Rapid synthesis of YAG phosphor by facile mechanical method

In this study, synthesis of yttrium aluminum garnet (YAG):Ce³⁺ phosphor powders for white light emitting diodes was investigated by mechanical method using the attrition-type mill with no external heating and no flux in dry phase. High mechanical energy input to the starting powder mixture of Y₂O₃, Al₂O₃ and CeO₂ achieved the synthesis of YAG:Ce³⁺ without any flux materials. X-ray diffraction patterns of the processed powders after 5 min processing revealed the peaks of YAG were clearly identified. The maximum temperature of the mill chamber during the processing was 240℃. The YAG phosphor obtained by the mechanical method revealed the internal quantum yield of 65% in the case of the sample mechanically processed under a reducing atmosphere. The synthesized powder showed granule structure consisting of submicron size of YAG particles, which is better handling for the fabrication of light emitting diode devices.     

Phase composition,structural, and plasma erosion properties of ceramic coating prepared by suspension plasma spraying

Y₃Al₅O₁₂ (YAG), Y₂O₃, and Al₂O₃ ceramic coatings were manufactured to investigate the plasma erosion properties. The X‐Ray Diffraction (XRD) analysis confirmed that YAG coating was synthesized successfully by Y₂O₃ and Al₂O₃ mixture suspension using the plasma spraying method. Meanwhile, metastable phases were found in Y₂O₃ and Al₂O₃ coatings due to the quenching in cooling process of melted droplets. The coating surface morphology and microstructure of cross sections were characterized by SEM. The results reveal that coatings are composed by ultrafine splats and exhibit dense lamellar structure. The plasma erosion properties were evaluated at different etching test power under Ar/CF₄/O₂ plasma gas. The experimental results clarify that both of YAG and Y₂O₃ coatings show the better plasma erosion resistance than Al₂O₃ coatings. The formation of fluorination layer surface prevents the coatings from further erosion with plasma gas. Moreover, the etching rate of coatings depended on the fluorination and removing rate of fluoride layer.     

Oxide/oxide composites in the system Cr2O3-Y2O3-Al2O3

Ceramic compacts in the systems Al₂O₃–Y₂O₃, Cr₂O₃–Y₂O₃ and Y₃(Cr_yAl_1-y)₅O₁₂ (Cr-doped YAG) were prepared by solid state reaction in calcined co-precipitated powder mixtures of appropriate compositions. Various solid-solution phases were formed, e.g. Y₃(Al_1-xCr_x)₅O₁₂, YAl_yCr_1-yO₃ and Al_2-xCr_xO₃. Composite materials in the pseudo-binary or ternary systems Al₂O₃–Y₃Al₅O₁₂, Cr₂O₃–Y₂O₃ and Y₃(Al_1–xCr_x)₅O₁₂–YAl_yCr_1–yO₃–(Al_zCr_1−z)₂O₃ were obtained by hot-pressing appropriate powder precursors at 1600–1650°C for 1 h. The microstructure of the prepared materials was studied in a scanning electron microscope with element analysis facilities. X-ray diffraction was used to reveal the phases present and their lattice parameters. The chemical compatibility of these phases was investigated. The results are discussed with a special emphasis on the solubility of Cr in the YAG structure, and on the compatibility relationship between Cr-doped YAG and its neighbouring phases. A gel-coating process for preparing Al₂O₃–YAG composites with tailored microstructures is also described.     

Ultrafast formation of Al2O3–Y3Al5O12 eutectic ceramic by flash sintering

In this study, a dense Al₂O₃–Y₃Al₅O₁₂ (YAG) ceramic was synthesized by flash sintering a powder mixture of Al₂O₃ and Y₂O₃ in less than 150 seconds at a furnace temperature of 1350°C. The resultant ceramic has a well-defined eutectic structure consisting of alternating Al₂O₃ and YAG layers. The hardness and fracture toughness of the ceramic were measured to be 18.5 GPa and 4.3 MPa.m^1/2, respectively. These values are comparable to those of similar eutectic ceramics made by directional solidification techniques. The results suggest a new method for making high-performance eutectic ceramics, which could be applied in other systems.     

