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At least 649 records · Page 36
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Transfer hydrogenation over sodium-modified ceria: Enrichment of redox sites active for alcohol dehydrogenation

Ceria (CeO 2 ) and sodium-modified ceria (Ce-Na) were prepared through combustion synthesis. Palladium was deposited onto the supports (Pd/CeO 2 and Pd/Ce-Na) and their activity for the aqueous-phase transfer hydrogenation of phenol using 2-propanol under liquid flow conditions was studied. Pd/Ce-Na showed a marked increase (6×) in transfer hydrogenation activity over Pd/CeO 2 . Material characterization indicated that water-stable sodium species were not doped into the ceria lattice, but rather existed as subsurface carbonates. Modification of ceria by sodium provided more adsorption and redox active sites (i.e. defects) for 2-propanol dehydrogenation. This effect was an intrinsic property of the Ce-Na support and independent of Pd. The redox sites active for 2-propanol dehydrogenation were thermodynamically equivalent on both supports/catalysts. At high phenol concentrations, the reaction was limited by 2-propanol adsorption. Furthermore, the difference in catalytic activity was attributed to the different numbers of 2-propanol adsorption and redox active sites on each catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Dependency of CO 2 methanation on the strong metal-support interaction for supported Ni/CeO 2 catalysts

The strong metal-support interaction (SMSI) for supported Ni/CeO 2 catalysts with different CeO 2 nanomorphologies was systematically explored. The degree of encapsulation of Ni particles originating from the SMSI effect was found to follow the trend of Ni/CeO 2 -(1 1 1) > Ni/CeO 2 -(1 0 0) > Ni/CeO 2 -(110 + 100), which parallels the CO 2 hydrogenation activity. Quasi in situ XPS reveals the presence of Ce 3+ sites in accordance with the formation of an amorphous surface CeOx layer encapsulating the Ni nanoparticles. In situ DRIFTS indicates the reaction pathway and rate-determining step are dependent on the degree of the SMSI effect, leading to distinct selectivities towards CH 4 , especially at a high weight hourly space velocity (WHSV). Finally, these findings present a fundamental strategy about tailoring catalytic performance through support facet dependent susceptibility of SMSI phenomena.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Revisiting the influence of Ni particle size on the hydrogenation of CO 2 to CH 4 over Ni/CeO 2

Nickel nanoparticles were supported on CeO 2 and evaluated in the hydrogenation of CO 2 to CH 4 at 538 K and 1 atm. Chemisorption of H 2 was used to estimate the average Ni particle size, which ranged from 1.3 to 17 nm. The apparent activation energy for CH 4 formation and turnover frequency for CO 2 conversion was independent of Ni particle size. The smallest Ni particles (1.3 nm) were less selective to CH 4 . Comparisons to alumina-supported Ni reveal the same performance as Ni/CeO 2 when normalized to active Ni atoms counted by H 2 chemisorption. A beneficial effect of ceria relative to alumina is the enhanced reducibility of Ni as evaluated by H 2 temperature-programmed reduction. The constancy of the turnover frequency on Ni particles suggests the acid-base and/or redox properties of the support do not play a significant role in the CO 2 methanation reaction under the conditions of study, which contrasts many earlier works.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Two-stage epitaxial growth of vertically-aligned SnO2 nano-rods on (001) ceria

Growth of high-aspect ratio oriented tin oxide, SnO2, nano-rods is complicated by a limited choice of matching substrates. We show that a (001) cerium oxide, CeO2, surface uniquely enables epitaxial growth of tin-oxide nano-rods via a two-stage process. First, (100) oriented nano-wires coat the ceria surface by lateral growth, forming a uniaxially-textured SnO2 deposit. Second, vertical SnO2 nano-rods nucleate on the deposit by homoepitaxy. We demonstrate growth of vertically oriented 1-2 mu m long nano-rods with an average diameter of approximate to 20 nm. 2014 Elsevier B.V. All rights reserved.

