JCPDS Research Articles

Crystal Structure Determination from Powder Diffraction Patterns with Generative Machine Learning.

Powder X-ray diffraction (PXRD) is a cornerstone technique in materials characterization. However, complete structure determination from PXRD patterns alone remains time-consuming and is often intractable, especially for novel materials. Current machine learning (ML) approaches to PXRD analysis predict only a subset of the total information that comprises a crystal structure. We developed a pioneering generative ML model designed to solve crystal structures from real-world experimental PXRD data. In addition to strong performance on simulated diffraction patterns, we demonstrate full structure solutions over a large set of experimental diffraction patterns. Benchmarking our model, we predicted the structure for 134 experimental patterns from the RRUFF database and thousands of simulated patterns from the Materials Project on which our model achieves state-of-the-art 42 and 67% match rate, respectively. Further, we applied our model to determine the unreported structures of materials such as NaCu2P2, Ca2MnTeO6, ZrGe6Ni6, LuOF, and HoNdV2O8 from the Powder Diffraction File database. We extended this methodology to new materials created in our lab at high pressure with previously unsolved structures and found the new binary compounds Rh3Bi, RuBi2, and KBi3. We expect that our model will open avenues toward materials discovery under conditions which preclude single crystal growth and toward automated materials discovery pipelines, opening the door to new domains of chemistry.

Importance of powder diffraction raw data archival in a curated database for materials science applications.

In recent years, there is a significant interest from the crystallographic and materials science communities to have access to raw diffraction data. The effort in archiving raw data for access by the user community is spearheaded by the International Union of Crystallography (IUCr) Committee on Data. In materials science, where powder diffraction is extensively used, the challenge in archiving raw data is different to that from single crystal data, owing to the very nature of the contributions involved. Powder diffraction (X-ray or neutron) data consist of contributions from the material under study as well as instrument specific parameters. Having raw powder diffraction data can be essential in cases of analysing materials with poor crystallinity, disorder, micro structure (size/strain) etc. Here, the initiative and progress made by the International Centre for Diffraction Data (ICDDR) in archiving powder X-ray diffraction raw data in the Powder Diffraction FileTM (PDFR) database is outlined. The upcoming 2025 release of the PDF-5+ database will have more than 20 800 raw powder diffraction patterns that are available for reference.

Understanding Lithium-Gold Electrochemical Reactions Using Operando X-Ray Diffraction

Gold electrodes are used in lithium-based battery research as catalysts and micro / quasi-reference electrodes despite their high cost and unclear reactivity with lithium. Here we present an investigation of the electrochemical reactions of gold-lithium (Au-Li) mixtures using variable-temperature electrochemistry and operando X-ray diffraction.Multiple solid solutions (alpha, beta, delta) and intermetallic phases (AuLi3, Au4Li15) are expected based on the equilibrium phase diagram.1 Previous electrochemical investigations conclusively identified only AuLi3;2,3 alpha and beta may be bypassed during lithium insertion, and the structure of delta is unclear.4 We are unaware of any previous reports of the electrochemical formation of Au4Li15. Metastable crystallographic solutions have been proposed.5 X-ray diffraction patterns collected during the galvanostatic lithiation of gold leaf (at 60 °C and a rate of ca. C/50) are provided in Figure 1. Reference diffraction patterns and the associated Powder Diffraction File card number are indicated, along with proposed phases.4,5 X-ray and electrochemical data align with earlier results suggesting that the equilibrium alpha and beta phases are seemingly bypassed during the first insertion. Delta is the first phase to form at a potential of 0.25 V vs. Li/Li+, followed by the formation of AuLi3 at 0.15 V vs. Li/Li+ at all conditions and Au4Li15 at 0.05 V vs. Li/Li+ in select conditions. Electrochemical data suggests AuLi3 may also have a small range of solubility. Peaks associated with AuLi3 and Au4Li15 align with existing literature but peaks associated with delta do not. Reactions are reversible to delta, followed by the formation of another phase near 0.3 V vs. Li/Li+ and alpha at potentials above 0.4 V vs. Li/Li+ during lithium removal. Significant hysteresis is present in cell potential and reaction pathways in the low-lithium content region. The second cycle (not shown) is reversible between alpha (not pure gold) and the terminal phase without a significant loss in capacity. Alternative crystallographic unit cell(s) for delta and other gold-lithium phases will be described.While the delta / AuLi3 reaction exhibited a consistent potential during lithium insertion and removal, the potential otherwise varied strongly with temperature, rate, and composition, implying that gold quasi-reference electrodes may not be suitable for lithium-ion battery research.

