and 10 h (C-10). XRD data and TPR analysis detect the maximum amount of NiAl2O4/MgAl2O4 phases and strongest metal-support interaction, respectively, for the C-20 sample. FESEM reveals the particle size of the calcined and reduced C-20 sample to be smaller than that of the C-4 and C-10 samples. Whereas, H2 pulse-chemisorption characterization demonstrates the highest metal surface area, metal dispersion, and smallest Ni particle size for the C-20 catalyst. While, no carbon deposition on any catalyst occurs for the CH4/CO2 ratio of one, lowest amount of carbon nanotubes is formed on the C-20 sample for the CH4/CO2 ratio of 1.5 and 2.0, as observe by DTA-TGA. EDX reveals concentration variation of Mg and Si from the cordierite monolith wall along the thickness of the coating for all the samples. In addition, the maximum amount of these elements is observed for the calcined C-20 catalyst coating. These implies that the diffusion of Mg and Si from the cordierite monolith to the catalyst coating during calcination contribute significantly in controlling the physicochemical properties of the catalysts. As a result, the higher stability and activity of the C-20 could be attributed to the formation of higher amount of the Ni– Mg- alumina spinel complex in the catalyst coating during longer calcination time, which leads to the improved metal-support interaction and higher nickel dispersion over monolith.