Solovyov, VF↗
DOE OSTI2020

Effects of Zr substitution on soot combustion over cubic fluorite-structured nanoceria: Soot-ceria contact and interfacial oxygen evolution

Ceria is widely used as a catalyst for soot combustion, but effects of Zr substitution on the reaction mechanism is ambiguous. The present work elucidates effects of Zr substitution on soot combustion over cubic fluorite-structured nanoceria. The nanostructured CeO 2 , Ce 0.92 Zr 0.08 O 2 , and Ce0.84Zr0.16O2 composed of 5–6 nm crystallites display Tm-CO 2 (the temperature at maximum CO 2 yield) at 383, 355, and 375°C under 10 vol.% O 2 /N 2 , respectively. Additionally, the size of agglomerate decreases from 165.5 to 51.9–57.3 nm, which is beneficial for the soot-ceria contact. Moreover, Zr increases the amount of surface oxygen vacancies, generating more active oxygen (O2- and O-) for soot oxidation. Thus, the activities of Ce 0.92 Zr 0.08 O 2 and Ce 0.84 Zr 0.16 O 2 in soot combustion are better than that of CeO2. Although oxygen vacancies promote the migration of lattice O 2- , the enriched surface Zr also inhibits the mobility of lattice O 2- . Therefore, the Tm-CO 2 of Ce 0.84 Zr 0.16 O 2 is higher than that of Ce 0.92 Zr 0.08 O 2 . Based on reaction kinetic study, soot in direct contact with ceria preferentially decomposes with low activation energy, while the oxidation of isolated soot occurs through diffusion with high activation energy. The obtained findings provide new understanding on the soot combustion over nanoceria.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Surface redox characters and synergetic catalytic properties of macroporous ceria-zirconia solid solutions

Macroporous CeO 2 -ZrO 2 (CZ) solid solutions with gradually changing ceria content were prepared through the EISA method. Pore sizes of the samples are about 100 nm- 1μm and pore walls are 100 nm- 1.5 μm. The surface and near surface reduction bands of Ce 4+ below 600 °C were maximized for the Ce 0.5 Zr 0.5 O 2 sample (C5) according to the quantitative de-convolution to the acquired TPR curves. The area percentage of the O 2- -2p 6 → Ce 3+ 3d 9 4f 2 electronic transition band on XPS spectra, which related to the concentration of the Ce 3+ , was found to be a function of the ceria content. The oxygen storage capacity showed a positive relationship with the chemical compositions. Redox reactions below 600 °C play a key role in determining the reduction performances of ceria based TWCs. Three-way catalytic performances of the Pd + Rh + Pt /C5 sample showed an ignition temperature for CO and NOx at about 240 °C, and finished before 300 °C. The ignition of C 3 H 8 started at 270 °C while finished at differed samples. The maximum catalytic efficiencies of CO, NOx, and C 3 H 8 on C5 sample were revealed to 100%, 98%, 97% respectively. Here, the performances showed that porous CZ solid solutions are suitable for high performance catalytic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Component effects on crystallization of RE-containing aluminoborosilicate glass

Lanthanide-aluminoborosilicate (LABS) glass is one option for immobilizing rare earth (RE) oxide fission products generated during reprocessing of pyroprocessed fuel. This glass system can accommodate a high loading of RE oxides and has excellent chemical durability. The present study describes efforts to model equilibrium crystallinity as a function of glass composition and temperature as well as liquidus temperature (TL) as a function of glass composition. The experimental method for determining TL was ASTM C1720-11. Typically, three crystalline phases were formed in each glass: Ce-borosilicate (Ce 3 BSi 2 O 10 ), mullite (Al 10 Si 2 O 19 ), and corundum (Al 2 O 3 ). Cerianite (CeO 2 ) was a common minor crystalline phase and Nd-silicate (Nd 2 Si 2 O 7 ) occurred in some of the glasses. In the composition region studied, TL decreased as SiO 2 and B 2 O 3 fractions increased and strongly increased with increasing fractions of RE oxides; Al 2 O 3 had a moderate effect on the TL but, as expected, it strongly affected the precipitation of Alcontaining crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Impact of rare earth ion size on the phase evolution of MoO3-containing aluminoborosilicate glass-ceramics