Crystal chemistry and ionic conductivity of garnet-type solid-state electrolyte, Li5-xLa3(NbTa)O12-y

Crystal structures, microtopography, morphologies, elemental compositions, and ionic conductivity have been investigated for Li5-xLa3(Nb,Ta)O12-y using X-ray diffraction (XRD), field-emission analytical scanning and transmission electron microscopies (S/TEM), and electrochemical impedance spectroscopy. Using Rietveld refinements with powder XRD patterns, we determined that the number of Li atoms in the formula is less than 5 and that Li5-xLa3(NbTa)O12-y crystallizes in the cubic garnet structure with a space group Ia-3d. Sintering at varying temperatures (750–1000 °C) for 5 h in an ambient atmosphere produced distinct outcomes. Rietveld refinements disclosed that the sample sintered at 1000 °C (Li3.43(2)La3Nb1.07(2)Ta0.93(2)O12-y, a = 12.8361(7) Å, V = 2114.96(3) Å3) exhibited the highest ionic conductivity, while the 850 °C sample had the lowest conductivity, characterized by lower Li concentration and impurity phases (Li(Nb,Ta)3O88, Li2CO3). Analyses, including XRD and electron microscopy, confirmed the 1000 °C sample as a relatively phase pure with enhanced Li content (Li/La = 1.2), larger grains (15 μm), and uniform crystallinity. The 1000 °C sample introduced additional partially filled Li3 (96h) sites, promoting Li migration, and enhancing ionic conductivity. The resulting XRD pattern at 1000 °C has been submitted to the Powder Diffraction File as a reference.

Sonochemical Synthesis of Copper Borates: Effect of Reaction Conditions on the Characteristic Properties

The effect of ultrasonic treatment on liquid-state production and the characteristic features of synthesized powder were studied in liquid-state conditions. In sonochemical synthesis, the operation parameters of mole ratio, reaction temperature, and time were optimized. The synthesis was achieved in moderate conditions such as mole ratio of copper: sodium: boron (Cu: Na: B) 1:2:1, 70°C and 2.5 minutes. The prepared samples were identified as copper borate (Cu(BO2)2) with the powder diffraction file number "00-001-0472". The reaction yields were also increased from 50% to 71.5% with the modification of the experimental procedure. The specific FT-IR peaks were observed at 1090, 985, 872, 781 and 731 cm-1 band values. In the morphological analyses, the agglomerations of multi-angular particles were seen. The results showed the affirmative effects of the possible use of the ultrasonic treatment on both the practical synthesis and the increase of characteristics.

PDF-5+: a comprehensive powder diffraction file™ for materials characterization

For more than 80 years, the scientific community has extensively used International Centre for Diffraction Data's (ICDD®) Powder Diffraction File (PDF®) for material characterization, including powder X-ray diffraction analysis. Historically, PDF was made available for two major material types: one for inorganic analysis and the other for organic analysis. In the early years of the PDF, this two-material approach was implemented due to limited computer capabilities. With Release 2024, ICDD provides a comprehensive database consisting of the entire PDF in one database called PDF-5+, comprised of more than one million entries (1,061,898). The PDF-5+ with a relational database (RDB) construct houses extensive chemical, physical, bibliographic, and crystallographic data, including atomic coordinates and raw data, enabling qualitative and quantitative phase analysis. This wealth of information in one database is advantageous for phase identification, materials characterization, and several data mining applications in materials science. A database of this size needs rigorous data curation and structural and chemical classifications to optimize pattern search/match and characterization methods. Each entry in the PDF has an editorially assigned quality mark. An editorial comment will describe the reason if an entry does not meet the top-quality mark. The editorial processes of ICDD's quality management system are unique in that they are ISO 9001:2015 certified. Among several classifications implemented in PDF-5+, subfiles (such as Bioactive, Pharmaceuticals, Minerals, etc.) directly impact the search/match in minimizing false positives. Scientists with specific field expertise continuously review these subfiles to maintain their quality. This paper describes the features of PDF with an emphasis on the newly released PDF-5+.