Partial wet route for YAG powders synthesis leading to transparent ceramic: A core–shell solid-state reaction process

Synthesis of Y₃Al₅O₁₂ (YAG) powders respectively presents morphology control and chemical stoichiometry problems when employing the solid-state reaction or the wet-chemical route. YAG powder retaining the morphology of Al₂O₃ powder was designed and synthesized via a partial wet-chemical process with yttrium ions precipitating on the Al₂O₃ particles. The formation process of the Y-compound/Al₂O₃ core–shell structure is discussed on the basis of zeta-potential measurements and HRTEM results. Two stages, including direct precipitation at the surface of the Al₂O₃ particles and the assembly of the yttrium precipitate from explosive nucleation onto the yttrium compound-coated Al₂O₃ particles, are proposed. A spherical surface reaction process is illustrated. A pure YAG phase can be realized at a temperature about 300 °C lower than that of the traditional solid-state reaction process.     

Synthesis of YAG powders by the co-precipitation method

YAG (Y₃Al₅O₁₂) powders have been prepared by co-precipitation technique in which NH₄HCO₃ is used as a precipitant and Y₂O₃, A1((NO₃)₃·9H₂O—as raw materials. Two kinds of surfactant are added into the solution, i.e. Polyethylene glycol (PEG10000) as steric stabilizer and (NH₄)₂SO₄ as electrical stabilizer. The composition of YAG precursor, the phase formation process of YAG and the properties of the powders were investigated by means of differential scanning calorimetry and thermogravimetry analysis (DSC–TG), X-ray diffraction (XRD), Fourier transformation infrared spectroscopy (FT-IR) and Scanning electron microscopy (SEM). The results of XRD show that phase YAG crystallite can be obtained as precursors when heated at 900 °C for 2 h. The powders loosely dispersed with narrow size distribution and spherical shapes could be observed by SEM. It has been found that the presence of PEG and (NH₄)₂SO₄ is beneficial for the dispersion of the resulting YAG powder. In the presence of surfactants, the synthesized product consists of highly dispersed nano-sized particles.     

Strain measurement of the directionally solidified eutectic Al2O3/Y3Al5O12 (YAG) ceramic by neutron diffraction

The eutectic Al₂O₃/Y₃Al₅O₁₂ (YAG) ceramic has been reported to be composed by single-crystalline Al₂O₃ and YAG, the microstructure of which is characterized by the three dimensionally entangled two single-crystalline composites. Therefore, Laue diffraction and high-resolved energy-dispersive neutron diffraction (time-of-flight method) techniques were employed to measure residual strain precisely. It was found that the YAG phase was in tension and the Al₂O₃ phase was in compression with strains in the range of ∼10⁻⁴ at room temperature through comparing the lattice spacings of the sintered YAG and sintered Al₂O₃ as the references of strain-free materials.     

Effect of Y2O3 on the corrosion resistance of two-step sintered Al5Y3O12-MgAl2O4 sidewalls in the aluminum electrolyte

Magnesium–aluminum spinel (MAS) precursor powder was synthesized through a microwave hydrothermal method. The synergistic effects of sintering process and sintering aids on the densification, hardness and corrosion resistance of MAS were revealed. X-ray diffraction analysis (XRD), Archimedes’ drainage method, fully automatic micro-Vickers hardness test and scanning electron microscopy (SEM) were performed to analyze the phase composition, bulk density, hardness microstructure and corrosion depth of the samples, respectively. Results revealed that the best two-step sintering condition is 1650 °C/3 min/1550 °C/20 h. The MAS products obtained under the best condition have clear grain boundaries, uniform particle size distribution, and few pores. When the amount of Y₂O₃ added is 4 wt.%, Y₂O₃ and Al₂O₃ form the second-phase solid solution Al₅Y₃O₁₂, which activates the crystal lattice and benefits the sintering densification of MAS. Under these conditions, the relative density of the MAS composite ceramics prepared is relatively large (95.94 %), the grain size is relatively uniform, the hardness is relatively large (1264 HV), and the corrosion depth is relatively small (94.58 μm).     

