Browsing by Author "Anjana, A.P."

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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.
Effect of Ag loading on praseodymium doped ceria catalyst for soot oxidation activity
(Springer, 2022) Govardhan, P.; Anjana, A.P.; Patil, S.S.; Prasad Dasari, H.P.; Harshini, H.; Shourya, A.
Silver-loaded praseodymium doped ceria (XAg/PDC) was synthesized by microwave-assisted co-precipitation and wetness impregnation. XRD confirms the fluorite structure of ceria without secondary phase, and Raman spectroscopy represents the increased generation of oxygen vacancies with Ag loading. The TEM analysis shows lattice fringes corresponding to both CeO2 and Ag on the surface. The BET and BJH analysis of catalyst confirms the high porosity accompanied by high surface area and pore diameter of 5Ag/PDC and 15Ag/PDC, making it more active for the oxidation reaction. From the XPS analysis the amount of surface Ce3+ concentration and the surface chemisorbed oxygen species (O2 2) is high for 5Ag/PDC and 15Ag/PDC, in line with XRD and Raman results. The soot oxidation T50 temperature follows the trend: 5Ag/PDC∼15Ag/PDC<10Ag/PDC<20Ag/PDC<0Ag/PDC. The Ag loading increased the surface reducibility of cerium ions and thus 5 wt% was optimized. © 2021, The Korean Institute of Chemical Engineers.
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.
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. © 2022
Effect of synthesis method on structural properties and soot oxidation activity of gadolinium-doped ceria
(Springer International Publishing kasia@cesj.com, 2018) Anjana, A.P.; Gadiyar, H.J.; Surendran, M.; Rao, A.S.; Prasad Dasari, H.P.; Harshini, H.; Babu, G.U.B.
Abstract: EDTA–citrate complex and solvothermal methods were adopted for the synthesis of gadolinium-doped ceria (GDC) (Ce0.9Gd0.1O2) solid solution, and the obtained GDC sample is tested for soot oxidation activity. Based on XRD results, it was evident that the reactive facet planes of {100} and {110} were highly intense [intensity ratio (%) of (200)/(100) (34.2%) and (220)/(111) (51.2%)] for GDC prepared by the EDTA–citrate method in comparison with the solvothermal method, and this highly intense reactive facet plane correlates to the lower energy for oxygen vacancy formation. Apart from the smaller crystallite size (10 nm) the GDC sample prepared by the EDTA–citrate method displayed lower band gap energy (2.99 eV), higher ratio of reducibility (45.45%) and lower binding energy (528.8 eV) for surface-adsorbed oxygen. The GDC obtained by EDTA–citrate method displayed a better soot oxidation activity (T50 = 468 °C) than compared to the GDC obtained by solvothermal method (T50 = 500 °C). The obtained results significantly show that the synthesis method plays a crucial role in controlling the structural properties and in enhancing the soot oxidation activity. © 2018, Institute of Chemistry, Slovak Academy of Sciences.
Potential of pyrochlore structure materials in solid oxide fuel cell applications
(Elsevier Ltd, 2021) Anjana, A.P.; Prasad Dasari, H.P.
Pyrochlore structure material (A2B2O7) has gained interest in diverse applications like catalysis, nuclear waste encapsulation, sensors, and various electronic devices due to the unique crystal structure, electrical property, and thermal stability. This review deals with the ionic/electronic conductivity of numerous pyrochlore structure materials (titanates, zirconates, hafnates, stannates, niobates, ruthenates, and tantalite based pyrochlore) as electrolyte and electrode materials for solid oxide fuel cells (SOFCs). The impact of cation radius ratio (rA/rB) on the lattice constant and oxygen ‘x’ parameter of different pyrochlore structure materials obtained by various synthesis methods are reported. Higher ionic conductivity is essential for better ion transport in an electrolyte, and mixed ionic and electronic conductivity in electrode is essential for attaining higher efficiency in a typical SOFC. GdxTi2O7-δ, Gd2-xCaxTi2O7-δ, Nd2-yGdyZr2O7, Y2Zr2O7, Y2Zr2-xMnxO7-δ, SmDy1-xMgxZr2O7-x/2, Gd2-xCaxTi2O7-δ pyrochlore are reported as electrolytes for fuel cell applications. Some pyrochlore material (La2-xCaxZr2O7, Sm2-xMxTi2O7 (M = Mg, Co, and Ni) pyrochlore) shows protonic conductivity at lower temperatures and ionic conductivity at higher temperature condition. Also, the mixed ionic-electronic conductivity behavior is reported in electrode materials for SOFC such as R2MnTiO7 (R = Er and Y), R2MnRuO7 (R = Tb, Dy, Ho, Er, Tm, Yb, Lu, and Y), R2Ru2O7 (R = Bi, Pb and Y), Y2-xPrxRu2O7, Ni-(Gd0.9Ca0.1)2Ti2O7-δ, (Gd0.9Ca0.1)2Ti2O7-δ, Gd2(Ti0.8Ru0.2)2O7-δ, (Sm0.9Ca0.1)2Ti2O7-δ and (Y0.9Ca0.1)2Ti2O7-δ pyrochlore. The detailed study of the electronic behavior of these pyrochlore system confirms the necessity of defect structure with high oxygen mobility, lower activation energy, ionic radii ratio criterion should satisfy, and possess notable ion-ion interaction. Ionic conductivity in pyrochlore is increased by enhancing the oxygen migration through 48f-48f site with the formation of oxygen vacancy. Vacancy formation can be achieved by adding a suitable dopant that creates oxygen vacancy by charge compensation mechanism or as anion Frenkel defects. Similarly, the electrical conductivity is improved while adding suitable dopant (Ce, Pr, Ru, etc.) due to disordered structure and anti-Frenkel defect formation which leads to oxygen vacancy formation and thus improves conductivity. © 2020 Elsevier Ltd and Techna Group S.r.l.
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.
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.