Faculty Publications
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Item Soot Oxidation Activity of Redox and Non-Redox Metal Oxides Synthesised by EDTA–Citrate Method(Springer New York LLC barbara.b.bertram@gsk.com, 2017) Anjana, A.P.; Prasad Dasari, H.P.; Lee, J.-H.; Harshini, H.; Babu, G.U.B.Abstract: In the present study, redox (CeO2, SnO2, Pr6O11 and Mn3O4) and non-redox (Gd2O3, La2O3 ZrO2 and HfO2) metal oxides were successfully synthesised using the EDTA–citrate complexing method and tested for soot oxidation activity. The characterization of the metal oxides is carried out using FTIR, XRD, BET surface area, pore volume analyser, SEM and TEM. The redox nature and metal–oxygen bond information of the metal oxides are obtained from XPS analysis. In redox metal oxides, three critical parameters [lattice oxygen binding energy, reduction temperature and ?r (ionic size difference of the corresponding metal oxide oxidation states)] govern the soot oxidation activity. Among the redox metal oxide samples, Mn3O4 and Pr6O11 samples showed lower binding energy for oxygen (O?—529.4, 528.9 eV respectively), lower reduction temperature (T?—317 and 512 °C respectively) and have smaller ?r value (9 pm and 17 pm respectively). Thus, displayed a better soot oxidation activity (T50 = 484 and 482 °C respectively) than compared to other redox metal oxides. Among the non-redox metal oxides, HfO2 sample displayed higher BET surface area (21.06 m2/g), lattice strain (0.0157), smaller ionic radius (58.2 pm) and higher relative surface oxygen ratio (58%) and thus resulted in a significantly better soot oxidation activity (T50 = 483 °C) than compared to other non-redox metal oxides. Graphical Abstract: [Figure not available: see fulltext.]. © 2017, Springer Science+Business Media, LLC.Item Ceria-samarium binary metal oxides: A comparative approach towards structural properties and soot oxidation activity(Elsevier B.V., 2018) Anjana, A.P.; Geethu, J.; P, M.R.; Prasad Dasari, H.P.; Lee, J.-H.; Harshini, H.; Bhaskar Babu, G.U.Binary metal oxides of CeO2-Sm2O3 (CSx, x varies from 10 to 90 mol%) along with pure CeO2 and Sm2O3 were synthesised successfully by the EDTA-Citrate method. From XRD, Raman spectroscopy and UV–vis DRS results, the whole composition of metal oxides exist in three phases: (fluorite phase (F) (CS10-CS30), bi-phase (fluorite (F) + cubic (C)) (CS30-CS90) and cubic phase (C) (Sm2O3)). For CSx samples, the calculated band gap energy values obtained from the UV–vis DRS results were in between 3.0–5.1 eV and fluorite phase samples (CS10–CS30) displayed lower band gap energy values (3.04–3.07 eV) than compared to the samples in other phases. Similarly, from XPS analysis, fluorite phase samples (CS10–CS30) showed higher surface oxygen vacancy concentration than compared to samples in other phases. Catalytic activity for soot oxidation is carried out on CSx samples, and the T50 temperature is in between 480–540 °C. Fluorite phase samples (CS10 CS30) showed higher surface area, lower degree of agglomeration, lower band gap energy, higher oxygen vacancy concentration and better catalytic activity for soot oxidation. Among all the CSx samples, CS10 sample displayed highest surface area (38 m2/g), lowest degree of agglomeration (0.36), lowest band gap energy (3.04 eV), highest oxygen vacancy concentration (64%) and highest soot oxidation activity (T50 = 480 °C). The order of the soot oxidation activity of CSx samples followed the same trend of band gap energy values. © 2018 Elsevier B.V.Item Surface morphology and phase stability effect of Ceria-Hafnia (CHx) binary metal oxides on soot oxidation activity(Elsevier B.V., 2018) Anjana, A.P.; Prasad Dasari, H.P.; Harshini, H.; Babu, G.U.B.CeO2-HfO2 (CHx) binary metal oxides over whole composition range (0–100%) are synthesised using the EDTA-Citrate method and calcined at 600 °C/5 h. From XRD analysis, the sample series are classified as fluorite (F) phase for CH10-CH30, hybrid (F + M) phase for CH40-CH90 and monoclinic (M) phase for CH100 sample, respectively and the results were further confirmed using Raman spectroscopy. From SEM analysis, a clear surface morphology change is noticed for fluorite, hybrid and monoclinic phases of the CHx binary metal oxides. Further, Selected Area Electron Diffraction (SAED) analysis also confirmed the single and hybrid phases of CHx binary metal oxides. The soot oxidation for the CHx binary metal oxides displayed high catalytic activity for Fluorite phase (CH10 ? CH30) samples and a decrease in catalytic activity is noticed for the Hybrid phase (CH40 ? CH90) samples. The change in catalytic activity coincides with the change in the surface morphology and phase change for the CHx binary metal oxides. Among the Fluorite phase samples, CH10 sample displayed the highest catalytic activity (T50 = 430 °C) with higher surface area (29 m2/g), lower particle size (26 nm), lower degree of agglomeration (? = 2.8) higher surface oxygen concentration (44%). Isothermal-Time-on-stream (ITOS) analysis also showed that the CH10 sample can achieve T50 in a shorter time than compared to other CHx binary metal oxides. Surface morphology and phase stability can also play as key descriptors in screening CHx binary metal oxides for soot oxidation activity. © 2018 Elsevier B.V.Item Effect of Nd-doping on soot oxidation activity of Ceria-based nanoparticles synthesized by Glycine Nitrate Process(Elsevier B.V., 2019) Patil, S.S.; Prasad Dasari, H.P.; Harshini, H.Neodymium-doped Ceria (NDC, Nd = 0, 1, 3, 5, 10, 20 and 30 mol %) catalysts were successfully synthesized by Glycine-Nitrate-Process (GNP) and tested for soot oxidation activity. For all NDC catalysts, XRD and Raman spectroscopy analyses showed a fluorite structure of ceria having an F2gRaman active symmetric breathing mode (O-Ce-O). 1NDC catalyst displayed better T50 temperature (427?C) followed by 0NDC (435?C), and 30NDC showed the highest T50 temperature (460?C). From XPS analysis, 1NDC and 0NDC catalysts showed a high amount of Ce3+ concentration and the surface-active oxygen species than compared to other NDC catalysts and thus, resulted in better soot oxidation activity indicating that the surface Ce3+ concentration and surface-active oxygen species play a key descriptor role in tuning the soot oxidation activity of NDC catalysts. © 2019 Elsevier B.V.Item Studies on the Solid Oxide Cell Perovskite Electrode Materials for Soot Oxidation Activity(Springer, 2019) Shenoy, C.S.; Patil, S.S.; Govardhan, P.; Shourya, A.; Prasad Dasari, H.P.; Saidutta, M.B.; Harshini, H.Solid oxide cell (SOC) perovskite electrode materials (BSCF (Ba0.5Sr0.5Co0.8Fe0.2O3-?), LSCF (La0.6Sr0.4Co0.2Fe0.8O3-?) and LSCM (La0.75Sr0.25Cr0.5Mn0.5O3-?)) were synthesised using microwave-assisted reverse-strike co-precipitation method and tested for soot oxidation activity. The calcined perovskite materials were characterized using FT-IR, XRD, SEM and BSE, BET and BJH and XPS analysis. The mean activation energy for soot oxidation was calculated from Ozawa plots at various heating rates (5, 10, 15 and 20 K/min) at different levels of soot conversions (T10 to T90) for BSCF, LSCM and LSCF perovskite materials and was around 133 ± 11.5, 138 ± 9.9 and 152 ± 7.2 kJ/mol, respectively. Irrespective of the heating rates, BSCF material showed the lowest T50 temperature than compared to other samples, and it is correlated to the presence of Fe3O4 as a secondary phase. © 2019, Springer Nature Switzerland AG.Item A Negative Effect of Niobium-Doped Ceria on Soot Oxidation Activity‡(John Wiley and Sons Inc, 2022) Patil, S.S.; Naik, S.; Ramesh, M.D.; Harshini, H.; Prasad Dasari, H.P.Niobium-doped ceria catalysts were synthesized to study soot oxidation activity. X-Ray diffraction (XRD) and Raman analysis of the samples revealed the presence of a fluorite structure of CeO2 for all the doped samples. The T50 temperature of the pure CeO2 sample was more significant than that of bare soot. The high catalytic activity of the CeO2 catalyst can be attributed to the low crystallite size, high facet ratio, and the large Brunauer-Emmett-Teller (BET) surface area as compared to Nb-doped samples. The activation energy calculated by both Ozawa and KAS methods were found to be low for CeO2 when compared to Nb-doped samples. CeO2 resulted in better soot oxidation activity with low activation energy. © 2022 Wiley-VCH GmbHItem Soot Oxidation Kinetics on Nickel Oxide: Effects of Various Synthesis Techniques(Pleiades Publishing, 2024) Patil, S.S.; Prasad Dasari, H.P.; Gouramma, P.; Harshini, H.Abstract: Nickel oxide (NiO) nanoparticles were synthesized using four different methods: microwave co-precipitation (MCP), solution combustion synthesis (SCS), direct nitrate calcination (DNC), and the sol-gel process (SGP), incorporating organic additives such as glucose and fructose. X-ray diffraction and Raman spectroscopy analyses revealed that the NiO nanoparticles formed a face-centered cubic phase characterized by Ni–O bond stretching. The SCS method produced NiO nanoparticles with higher lattice strain, smaller crystallite size, and an increased facet ratio ({110}) compared to the other methods. Transmission electron microscopy indicated that the order of nano-agglomeration size for the NiO nanoparticles was DNC > MCP > SGP > SCS. The NiO nanoparticles synthesized via SCS, SGP and MCP exhibited irregular hexagonal shapes. Among the synthesized nanoparticles, those produced by the SCS method demonstrated the highest catalytic activity (T50 = 478°C), followed by DNC (T50 = 492°C), MCP (T50 = 495°C), and SGP (T50 = 538°C). A kinetic study was conducted to evaluate key parameters, including activation energy, preexponential factor, and reaction model. The experimental curves of soot conversion were compared with theoretical curves derived from the evaluated kinetic parameters. The NiO nanoparticles synthesized via SCS exhibited the highest kinetic activity with the enhanced reaction rate at lower temperatures. © Pleiades Publishing, Ltd. 2024.