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    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.
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    Low-temperature sonochemical synthesis of high dielectric Lanthanum doped Cerium oxide nanopowder
    (Elsevier Ltd, 2018) Kishor Kumar, M.J.; Kalathi, J.T.
    Lanthanum (La) doped Cerium Oxide (CeO2) nanopowder was synthesized at a relatively lower temperature (70°C), without calcination in a simple, faster, and efficient way through sonochemical method. X-ray diffraction (XRD) results confirmed the formation of a cubic fluorite structure of nanocrystalline CeO2 and lattice deformation due to La-doping in CeO2. TEM analysis revealed that the size of La-doped CeO2 particles is in the range of 20?50 nm. In addition, selective area electron diffraction (SAED) and high-resolution TEM (HRTEM) analyses portrayed the nano-crystallinity, lattice fringe pattern, and d-spacing details of La-doped CeO2 powder. Lanthanum doping in CeO2 was further confirmed by a shift in Raman band towards the lower frequency (from 464 cm?1 to 457cm?1) along with peak intensity increase. Photoluminescence (PL) emission spectra showed that emission intensity of the La-doped CeO2 at 510 nm is increased due to oxygen vacancy mediated charge transfer. All these results confirm the successful doping of La in CeO2. The La-doped CeO2 powder possesses a high dielectric constant (?r) of 106 and a low dielectric loss (tan ?) of < 0.4 % at 1 kHz. The La-doped CeO2 finds potential applications on developing devices in the field of a thin film capacitor, transistors, and solid oxide fuel cells. © 2018 Elsevier B.V.
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    Praseodymium doped ceria as electrolyte material for IT-SOFC applications
    (Elsevier Ltd, 2018) Shajahan, I.; Ahn, J.; Nair, P.; Medisetti, S.; Patil, S.; Niveditha, V.; Uday Bhaskar Babu, G.; Prasad Dasari, H.P.; Lee, J.-H.
    Praseodymium-doped ceria (PDC, Ce0.9Pr0.1O2) electrolyte material for intermediate temperature solid oxide fuel cells (IT-SOFCs) has been successfully synthesised by EDTA-citrate method. From X-Ray diffraction (XRD), fluorite structure along with a crystallite size of 5.4 nm is obtained for PDC nanopowder calcined at 350 °C/24 h. Raman spectroscopy confirmed the structure, presence of oxygen vacancies with the manifestation of the main peak at 457 cm?1 and with a secondary peak at 550 cm?1. From Transmission Electron Microscopy (TEM) analysis, the average particle size is around 7–10 nm and selected area electron diffraction (SAED) patterns further confirmed the fluorite structure of PDC nanopowder. The PDC nanopowder displayed a BET surface area of 65 m2/g with a primary particle size of ?13 nm (calculated from BET surface area). Dilatometer studies revealed a multi-step shrinkage behaviour with the multiple peaks at 522, 1171 and 1461 °C which may be originated due to the presence of multiple size hard agglomerates. The PDC electrolyte pellet sintered at 1500 °C displayed an ionic conductivity of 1.213E-03 S cm?1 along with an activation energy of 1.28eV. Instead of a single fluorite structure, XRD of sintered PDC pellet showed multiple structures (Fluorite structure (CeO2) and cubic structure (PrO2). © 2018 Elsevier B.V.
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    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.
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    Effect of ionic radius on soot oxidation activity for ceria-based binary metal oxides
    (John Wiley and Sons Ltd vgorayska@wiley.com Southern Gate Chichester, West Sussex PO19 8SQ, 2019) Anjana, A.P.; Prasad Dasari, H.P.; Harshini, H.; Babu, G.U.B.