Transition metal and rare earth cations are important fission products present in used nuclear fuel, which in high concentrations tend to precipitate crystalline phases in vitreous nuclear waste forms. Two phases of particular interest are powellite (CaMoO 4 ) and oxyapatite (Ca 2 RE 8 (SiO 4 ) 6 O 2 ). The glass compositional dependencies controlling crystallization of these phases on cooling from the melt are poorly understood. In the present study, the effect of rare earth identity and modifier cation field strength on powellite and apatite crystallization were studied in a model MoO3-containing alkali/alkaline-earth aluminoborosilicate glass with focus on (1) influence of rare earth cation size (for RE 3+ : Ce, La, Nd, Sm, Er, Yb) and (2) influence of non-framework cations (RE 3+ , Mo 6+ , Na + , Ca 2+ ). Quenched glasses and glass-ceramics (obtained by slow cooling) were characterized by X-ray diffraction (XRD), Raman spectroscopy, X-ray absorption (XAS), and electron probe microanalysis (EPMA). All samples were X-ray amorphous upon quenching, except the Ce-containing composition which crystallized ceria (CeO 2 ), and the sample devoid of any rare earth cations which crystallized powellite (CaMoO 4 ). On heat treatment, powellite and oxyapatite crystallized in the majority of the samples with the former crystallizing in the volume, while the latter on the surface. The EPMA results confirmed a small concentration of boron in the oxyapatite crystal structure. RE cations were incorporated in the glass, as well as in powellite, oxyapatite, and in the case of Yb 3+ , keiviite (Yb 2 Si 2 O 7 ). Raman spectroscopy showed that the primary vibration band for molybdate MoO 4 2- in the glasses was strongly affected by the ionic field strength of the modifying cations (alkali, alkaline earth, and RE), suggesting their proximity to the MoO 4 2- ions in the glass, though the MoO bond length and coordination according to XAS suggested little local change.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Structure and magnetic properties of Ba{sub 5}Ce{sub 1.25}Mn{sub 3.75}O{sub 15}, a new 10H-polytype in the Ba-Ce-Mn-O system

Based on the peculiar magnetic properties that are observed in pseudo one-dimensional manganites, we decided to synthesize the new Ba{sub 5}Ce{sub 1.25}Mn{sub 3.75}O{sub 15} compound. The preparation was performed by solid state reaction in air at about 1350 Degree-Sign C, for which we found that the compound crystallizes in a hexagonal symmetry with space group P6{sub 3}/mmc (No-194) and cell parameters a=b=5.7861(2) A and c=23.902(1) A. The structural description was correlated with neutron diffraction and bond valence calculations, confirming the presence of Ce{sup 4+} and Mn{sup 4+} segregated in the different crystallographic positions. Ba{sub 5}Ce{sub 1.25}Mn{sub 3.75}O{sub 15} displays evidence for strong AFM couplings already set at room temperature. The main arrangement of Mn{sup 4+} in magnetically isolated tetramers of face-sharing octahedra is responsible for a metamagnetic-like transition around 50 K. - Graphical abstract: The new Ba{sub 5}Ce{sub 1.25}Mn{sub 3.75}O{sub 15} polytype shows strong AFM couplings in magnetically isolated [Ce{sub 0.25}Mn{sub 3.75}O{sub 15}] tetramers of face-sharing octahedral, resulting in a metamagnetic-like transition around 50 K. Highlights: Black-Right-Pointing-Pointer Ba{sub 5}Ce{sub 1.25}Mn{sub 3.75}O{sub 15}, a new 10H polytype, has been prepared in the Ba-Ce-Mn-O system. Black-Right-Pointing-Pointer The compound crystallizes in the P6{sub 3}/mmc space group with (cchhh){sub 2} stacking sequence. Black-Right-Pointing-Pointer [Ce{sub 0.25}Mn{sub 3.75}O{sub 15}] tetramers are separated by [CeO{sub 6}] octahedra in the structure. Black-Right-Pointing-Pointer Instead of robust AFM ordering, a metamagnetic-like transition is found around 50 K.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Mechanosynthesis and structural characterization of nanocrystalline Ce{sub 1–x}Y{sub x}O{sub 2–δ} (x=0.1–0.35) solid solutions