Structure formation in yttrium aluminum garnet (YAG) fibers

Polycrystalline yttrium aluminum garnet (YAG, Y₃Al₅O₁₂) fibers were prepared from aqueous solutions of aluminum chlorohydrate and yttrium chloride. Fiber processing was accomplished via dry spinning. Poly(vinylpyrrolidone) (PVP) was used as spinning aid. Polycrystalline YAG fibers were obtained by pyrolysis of the green fibers followed by sintering at defined temperatures in air. Ceramic fibers were 9–16 μm in diameter. Differential scanning calorimetry/thermogravimetric analysis coupled with mass spectrometry (DSC/TGA-MS) showed an exothermic peak at 920 °C assigned to the crystallization of YAG and an overall ceramic yield of 38% at 1400 °C. X-ray diffraction (XRD) analysis showed that phase-pure YAG can be obtained at 1600 °C after intermediate formation of Y₂O₃ and monoclinic yttrium aluminum oxide (YAM, Y₄Al₂O₉) phases.     

CaO–SiO2–Al2O3–Y2O3 glasses as model grain boundary phases for Si3N4 ceramics

The glasses with compositions derived from the eutectic composition [37.78 (Y₃Al₅O₁₂)·62.22 (SiO₂)] of the quasi-binary glass system (Y₃Al₅O₁₂)-(SiO₂) with addition of up to 20 mol.% CaO were investigated as model grain boundary phases for Si₃N₄ ceramics. The influence of CaO as model impurity on the physical properties of the glass (density, thermal expansion) and on the crystallisation behaviour was studied. Although the initial composition of the basic glass was that of yttrium-aluminium garnet (Y₃Al₅O₁₂–YAG), no crystalline YAG was detected. Apart from yttrium disilicate (Y₂Si₂O₇), anorthite (CaAl₂Si₂O₈), tricalcium aluminate (Ca₃Al₂O₆), and calcium yttrium oxide silicate (Ca₄Y₆O(SiO₄)₆), a new phase was detected, not found in the powder diffraction file (PDF) database. Cavities were formed within the devitrified glass due to the volume contraction after crystallisation. Possible implications for the mechanical properties of Si₃N₄ ceramics sintered with addition of Y₂O₃–Al₂O₃ are discussed in terms of the observed compositional dependences of the physical properties of CaO–Y₂O₃–Al₂O₃–SiO₂ glasses.     

Al2O3–Ce:YAG composite phosphor ceramics for white laser lighting: Novel preparation and regulatable properties

In this work, a series of Al₂O₃–Ce:YAG phosphor powders were synthesized by regulating the excess Al³⁺ of (Y,Ce)₃Al₅O₁₂ via coprecipitation method for the first time, where Al³⁺, Ce³⁺, and Y³⁺ elements were uniformly distributed. With the increase of Al³⁺ content, the morphology of the powders changed from wormlike shapes to flaky shapes, and Y₃Al₅O₁₂ phases had a tendency to convert to YAlO₃ phases. The x wt.% Al₂O₃–(Y_0.999Ce_0.001)₃Al₅O₁₂ (x = 20, 30, 40, 50, 60, and 70) composite phosphor ceramics (CPCs) were obtained by vacuum sintering (1775°C × 10 h), where Al₂O₃ and Ce:YAG phases were also well-distributed. When the Al₂O₃ content was 30–40 wt.%, the average grain size of Al₂O₃ was close to that of Ce:YAG. A solid-state laser lighting device was constructed by a 450 nm laser source and CPCs in a reflection mode. By adjusting the laser power, the correlated color temperature (CCT) values of white laser diodes (LDs) were achieved close to the standard white light of 6500 K. Impressively, the white LDs equipped with the 40 wt.% Al₂O₃-containing CPCs showed the optimum CCT of 6498 K (color coordinates: 0.31 and 0.38), as well as a high luminous flux of 1169 lm and efficiency of 166 lm/W at the LD power of 7.05 W. This work has provided a potential idea to optimize the composition uniformity of Al₂O₃–Ce:YAG CPCs as also to explore their excellent performance in the application of white laser lighting.     