Simultaneous detection of melamine and cyanuric acid using powder X‐ray diffraction

AbstractA novel, non‐destructive, powder X‐ray diffraction (P‐XRD) approach was developed and validated for the simultaneous detection of melamine (ME) and cyanuric acid (CA). Sample holders, and a range of P‐XRD X‐ray tube parameters (voltage: 25–45 kV; current: 25–45 mA), and scanning conditions (scan step size: 0.006–0.10°; step time: 50–150 s) were experimented at 2θ conditions. Based on the obtained diffraction patterns, the following conditions were optimized: sample holder: reflection‐transmission spinner, tube voltage: 45 kV, tube current: 45 mA, scan step size: 0.006°, and scan step time: 150 s. The crystalline properties were assessed and phase quantification of both ME and CA was performed using Rietveld refinement, aligning to the International Center for Diffraction Data (ICDD) PDF4+ 2023 library. The approach was validated considering repeatability, precision, and linearity, and recovery and stability studies also support the findings. The limit of detection (LOD) was found to be 0.2 to 1 wt. % per phase of powder sample. Then, spiked and real food powder samples were screened for ME and CA. To date, there is no nondestructive technique available to simultaneously detect ME and CA in a single run. The developed P‐XRD approach can find vast applications in quality testing facilities.

Crystal structure and synchrotron X-ray powder reference pattern for the porous pillared cyanonickelate, Ni(3-amino-4,4′-bipyridine)[Ni(CN)4

The structure of Ni(3-amino-4,4′-bipyridine)[Ni(CN)4] (or known as Ni-BpyNH2) in powder form was determined using synchrotron X-ray diffraction and refined using the Rietveld refinement technique (R = 8.8%). The orthorhombic (Cmca) cell parameters were determined to be a = 14.7218(3) Å, b = 22.6615(3) Å, c = 12.3833(3) Å, V = 4131.29(9) Å3, and Z = 8. Ni-BpyNH2 forms a 3-D network, with a 2-D Ni(CN)4 net connecting to each other via the BpyNH2 ligands. There are two independent Ni sites on the net. The 2-D nets are connected to each other via the bonding of the pyridine “N” atom to Ni2. The Ni2 site is of six-fold coordination to N with relatively long Ni2–N distances (average of 2.118 Å) as compared to the four-fold coordinated Ni1–C distances (average of 1.850 Å). The Ni(CN)4 net is arranged in a wave-like fashion. The functional group, –NH2, is disordered and was found to be in the m-position relative to the N atom of the pyridine ring. Instead of having a unique position, N has ¼ site occupancy in each of the four m-positions. The powder reference diffraction pattern for Ni-BpyNH2 was prepared and submitted to the Powder Diffraction File (PDF) at the International Centre of Diffraction Data (ICDD).

Calculating the reference intensity ratio of crystalline phases with unknown atomic arrangements using the lattice parameters and chemical information

The reference intensity ratio (RIR) is the intensity ratio of a specified peak of the target crystalline phase to a certain peak of the reference phase in the powder X-ray diffraction pattern of a mixture of the target and reference phases in a weight ratio of 1:1. The RIR represents the diffraction power of the target phase compared with that of the reference phase. A quantitative phase analysis (QPA) can be readily made on the basis of only a powder pattern when the RIR values of all component phases in the mixture are available. The RIR of a target phase can be measured experimentally or calculated in accordance with its crystal structure. RIR values are given in most powder diffraction files (PDFs) published by the International Centre for Diffraction Data, but there are still more than 110 000 PDFs for which the RIR is absent. Newly discovered phases may be present in a mixture as components of unknown weight fractions, for which the RIR values can be neither measured nor calculated with the currently available method. Herein is presented a new method of calculating the RIR of a crystalline phase from its lattice parameters, the chemical content of the unit cell and a list of normalized intensities of reflections over a sufficiently large diffraction angle range. The new method can be used to calculate not only the absent RIRs in the PDFs but also the RIR of a component phase of a mixture of unknown weight fraction when the lattice parameters and chemical content of the unit cell of the corresponding phase are known.