A series of nanostructured fluorite-type Ce{sub 1–x}Y{sub x}O{sub 2–δ} (0≤x≤0.35) solid solutions, prepared via high-energy milling of the CeO{sub 2}/Y{sub 2}O{sub 3} mixtures, are investigated by XRD, HR-TEM, EDS and Raman spectroscopy. For the first time, complementary information on both the long-range and short-range structural features of mechanosynthesized Ce{sub 1–x}Y{sub x}O{sub 2–δ}, obtained by Rietveld analysis of XRD data and Raman spectroscopy, is provided. The lattice parameters of the as-prepared solid solutions decrease with increasing yttrium content. Rietveld refinements of the XRD data reveal increase in microstrains in the host ceria lattice as a consequence of yttrium incorporation. Raman spectra are directly affected by the presence of oxygen vacancies; their existence is evidenced by the presence of vibration modes at ~560 and ~600 cm{sup –1}. The detailed spectroscopic investigations enable us to separate extrinsic and intrinsic origin of oxygen vacancies. It is demonstrated that mechanosynthesis can be successfully employed in the one-step preparation of nanocrystalline Ce{sub 1–x}Y{sub x}O{sub 2–δ} solid solutions. - Graphical abstract: Mechanosynthesis of nanocrystalline Ce{sub 1–x}Y{sub x}O{sub 2–δ} (x=0.1–0.35) solid solutions. - Highlights: • One-step mechanosynthesis of nanoscale Ce{sub 1–x}Y{sub x}O{sub 2–δ} (0≤x≤0.35) solid solutions. • Complementary information on the long-range and short-range structural features of mechanosynthesized Ce{sub 1–x}Y{sub x}O{sub 2–δ} is provided. • Structural variations as a response to the yttrium doping. • Separation of extrinsic and intrinsic origin of the induced oxygen vacancies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Local atomic arrangement and scintillation properties of Eu- and Ce-doped NaYP{sub 2}O{sub 7}

Direct determination of rare earth location and local environment in NaYP{sub 2}O{sub 7} are presented. Undoped and Ln-doped NaYP{sub 2}O{sub 7} (Ln=Eu, Ce) were produced via PVA-assisted sol–gel method. Lattice parameters were determined from Rietveld refinement, showing monoclinic structure. XAS results suggested Eu{sup 3+} and Ce{sup 3+} are incorporated into NaYP{sub 2}O{sub 7} host in substitution to Y{sup 3+} site, with first coordination shell formed by six oxygen ions. Measurements at Eu edge showed a single peak in R space for Eu–O distribution. In this case, uniform interatomic distances implied to absence of significant disorder. Analysis at Ce edge presented different behavior, with Ce–O distribution characterized by a split peak in R space. Nearest neighborhood was found to be distributed with Ce occupying an off-center position in Y site. Under X-ray excitation, {sup 5}D{sub 0}→{sup 7}F{sub J} emission lines of Eu{sup 3+} were identified for NaYP{sub 2}O{sub 7}:Eu. NaYP{sub 2}O{sub 7}:Ce presented a broad emission formed by 5d→{sup 2}F{sub J} transitions of Ce{sup 3+}, with the superposition attributed to the effect of distorted oxygen octahedra around the dopant ions. - Graphical abstract: EuO{sub 6} and CeO{sub 6} octahedral arrangement relative to Y site in NaYP{sub 2}O{sub 7} host, and XEOL emission of corresponding doped samples. - Highlights: • Lattice parameters of NaYP{sub 2}O{sub 7} undoped sample confirmed monoclinic structure. • Dopants Eu and Ce are incorporated in the trivalent state. • Local order of Eu{sup 3+} and Ce{sup 3+} dopants substituting Y{sup 3+} consist of octahedral symmetry. • Off-center displacement in the case of Ce{sup 3+} position was discussed. • Luminescent properties under X-ray excitation may allow practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Thermally stimulated iron oxide transformations and magnetic behaviour of cerium dioxide/iron oxide reactive sorbents