Effect of YAG content on creep resistance and mechanical properties of Al2O3-YAG composite

Comprehensive study on effect of YAG amount on densification, creep resistance and room-temperature mechanical properties of Al₂O₃-YAG composite pressureless sintered at 1600 °C was conducted. The main goal was to optimize the amount of YAG in order to fabricate a composite with improved creep resistance and sufficiently good room-temperature mechanical properties. The composite was made by mixing a commercially available Al₂O₃ powder with fine YAG powder obtained by glycine-nitrate combustion synthesis starting from aluminum nitrate and yttrium nitrate. Increased driving force for sintering of fine YAG powder allowed fabrication of dense Al₂O₃-YAG composite with up to 30 vol% YAG. The presence of YAG was found to be very effective in improving creep resistance of Al₂O₃-YAG composite. Large Y³⁺ ions blocked diffusion along Al₂O₃ grain boundaries, reduced diffusivity and therefore enhanced creep resistance of Al₂O₃-YAG composite which continuously increased as the YAG amount increased. Тhe presence of YAG was also found to improve mechanical properties such as hardness and elastic modulus. The improvement of these properties was ascribed to increased density of Al₂O₃-YAG composites owing to high sintering activity of YAG powder. While fracture strength of the composite can be as high as that of monolithic Al₂O₃, fracture toughness of composite decreased continuously as the YAG content increased. The decrease was ascribed to transgranular fracture of both YAG and Al₂O₃ grains in samples containing larger amounts of YAG. The proper balance between fracture toughness and creep resistance was found in composite containing 18 vol% YAG which had considerably improved creep resistance accompanied by a relatively small decrease in fracture toughness.     

Phase composition,microstructure, and microwave dielectric properties of non-stoichiometric yttrium aluminum garnet ceramics

A series of Y_3+xAl₅O₁₂ (?0.12 ≤ x ≤ 0.12) ceramics were prepared via a solid-state reaction under a vacuum sintering environment to investigate the impact of variations in different cation composition on the phase composition, microstructure, and microwave dielectric properties of yttrium aluminum garnet (Y₃Al₅O₁₂; YAG) ceramics. X-ray diffraction analyses revealed that Al₂O₃ precipitates in the Al-excess samples. In contrast, the YAlO₃ secondary phase appeared in the Y-excess samples, and variations in the content of both contributed to an increase in lattice parameters. The Rietveld refinement results showed that the lattice parameters and unit cell volume increased as the |x| value increased. The secondary phases of granular Al₂O₃ and YAlO₃ crystallized at the extended grain boundaries in samples with excess Al and Y were visible in the scanning electron microscopy images. The electron diffraction patterns confirmed that a small amount of Y₂O₃ promoted continuous phase boundaries and facilitated the release of internal stresses. Ultimately, after sintering at 1750 °C for 12 h and at x = 0.03, the microwave dielectric properties of the non-stoichiometric YAG ceramic sample were ε_r = 11.18, Q×f = 236936 GHz, and τ_f = ?35.9 ppm/℃.     

Crystallographic characterization of silicon nitride ceramics sintered with Y2O3–Al2O3 or E2O3–Al2O3 additions

Silicon nitride ceramics were sintered using Y₂O₃–Al₂O₃ or E₂O₃–Al₂O₃ (E₂O₃ denotes a mixed oxide of Y₂O₃ and rare-earth oxides) as sintering additives. The intergranular phases formed after sintering was investigated using high-resolution X-ray diffraction (HRXRD). The use of synchrotron radiation enabled high angular resolution and a high signal to background ratio. Besides the appearance of β-Si₃N₄ phase the intergranular phases Y₃Al₅O₁₂ (YAG) and Y₂SiO₅ were identified in both samples. The refinement of the structural parameters by the Rietveld method indicated similar crystalline structure of β-Si₃N₄ for both systems used as sintering additive. On the other hand, the intergranular phases Y₃Al₅O₁₂ and Y₂SiO₅ shown a decrease of the lattice parameters, when E₂O₃ was used as additive, indicating the formation of solid solutions of E₃Al₅O₁₂ and E₂SiO₅, respectively.     

