Faculty Publications
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Item Record-low sintering-temperature (600 °c) of solid-oxide fuel cell electrolyte(Elsevier Ltd, 2016) Prasad Dasari, H.P.; Ahn, K.; Park, S.-Y.; Hong, J.; Kim, H.; Yoon, K.J.; Son, J.-W.; Kim, B.-K.; Lee, H.-W.; Lee, J.-H.One of the major problems arising with Solid-Oxide Fuel Cell (SOFC) electrolyte is conventional sintering which requires a very high temperature (>1300 °C) to fully densify the electrolyte material. In the present study, the sintering temperature of SOFC electrolyte is drastically decreased down to 600 °C. Combinational effects of particle size reduction, liquid-phase sintering mechanism and microwave sintering resulted in achieving full density in such a record-low sintering temperature. Gadolinium doped Ceria (GDC) nano-particles are synthesized by co-precipitation method, Lithium (Li), as an additional dopant, is used as liquid-phase sintering aid. Microwave sintering of this electrolyte material resulted in decreasing the sintering temperature to 600 °C. Micrographs obtained from Scanning/Transmission Electron Microscopy (SEM/TEM) clearly pointed a drastic growth in grain-size of Li-GDC sample (?150 nm) than compared to GDC sample (<30 nm) showing the significance of Li addition. The sintered Li-GDC samples displayed an ionic conductivity of ?1.00 × 10-2 S cm-1 at 600 °C in air and from the conductivity plots the activation energy is found to be 0.53 eV. © 2016 Elsevier B.V. All rights reserved.Item 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.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 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.Item 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 LLCItem Promotional effect of nickel addition on soot oxidation activity of Ce0.9Pr0.1O2 oxide catalysts(Springer, 2020) Rajvanshi, K.; Patil, S.S.; Lakhanlal, u.; Prasad Dasari, H.P.; Saidutta, M.B.; Harshini, H.The present study investigates the promotional effect of Ni addition on soot oxidation activity of Ce0.9Pr0.1O2 oxide catalysts. A series of xNi-PDC (x= 0, 3, 5, 7, 10, 15, and 20 mol%) catalysts were synthesized by solution combustion synthesis method and characterized by XRD, Raman spectroscopy and TEM analysis. XRD and SAED patterns of the catalysts show cubic fluorite structure of ceria with an average crystallite size of 6–8 nm, and only 20Ni-PDC display NiO as a secondary phase. Raman spectra of xNi-PDC catalysts display an increase in oxygen vacancies. With a minimum addition of 10 mol% Ni to PDC, i.e., the 10Ni-PDC catalyst showed optimum soot oxidation activity (T50 = 360 °C) than compared to PDC and other Ni-PDC catalysts. Lattice strain and oxygen vacancies played a key descriptor role in showing better soot oxidation activity of the 10Ni-PDC catalyst. From the soot oxidation kinetic studies, the activation energy obtained by Ozawa plots for the 10Ni-PDC catalyst is 137 kJ/mol. © 2020, Institute of Chemistry, Slovak Academy of Sciences.Item Effect of morphology and oxidation state of nickel on diesel soot oxidation activity(Elsevier Ltd, 2022) Vijay, M.P.A.; Patil, S.S.; Madhura, D.R.; Anjana, A.P.; Gouramma, P.; Prasad Dasari, H.P.; Arya, S.B.; Harshini, H.NiO sample is synthesized using the EDTA citrate complex method and calcined at 600 °C/5 h. Ni sample was acquired by reducing NiO to Ni at 600 °C in 4% H2/N2 atmosphere. Its physicochemical properties were obtained by XRD and Raman spectroscopy analysis, where it confirmed the complete reduction of NiO to Ni. SEM and TEM micrographs revealed a drastic particle growth for the Ni, indicating NiO sintering during the reduction process and a considerable surface morphology change. Ozawa and KAS methods were used to calculate the mean activation energy (Ea) value. NiO displayed lower Ea than Ni. Hence, NiO showed better catalytic activity than Ni. © 2022Item Printex-U soot oxidation kinetic behaviour over Alumina and Quartz(Elsevier Ltd, 2022) Ganiger, S.; Patil, S.S.; Prasad Dasari, H.P.; Priyanka, R.; Kollimarla, S.Printex-U carbon (Pure Soot, S0) on alumina (SA) and quartz (SQ) powder were considered to understand the behaviour of oxidation reaction and kinetic analysis. A similar model of the single-step reaction was followed by the Soot (S0) and SA sample, while SQ followed a complex mechanism of multiple-step reactions. From the experimental and theoretical calculations, it was observed that there was a slight decrease in the T50 temperature for SA, which also had the lowest Ea, but there was an increase in T50 and Ea for SQ compared to the S0 sample. From the present study, it can be understood that the alumina enhanced the catalytic activity when compared to pure soot alone, whereas quartz inhibited the activity. The T50 temperature, Ea, and A calculated were obtained in SA < S0 < SQ. The soot properties and their kinetics will further help to design catalyzed diesel particulate filters. © 2021 Elsevier LtdItem 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 Electrical conductivity studies on LAMOX based electrolyte materials for solid oxide fuel cells(Elsevier Ltd, 2022) Srijith; Lakhanlal, u.; Das, A.; Prasad Dasari, H.P.; Saidutta, M.B.In this study, the electrical conductivity of the LAMOX based electrolytes (La1.8Dy0.2Mo2-xWxO9 (x = 0, 0.1, 0.2, 0.5, and 1), and La1.8Dy0.2Mo2-xGaxO9 (x = 0.1)) synthesized by the citrate complexion method has been studied using DC four-probe method. The electrical conductivity of the electrolytes is measured in the temperature range of 800–400 °C in the air (∼100 ml min−1). The effect of W and Ga substitution at the Mo site on the electrical conductivity is evaluated. The long-term electrical conductivity stability test (time on stream) (5 h) is conducted at 650, 580, and 520 °C to study the effect of possible phase transition on electrical conductivity. A high-temperature XRD study is also conducted in the temperature range of 500–650 °C (during heating and cooling) on selected electrolyte materials (La1.8Dy0.2Mo2-xWxO9 (x = 0 and 0.1) and La1.8Dy0.2Mo2-xGaxO9 (x = 0.1)) to study the α↔β phase transition. The electrical conductivity of these electrolytes in the air at 800 °C is in the range of 5.3 × 10−2 – 14 × 10−2 S cm−1. The activation energy (EA) of these electrolytes is in the range of 1.11–1.62 eV. The VTF parameters σo, B, and To are in the range of 67.46–395.88 S cm−1 K0.5, 0.122–0.254 eV, and 247–347 °C, respectively. The La1.8Dy0.2Mo2-xWxO9 (x = 0.1) shows highest electrical conductivity (14 × 10−2 S cm−1, EA = 1.54 eV) among all electrolytes in air at 800 °C and for this material the VTF parameters σo, B, and To are 170.32 S cm−1 K0.5, 0.153 eV, and 302 °C, respectively. © 2022 Elsevier Ltd and Techna Group S.r.l.