The present paper is devoted to detailed study of the magnetically separable sorbents based on a cerium dioxide/iron oxide composite annealed at temperatures T{sub a} = 773 K, 873 K, and 973 K. The X-ray diffraction and high resolution transmission electron microscopy are used to determine the phase composition and microstructure morphology. Mössbauer spectroscopy at room (300 K) and low (5 K) temperatures has contributed to more exact identification of iron oxides and their transformations Fe{sub 3}O{sub 4} → γ-Fe{sub 2}O{sub 3} (ε-Fe{sub 2}O{sub 3}) → α-Fe{sub 2}O{sub 3} in dependence on calcination temperature. Different iron oxide phase compositions and grain size distributions influence the magnetic characteristics determined from the room- and low-temperature hysteresis loop measurements. The results are supported by zero-field-cooled and field-cooled magnetization measurements allowing a quantitative estimation of the grain size distribution and its effect on the iron oxide transformations. - Highlights: •Magnetically separable sorbents based on a CeO{sub 2}/Fe{sub 2}O{sub 3} composite were investigated. •Microstructure of sorbents was determined by XRD, TEM and Mössbauer spectroscopy. •Magnetic properties were studied by hysteresis loops at room- and low-temperatures. •Phase transitions of iron oxides with increasing annealing temperature are observed.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Aluminium doped ceria–zirconia supported palladium-alumina catalyst with high oxygen storage capacity and CO oxidation activity

Graphical abstract: Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} possessed high OSC and CO oxidation activity at low temperature. - Highlights: • A new OSC material of Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} is prepared via a mechanochemical method. • Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} showed high OSC even after calcination at 1000 °C for 20 h. • Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} exhibited the highest CO oxidation activity at low temperature correlates with enhanced OSC. - Abstract: The Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst prepared by a mechanochemical route and calcined at 1000 °C for 20 h in air atmosphere to evaluate the thermal stability. The prepared Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst was characterized for the oxygen storage capacity (OSC) and CO oxidation activity in automotive catalysis. For the characterization, X-ray diffraction, transmission electron microscopy and the Brunauer–Emmet–Teller (BET) technique were employed. The OSC values of all samples were measured at 600 °C using thermogravimetric-differential thermal analysis. Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst calcined at 1000 °C for 20 h with a BET surface area of 41 m{sup 2} g{sup −1} exhibited the considerably high OSC of 583 μmol-O g{sup −1} and good OSC performance stability. The same synthesis route was employed for the preparation of the CeO{sub 2}/Pd-γ-Al{sub 2}O{sub 3} and Ce{sub 0.5}Zr{sub 0.5}O{sub 2}/Pd-γ-Al{sub 2}O{sub 3} for comparison.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Synthesis of mesoporous Bi{sub 2}O{sub 3}/CeO{sub 2} microsphere for photocatalytic degradation of Orange II dye