    CeO2 (C) along with binary metal oxides of Ce0.9M0.1O2-? (M = Sn, Hf, Zr, Gd, Sm, and La; CT, CH, CZ CG, CS, and CL) are synthesized using the EDTA–citrate method. Samples having an ionic radius smaller (CT, CH, and CZ) and larger (CG, CS, and CL) than Ce4+ are classified separately, and their soot oxidation activity is analyzed. The incorporation of dopant is confirmed from lattice constant variation in X-ray diffraction result. The critical descriptors for the activity are dopant nature (ionic radius and oxidation-state), single-phase solid solution, lattice strain, reactive (200) and (220) planes, Raman intensity ration (Iov/IF2g), optical bandgap, reducibility ratio, and surface oxygen vacancy. Smaller ionic radius, isovalent dopants (CH and CZ) create a defect site by lowering the optical bandgap along with improved surface oxygen vacancy concentration and thus enhanced soot oxidation activity. Aliovalent dopant with larger ionic radius shows the involvement of lattice oxygen in oxidation reaction by charge compensation mechanism. CL showed the highest activity amongst larger ionic radius samples. © 2019 Curtin University and John Wiley & Sons, Ltd.
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    RF Sputtered CeO2 Thin Films-Based Oxygen Sensors
    (Institute of Electrical and Electronics Engineers Inc., 2019) Ramshanker, N.; Lakshmi Ganapathi, K.L.; Bhat, M.S.; Mohan, S.
    In this paper, we report the scalable, high sensitivity, fast response, and low operating temperature Cerium oxide (CeO2) thin film-based oxygen sensors by optimizing CeO2 film thickness. CeO2 thin films of thickness ranging from 90 to 340 nm have been deposited at 400°C using radio frequency (RF) magnetron sputtering on Al2O3 substrates. Ellipsometry, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM) have been used to characterize the CeO2 films for their thickness, structural, compositional/chemical, and surface morphology properties. Gas sensors have been fabricated using CeO2 film as a sensing material and tested in an oxygen gas environment. CeO2 film with an optimum thickness of 260 nm has shown high sensitivity (12.6) and fast response time (?10 s) along with fast recovery time (15 s) at a low operating temperature of 400°C. To the best of our knowledge, these are the best values reported till date for undoped CeO2 thin film-based oxygen sensors. Furthermore, from the sensor's response, it was observed that there was no drifting from the baseline. This superior performance of CeO2 thin film-based oxygen sensor may be attributed to the combination of three factors, i.e., 1) high surface energy and reactivity due to the presence of (200) oriented CeO2 plane; 2) low resistance due to better crystallinity; and 3) perfect stoichiometry with required roughness. © 2001-2012 IEEE.
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    Effect of fuel and solvent on soot oxidation activity of ceria nanoparticles synthesized by solution combustion method
    (KeAi Communications Co., 2019) Patil, S.S.; Prasad Dasari, H.P.
    Effect of fuel (glycine and urea) and solvent (water, acetone and ethanol) on the soot oxidation activity of ceria nanoparticles synthesized by solution combustion method is carried out in the present study. X-ray diffraction (XRD) patterns displayed a fluorite structure and the Tauc's plot obtained from UV-Diffusive Reflectance spectroscopy (UV-DRS) showed that the band gap value was around 2.9–3.1 eV for the synthesized ceria nanoparticles irrespective of the fuel and solvent used. Ceria nanoparticles synthesized using glycine and acetone resulted in lower crystallite size, higher facet ratios ([1 0 0]/[1 1 1] and [1 1 0]/[1 1 1]) and higher lattice strain than compared to other solvents and fuels and thus resulted in better soot oxidation activity (T50 = 416 °C). The present synthesis method has played a significant role in improving the reactive facet ratios, providing lower crystallite size and high lattice strain. © 2019
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    Dilatometer studies of praseodymium doped ceria: Effect of synthesis methods on sintering behaviour
    (Elsevier Ltd, 2020) Shajahan, I.; Prasad Dasari, H.P.; Govardhan, P.
    Praseodymium-doped ceria (Ce0.9Pr0.1O2, PDC), as an electrolyte material for IT-SOFCs, is investigated with respect to the effect of synthesis method and a detailed analysis was carried out to understand the effect on crystallite size, morphology, specific surface area and sintering behaviour. The various synthesis routes such as microwave assisted co-precipitation method, room temperature co-precipitation method and EDTA-citrate complexing method was adopted for the synthesis of praseodymium doped ceria-based nano-materials. XRD pattern confirms the fluorite-type crystal structure of ceria and Raman spectroscopy analysis confirms the structure with the presence of oxygen vacancies. PDC synthesised by microwave assisted co-precipitation method using isopropyl alcohol as solvent exhibited better sintering activity, reduced the sintering temperature and promoted the densification rate when compared to other synthesis methods with uni-model shrinkage behaviour with shrinkage maxima at 765 °C. Based on two sintering models (CHR/Dorn method), the initial stage sintering mechanism was investigated in the present study and confirmed that the grain boundary diffusion (m = 2) as the dominant mechanism and the activation energy was found to be 116 kJ/mol (CHR model) and 176 kJ/mol (Dorn Method) for initial stages of sintering for PDC material synthesised by microwave assisted co-precipitation method using isopropyl alcohol as solvent. © 2019 Elsevier B.V.