Isothermal section of the ZrO2–HfO2–Nd2O3 ternary phase diagram at 1100 °C

In the presented work, based on the results obtained by X-ray diffraction and microstructural analysis, phase equilibria have been studied and an isothermal section of the ZrO2–HfO2–Nd2O3 ternary phase diagram at 1100 °C has been constructed. Unit cell parameters were calculated by the least squares method using the LATTIC software. The International Powder Standards Committee database (JSPSDS International Center for Diffraction Data 1999) was used to determine the phase composition.It was found that in the studied system are formed regions of solid solutions based on a cubic fluorite-type (F) modification, a tetragonal (T) modification of ZrO2, a monoclinic (М) modification of HfO2, a hexagonal (А) modification of Nd2O3, as well as an ordered (Py) pyrochlore phase of Nd2Zr2O7 (Nd2Hf2O7). The boundaries of the phase regions and the unit cell parameters are determined. A continuous series of solid solutions based on the ordered pyrochlore (Py) phase of Nd2Zr2O7 (Nd2Hf2O7) at the studied temperature is derived. The unit cell parameters of the ordered pyrochlore (Py) phase vary from a = 1.0633 nm for the two-phase composition (Py + M), 47.5 mol% ZrO2 – 47.5 mol% HfO2 – 5 mol% Nd2O3) to a = 1.0639 nm for the boundary composition of the solid solution (37.5 mol% ZrO2 – 37.5 mol% HfO2 – 30 mol% Nd2O3) and then up to a = 1.0648 nm for the two-phase (Py + A) composition (30 mol% ZrO2 – 30 mol% HfO2 – 40 mol% Nd2O3) which located along the Nd2O3 – (45 mol% ZrO2 – 55 mol% HfO2) constant ratio line. The studied isothermal section is characterized by the formation of two three-phase (Py + F + M and F + T + M) and six two-phase (A + Py, Py + M, Py + F, F + M, T + M, F + T) regions. In the ZrO2–HfO2–Nd2O3 ternary system, no new phases are detected at the temperatures studied.

Materials development using powder diffraction techniques and the Powder Diffraction File

Materials development using powder diffraction techniques and the Powder Diffraction File

Synchrotron powder diffraction data for some smectite clay mineral standards

Synchrotron powder diffraction data is presented for a series of relatively phase-pure smectite clay mineral standards obtained from the Clay Minerals Society. Rietveld refinement using a model for turbostratic disorder was performed to estimate the lattice parameters and mineral impurities in the smectite standards. Bragg reflection lists and raw data have been provided for inclusion in the Powder Diffraction File.

Preparation and photothermal effect of Chitosan-Alginate-Molybdenum diselenide nanocomposite scaffolds for cancer therapy