Graphical abstract: - Highlights: • Bi{sub 2}O{sub 3}/CeO{sub 2} microspheres were successfully synthesized by a hydrothermal procedure. • Bi{sub 2}O{sub 3}/CeO{sub 2} microspheres were used to remove wastewater pollutant containing azo dye. • The activity of Bi{sub 2}O{sub 3}/CeO{sub 2} is synergically enhanced compared to its pristine forms. - Abstract: We report on the visible-light responsive porous assembly of Bi{sub 2}O{sub 3}/CeO{sub 2} microspheres, which were synthesized via a simple hydrothermal reaction between Bi(NO{sub 3}){sub 3}·5H{sub 2}O and Ce(NO{sub 3}){sub 3}·6H{sub 2}O in the presence of ethylene glycol and ethanol. Systematic structural (X-ray diffraction (XRD)), morphological (field emission scanning electron microscopy (FE-SEM) and transmission electron microscopic (TEM)), BET surface area and diffuse reflectance spectral (DRS) analyses were carried out to characterize the formed product. The effects of experimental parameters on the microstructural and morphological behavior of Bi{sub 2}O{sub 3}/CeO{sub 2} composites were discussed. The semiconductor material as obtained was evaluated as a heterogeneous photocatalyst for the photolytic degradation of an azo dye in water and the degradation was found to follow pseudo-first-order rate kinetics. The study compares the rate constants of the new hybrid catalyst to a pristine Bi{sub 2}O{sub 3} and CeO{sub 2}, which has excellent catalytic properties under visible light irradiation for the degradation of Orange II dye.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Fabrication and microstructure of cerium doped lutetium aluminum garnet (Ce:LuAG) transparent ceramics by solid-state reaction method

Highlights: • We fabricate Ce doped lutetium aluminum garnet ceramics by solid-state method. • The raw materials include Lu{sub 2}O{sub 3} nanopowders synthesized by co-precipitation method. • The density of the transparent ceramics reach 99.7% of the theoretical value. • The optical transmittance of the bulk ceramic at 550 nm was 57.48%. • Some scattering centers decrease the optical characteristic of the ceramic. - Abstract: Polycrystalline Ce{sup 3+} doped lutetium aluminum garnet (Ce:LuAG) transparent ceramics fabricated by one step solid-state reaction method using synthetic nano-sized Lu{sub 2}O{sub 3}, commercial α-Al{sub 2}O{sub 3} and CeO{sub 2} powders were investigated in this paper. The green compacts shaped by the mixed powders were successfully densified into Ce:LuAG transparent ceramics after vacuum sintering at 1750 °C for 10 h. The in-line optical transmittance of the Ce:LuAG ceramic made by home-made Lu{sub 2}O{sub 3} powders could reach 57.48% at 550 nm, which was higher than that of the ceramic made by commercial Lu{sub 2}O{sub 3} powders (22.96%). The microstructure observation showed that light scattering centers caused by micro-pores, aluminum segregation and refraction index inhomogeneities induced the decrease of optical transparency of the Ce:LuAG ceramics, which should be removed and optimized in the future work.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Synthesis and electrochemical assessment of Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} ceramics and derived composite electrolytes

Highlights: • Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} prepared for the first time through solid state reaction. • High energy milling needed to assist the ceramic route. • Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} is oxide-ion conductor in air and n-type conductor at low pO{sub 2}. • Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} decomposes slightly when exposed to alkaline carbonates. • Composites based on Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} show standard electrical performance. - Abstract: Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} was prepared for the first time through high temperature (1600 °C for 5 h) solid state reaction, after high energy milling to enhance the mechano-chemical interaction of precursor oxides (CeO{sub 2} and Yb{sub 2}O{sub 3}). Single phase formation was confirmed by powder X-ray diffraction. Impedance spectroscopy data obtained under wide temperature (300–800 °C) and oxygen partial pressure (0.21 to about 10{sup −25} atm) ranges indicates that this material exhibits predominant oxide-ion conductivity under oxidizing conditions while n-type electronic conductivity prevails at low oxygen partial pressure. The mixed oxide shows modest ionic conductivity (1.1 × 10{sup −3} S cm{sup −1} at 800 °C) with activation energy of 1.3 eV in the 600–800 °C temperature range. When combined with molten carbonates (Li{sub 2}CO{sub 3} + Na{sub 2}CO{sub 3}, 1:1 molar ratio) to produce composite electrolytes, Ce{sub 0.5}Yb{sub 0.5}O{sub 1.75} slightly decomposed. However, the composite electrical performance is still acceptable and closely matches the conductivity of similar materials (>0.1 S cm{sup −1} immediately above 500 °C)