The effect of precursor composition and sintering additives on the formation of β-sialon from Al, Si and Al2O3 powders

A study was performed to investigate the effect of increasing the Al or Al₂O₃ precursor content, above the stoichiometric amount, on the formation of β-sialon by pressureless sintering of Al, Si and Al₂O₃ powders in flowing nitrogen gas. The effect of adding Y₂O₃ or Fe to the precursor mixture, on the β-sialon formation, was also studied. The phase morphology and yield produced by the various compositions were examined using X-ray diffraction (XRD). Additional Al₂O₃ decreases the β-sialon phase yield and results in a greater amount of Al₂O₃ in the final sintered material. Additional Al improved the conversion to β-sialon up to a maximum of 4 wt% Al beyond which the β-sialon:15R sialon ratio in the sintered material decreases. 1 wt% Y₂O₃ was determined to be the optimum sintering additive content, as yttrium aluminium garnet (YAG) was found to be present in materials formed from higher Y₂O₃ containing precursors. The presence of Fe in the precursor powder retards the formation of β-sialon by preferentially forming Fe silicides at low temperatures, thus depleting the reaction system of elemental Si, favouring the formation of 15R sialon.     

CHARACTERIZATION OF CERIUM-DOPED YTTRIUM ALUMINIUM GARNET NANOPOWDERS SYNTHESIZED VIA SOL-GEL PROCESS

In this work the sol-gel process was used to prepare Ce-doped yttrium aluminium garnet (Y ₃ A l ₅ O ₁₂, YAG) samples. The synthesis products were characterized by infrared spectroscopy (IR), X-ray powder diffraction analysis (XRD), and transmission electron microscopy (TEM). The particle size and luminescence properties of synthesized samples were also determined. The XRD patterns of Y ₃ A l ₅ O ₁₂:Ce samples showed that phase purity of garnets depends on the synthesis temperature and concentration of dopant. The YAG:Ce samples calcined at 1000°C showed the formation of single-phase YAG in the whole doping range (from 0 up to 10 mol% of Ce). However, during calcination at 1300°C the formation of CeO₂ as an impurity phase at >4 mol% of Ce was observed. The mean particle size of Y ₃ A l ₅ O ₁₂:Ce sample (4 mol% of Ce) synthesized at 1300°C was determined to be approximately 180–280 nm. The luminescence properties of Ce-doped YAG also depend on cerium concentration in the samples. The highest emission (λ _ex  = 450nm) intensity was determined for Y ₃ A l ₅ O ₁₂:Ce samples doped by 5–6 mol% of Ce.     

Preparation of uniformly dispersed YAG ultrafine powders by co-precipitation method with SDS treatment

Uniformly dispersed yttrium aluminum garnet (Y₃Al₅O₁₂, YAG) ultrafine powders were synthesized by co-precipitating a mixed solution of aluminum and yttrium nitrates with ammonium hydrogen carbonate in the presence of sodium dodecyl sulfate (SDS) as dispersing agent. The primary purpose of introducing SDS was to protect YAG particles from agglomeration. The evolution of phase composition and micro-structure of the as-synthesized YAG powders were characterized by thermogravimetry/differential scanning calorimetry, X-ray diffraction, infrared spectra and scanning electron microscopy. The results showed that phase-pure YAG powders could be achieved by calcination of the precursor at 900 °C for 2 h. Uniformly dispersed YAG powders with a particle size of approximately 90-100 nm were obtained with optimum molar ratio of Al³⁺ to SDS at 2. And excessive SDS restrained good dispersion of the YAG powders. The dispersion mechanism of SDS in the preparation process was discussed.     