Transition metal dichalcogenides (TMDs) have gained significant attention for biological and biomedical applications due to their biocompatible properties and photothermal effects. In the current study, TMD nanosheets were fabricated with poly(ethylene glycol)-block-poly(propylene glycol)-block-poly(ethylene glycol) (PPP) triblock copolymer using the liquid exfoliation method. This study prepared TMD nanosheets of PPP-molybdenum sulfide (PPP-MoS2), PPP-tungsten disulfide (PPP-WS2), PPP-molybdenum diselenide (PPP-MoSe2), and PPP-tungsten diselenide (PPP-WS2). The synthesized PPP-TMD nanosheets were characterized using DLS, FT-IR, XRD, SEM, TEM, XPS, and photothermal studies. The DLS results indicated that the nanosheets were 165.1 ± 2.2 to 217.7 ± 2.8 nm and had a zeta potential of −40.9 ± 0.6 to −43.3 ± 0.4 mV and a polydispersity index (PDI) of 0.2. The FT-IR results showed that the fabricated nanosheets contained polymeric substances, and the UV results confirmed that each PPP-TMD had surface plasmon resonance peaks. The XRD patterns of the nanosheets were consistent with those of the International Centre for Diffraction Data. The SEM and TEM results determined that the PPD-TMD sheets were 150 ± 20 nm wide and were single-layer nanosheets with selective area diffraction patterns. The photothermal effects of the PPP-MoSe2 nanosheets at a 30 µg/mL concentration were evaluated at 808 nm with a 1 W cm−2 current. PPP-MoSe2 exhibited the strongest photothermal effect at > 55 °C for 5 min of laser exposure. In addition, the cytotoxicity effects of PPP-MoSe2 were measured with breast cancer cells (MDA-MB-231) with a 5 min laser treatment. At a 30 µg/mL concentration, PPP-MoSe2 inhibited cancer cells by up to 95 %. Further, alginate-chitosan-PPP-MoSe2 composites were developed and evaluated for their photothermal effect. We believe that PPP-MoSe2 will be an excellent material in cancer therapy.

Sintesis dan Karakterisasi Fe₂TiO₅ dari Besi Oksida dan Titanium Dioksida dengan Metode Planetary Ball-Mill

The method of solid hydrogen storage through integration in metal hydride compounds is a new, promising method. This research has succeeded in synthesizing and characterizing the metal hydride alloy Fe-Ti system through a planetary ball-mill process. Based on the XRF analysis, it was found that the composition of Fe oxide content reached 56.22% while Ti oxide reached 43.78%. The FTIR study showed absorption at wavenumbers of 900 cm-1 and 500 cm-1. Both are typical absorptions for Ti-O and Fe-O groups, suggesting that the synthesized sample was successful. It can be seen from the XRD data that some of the diffractogram peaks of the resulting Fe-Ti compound match the peaks of the Fe2TiO5 and TiO2 compounds obtained from the Powder Diffraction File (PDF) database number 00-003-0374. After the refinement was performed, information was obtained that the synthesis of Fe-Ti alloy material using the planetary ball mill technique produced Fe2TiO5.

FFT pattern recognition of crystal HRTEM image with deep learning

Rapid analysis and processing of large quantities of data obtained from in-situ transmission electron microscope (TEM) experiments can save researchers from the burdensome manual analysis work. The method mentioned in this paper combines deep learning and computer vision technology to realize the rapid automatic processing of end-to-end crystal high-resolution transmission electron microscope (HRTEM) images, which has great potential in assisting TEM image analysis. For the fine-grained result, the HRTEM image is divided into multiple patches by sliding window, and 2D fast Fourier transform (FFT) is performed, and then all FFT images are inputted into the designed LCA-Unet to extract bright spots. LCA-Unet combines local contrast and attention mechanism on the basis of U-net. Even if the bright spots in FFT images are weak, the proposed neural network can extract bright spots effectively. Using computer vision and the information of bright spots above mentioned, the automatic FFT pattern recognition is completed by three steps. First step is to calculate the precise coordinates of the bright spots, the lattice spacings and the inter-plane angles in each patch. Second step is to match the lattice spacing and the angles with the powder diffraction file (PDF) to determine the material phase of each patch. Third step is to merge the patches with same phase. Taking the HRTEM image of zirconium and its oxide nanoparticles as an example, the results obtained by the proposed method are basically consistent with manual identification. Thus the approach could be used to automatically and effectively find the phase region of interest. It takes about 3 s to process a 4 K × 4 K HRTEM image on a modern desktop computer with NVIDIA GPU.