36 MATERIALS SCIENCE↗
DOE OSTI2016

A flux-free method for synthesis of Ce{sup 3+}-doped YAG phosphor for white LEDs

Highlights: • A series of CeF{sub 3}-doped YAG phosphors were successfully synthesized. • CeF{sub 3} not only can be used as the Ce{sup 3+} source but also can play the role of a flux. • The QY of YAG:CeF{sub 3} phosphor is 91% but the QY of YAG:Ce{sub 2}O{sub 3} phosphor is just 80%. • YAG:CeF{sub 3} phosphor exhibits excellent thermal stability. • Using CeF{sub 3} as the Ce{sup 3+} source is a promising flux-free method to prepare YAG:Ce{sup 3+}. - Abstract: A series of CeF{sub 3}-doped Y{sub 3}Al{sub 5}O{sub 12} (YAG:CeF{sub 3}) phosphor, CeO{sub 2}-doped Y{sub 3}Al{sub 5}O{sub 12} (YAG:Ce{sub 2}O{sub 3}) phosphor and 5 wt% BaF{sub 2} added YAG:Ce{sub 2}O{sub 3} (YAG:Ce{sub 2}O{sub 3} + BaF{sub 2}) phosphor were successfully synthesized by a solid-state reaction method. The microstructure, morphology, luminescence spectra, luminescence quantum yield (QY) and thermal quenching of the phosphors were investigated. The QY of YAG:CeF{sub 3} phosphor is 91% but the QY of YAG:Ce{sub 2}O{sub 3} phosphor is just 80%. At 150 °C, the luminescence intensity of YAG:CeF{sub 3} phosphor, YAG:Ce{sub 2}O{sub 3} phosphor and YAG:Ce{sub 2}O{sub 3} + BaF{sub 2} phosphor was 85%, 86% and 89% of that measured at 25 °C, respectively. The comprehensive performance of the white LED lamp employing YAG:CeF{sub 3} phosphor is even better than that of the white LED lamp employing YAG:Ce{sub 2}O{sub 3} + BaF{sub 2} phosphor. The experimental results show that it is a promising flux-free method to synthesize Ce{sup 3+}-doped YAG phosphor by employing CeF{sub 3} as the Ce{sup 3+} source.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Mn-substituted cerium oxide nanostructures and their magnetic properties

Highlights: • Mn{sub x}Ce{sub 1-x}O{sub 2} (0.1 ≤ x ≤ 0.5) nanostructures were prepared by one step microwave refluxing method. • The saturation magnetization values for the samples rose with increased Mn content. • The oxygen vacancies inherently played crucial role in increasing the magnetization values. - Abstract: In this study, we report the magnetic properties of nanostructured Mn{sub x}Ce{sub 1-x}O{sub 2} (0 0.1 ≤ x ≤ 0.5) materials, synthesized via microwave refluxing technique. Phase purity of the samples was investigated using the structural characterization techniques such as X-ray diffraction (XRD) and transmission electron microscopy (TEM). These analyses indicated the substitution of Ce-ions with Mn-ions in the lattice. The progressive increase in the oxygen vacancies with increased dopant concentration was demonstrated by Raman, UV–vis and photoluminescence spectroscopic studies. X-ray photoelectron spectroscopy analysis further supported the presence of Mn{sup 2+}, Ce{sup 3+} and Ce{sup 4+} ions as well as oxygen vacancies in the samples. The Mn substituted CeO{sub 2} nanostructures were found to exhibit room temperature ferromagnetism (RTFM). There was a continuous improvement in the saturation magnetization (M{sub S}) values with increased Mn concentration. This might be due to the prevalence of surface oxygen vacancies and the systematic rise in their concentration with increased dopant content.

77 NANOSCIENCE AND NANOTECHNOLOGY↗