The influence of Gd doping on thermophysical properties,elasticity modulus and phase stability of garnet-type (Y1-xGdx)3Al5O12 ceramics

In this work, Gd³⁺ was selected to partially substitute the Y³⁺ in yttrium aluminum garnet (YAG) in order to improve the thermophysical properties of YAG. A series of (Y_1-xGd_x)₃Al₅O₁₂ (x = 0, 0.1, 0.2, 0.3, 0.4) ceramics were synthesized through chemical co-precipitation route. The microstructure, thermophysical properties and elasticity modulus of (Y_1-xGd_x)₃Al₅O₁₂ were investigated. The (Y_1-xGd_x)₃Al₅O₁₂ ceramics was comprised of single garnet-type Y₃Al₅O₁₂ phase. The thermal conductivities of (Y_1-xGd_x)₃Al₅O₁₂ bulk samples decreased with increasing doping concentration to 0.2, but increased with furthering increasing the concentration to 0.4. The thermal conductivity of (Y_0.8Gd_0.2)₃Al₅O₁₂ was 1.51 W m⁻¹ K⁻¹ at 1200 °C. The average thermal expansion coefficient of (Y_0.8Gd_0.2)₃Al₅O₁₂ was slightly larger than that of Y₃Al₅O₁₂. (Y_0.8Gd_0.2)₃Al₅O₁₂ bulk sample exhibited the lowest elasticity modulus among the investigated (Y_1-xGd_x)₃Al₅O₁₂. In addition, (Y_0.8Gd_0.2)₃Al₅O₁₂ ceramic remained good phase stability from room temperature to 1600 °C.     

Sol–gel synthesis of YAG/Al2O3 long fibres from water solvent systems

Y₃Al₅O₁₂(YAG)/Al₂O₃ long fibres were prepared by a sol–gel method using water as the solvent. They were synthesized from aluminium nitrate and chloride solutions, aluminium salt, aluminium metal and Y₂O₃. The starting materials were dissolved by refluxing at 100°C for 2–18 h and were then condensed. The fibre spinnability was examined by a hand drawing method using a glass rod. In the nitrate solution system, the composition range available for fibre preparation was very limited because nitrate ions decomposed during the refluxing, raising the solution pH and precipitating the Y component. On the other hand, the composition range of the fibres prepared from the chloride system was 0/10⩽YAG/Al₂O₃⩽6/4 (volume ratio) and was wider than that from the nitrate system. The YAG/Al₂O₃ fibres prepared by firing at 1300°C became denser with faster heating rates. The grain size in the fired fibres was small, below the firing temperature at 1400°C, but increased greatly above that temperature.     

Efficient photocatalytic degradation of organic dyes over titanium dioxide coating upconversion luminescence agent under visible and sunlight irradiation

In order to use the sunlight efficiently, a new titanium dioxide (TiO₂) photocatalyst with high catalytic activity under visible light irradiation was prepared with sol–gel technique. In this work, an upconversion luminescence agent, crystallized Er³⁺:Y₃Al₅O₁₂, was synthesized and its characters were determined. It is found that this crystallized Er³⁺:Y₃Al₅O₁₂ can emit three upconversion fluorescent peaks below 387 nm under the excitation of 488 nm visible light. Hence, this upconversion luminescence agent could transform visible light into ultraviolet light, which could satisfy the genuine requirement of TiO₂ photocatalyst. Additionally, the upconverison mechanisms were also discussed. Meanwhile, the prepared TiO₂ photocatalysts coating upconversion luminescence agent were characterized by powder X-ray diffraction (XRD) and transmission electron microscopy (TEM). The photocatalytic activity of prepared TiO₂ powder was tested through the degradation of congo red in aqueous solution as a model compound under visible and sunlight irradiation. To affirm the complete mineralization, the ion chromatography and total organic carbon (TOC) were used to observe the mineralized anions and organic residues. The experimental results proved that the prepared TiO₂ photocatalyst coating crystallized Er³⁺:Y₃Al₅O₁₂ behaved much higher photocatalytic activity under visible light and sunlight irradiation, and was able to decompose the congo red in aqueous solution efficiently. Therefore, this method may be envisaged as a novel technology for treating dyes wastewater using solar energy, especially for textile industries in developing countries.