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    Effect of sintering aids on sintering kinetic behavior of praseodymium doped ceria based electrolyte material for solid oxide cells
    (Elsevier Ltd, 2020) Shajahan, I.; Prasad Dasari, H.P.; Saidutta, M.B.
    The present study investigates the effect of sintering additives (Li, Co, Fe, and Mg) on the sintering kinetic behavior of the praseodymium-doped-ceria (PDC) electrolyte of solid oxide electrolyzer cell. 3Li-PDC, 3Co-PDC, 3Fe-PDC, and 3 Mg-PDC pellets were obtained from the synthesis of PDC nano-powder by microwave-assisted co-precipitation method using isopropyl alcohol as a solvent and followed by sintering additive wetness impregnation method. Linear shrinkage and shrinkage rate data suggest a positive sintering effect for 3Li-PDC and 3Co-PDC pellets and a negative sintering effect for 3 Mg-PDC and 3Fe-PDC pellets than compared to PDC pellets alone. The addition of lithium as a sintering additive (3Li-PDC) had reduced the sintering temperature of PDC from 1100 °C to 850 °C. For PDC, 3Li-PDC, 3Co-PDC, 3Fe-PDC and 3 Mg-PDC pellets sintered at 1100 °C, 850 °C, 1000 °C, 1200 °C, 1100 °C for 2 h resulted in a relative density of 93.6 ± 0.25, 95.8 ± 0.45, 95.0 ± 0.20, 92.7 ± 0.10, and 94.5 ± 0.10%, respectively. The XRD patterns of the sintered PDC pellets suggested a secondary phase formation (PrO2) in 3Co-PDC, 3Fe-PDC, and 3 Mg-PDC pellets indicating that the addition of these sintering aids results in poor solubility limit of Pr in CeO2. On the other hand, XRD patterns of PDC and Li-PDC sintered pellets displayed no secondary peak indicating good solid-solution formation. The activation energy of the 3Li-PDC pellet is obtained from CHR and Dorn methods and was found to be 182 kJ/mol and 196 kJ/mol. From the CHR method, for the 3Li-PDC pellet, the initial sintering behavior is by the grain boundary diffusion mechanism (m = ~2). © 2020 Hydrogen Energy Publications LLC
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    Influence of (Er3+, La3+, Ce4+) additions on physical and optical properties of 50CaO–50P2O5 glasses
    (Elsevier B.V., 2020) Dutebo, M.T.; Shashikala, H.D.
    Calcium phosphate glass samples with the addition of 5 mol% of three different rare earth oxides (Erbium, Lanthanum and Cerium oxides) were made by melt quenching process. Effect of rare earth ions addition on structural, physical and optical properties has been investigated using density measurement, XRD diffraction, Fourier transformed infrared (FTIR) spectroscopy, ultra violet visible spectroscopy and Abbe Refractometer. The random short range order of synthesized glass samples was analyzed by XRD diffraction. The absorption spectra have been recorded and optical band gap energy was determined by using Tauc plotting. The band gap energy showed a decrease when 5 mol% of rare earth (Er2O3, La2O3, and CeO2) oxides were added to the host glass. Fourier transformed infrared (FTIR) spectrometer was applied to study the structural changes of the synthesized glasses. The density and refractive index of synthesized glasses was measured and related parameters were calculated. These values are compared with the un-doped metaphosphate glass. Based on measured density, the concentrations of added rare-earth ion is calculated. With an increase in ion concentration, the internuclear distance decreased leading to an increase in field strength. © 2020 Elsevier B.V.