The Occurrence of Platinum (Pt) and Skaergaardite (Pd Cu) in the Hutti Underground Gold Mines, Eastern Dharwar Craton, Karnataka, India

Abstract The novelty of this study consists, use of the Powder X-Ray Diffraction (PXRD) technique facility at CSIR-NGRI to report the occurrence of platinum and skaergaardite (Pd Cu) in the Hutti underground gold mines. This study utilized a quartz-bearing sample from the Hutti underground gold mines. One of the split samples were analyzed by PXRD. In this study, quartz samples are found to be associated with sulphides composed of pyrite, chalcopyrite, and arseno-pyrite with intense chemical alterations. The mineral phase of skaergaardite shows a strong intensity at 2θ 43.5° and confirmed with database of International Centre for Diffraction Data Powder Diffraction File – ICDD-2021-PDF4+ PDF00-057-0606 and native platinum, syn (Pt) Pt 0.0999 Sn 0.001 matched with PDF 04-001-3300. Further research work is planned on this interesting mineral association with primary gold ore in Hutti underground gold mine.

Powder X-ray structural analysis and bandgap measurements for (CaxSr2−x)MnWO6 (x = 0.25, 0.5, 0.75, 1.5, 1.75)

The structure, powder diffraction patterns and bandgap measurements of a series of manganese- and tungsten-containing alkaline-earth double perovskites (CaxSr2−x)MnWO6 (x = 0.25, 0.5, 0.75, 1.5, 1.75) have been investigated. Powder X-ray diffraction patterns of this series of compounds measured at room temperature have been submitted to be included in the Powder Diffraction File (PDF). These compounds crystallize in monoclinic space group P21/n (No.14). From (Ca1.75 Sr0.25)MnWO6 to (Ca0.25Sr1.75)MnWO6, lattice parameters a range from 5.6729(2) Å to 5.6774(4) Å, b from 5.5160(2) Å to 5.6638(4) Å, c from 7.8741(3) Å to 8.0051(4) Å, V from 240.39(2) Å3 to 257.410(12) Å3, and Z = 2. These compounds are pseudo-tetragonal. They all consist of distorted MnO6 and WO6 octahedra with rotational mismatch angles and tilt angles with respect to each other. For (CaxSr2−x)MnWO6, as x increases, the mismatch angles for MnO6 octahedra increase from 7.96 (6)° to 13.12(8)° and from 9.28(7)° to 14.87(9)° for WO6 octahedra. Correspondingly, the tilt angles range from 11.60(15)° to 14.20(3)° for MnO6, and from 13.34(2)° to 16.35(3)° for WO6. Bandgap measurements suggest that these compounds to be direct-allowed semiconductors with bandgaps ranging from 1.5 to 2.5 eV, indicating that members of (CaxSr2−x)MnWO6 are potential photocatalysts and photovoltaic materials that absorb visible light of the solar spectrum.

Ultra-fast and effective ultrasonic synthesis of potassium borate: Santite

Abstract In this study, a potassium borate compound of santite is synthesized at 60°C, 70°C, 80°C, and 90°C reaction temperature for 2.5, 5, 10, and 15 min reaction time by using eight different raw material combinations of K2CO3, KNO3, NaOH, H3BO3, B2O3, Na2B4O9·5H2O, and Na2B4O9·10H2O. According to the X-ray diffraction analysis synthesized potassium borate compound is identified as “santite (KB5O8·4H2O)” with powder diffraction file no. 01-072-1688. Raman spectroscopy results showed that the synthesized compound consists of typical boron mineral bands, and the spectra obtained were in mutual agreement with potassium borate, according to the literature. Scanning electron microscopic morphologies showed that obtained santite has different particle shapes as the raw material combination changed and the particle sizes are found between 305 nm and 2.03 µm. Overall reaction yields are found between 76.11% and 99.26%, even such lower reaction times with respect to the literature.

Synthesis and Photoluminescence Properties of White Emitting Alkaline Earth Chalcogenide Phosphors doped with Sn for Solid State Lighting

Sn2+ doped white emitting alkaline-earth chalcogenide CaS and SrS phosphors were synthesized by carbo-thermal reduction method. In this method special requirement such as H2S gas flow is not required as a source of sulphur and is comparatively easy method to prepare sulfides. The crystalline phase, morphology, and photoluminescence properties were characterized by x-ray diffraction (XRD), scanning electron microscope (SEM), and fluorescence spectrophotometer, respectively. Phosphors exhibit broad band excitation which has excellent spread over nUV as well as blue region of visible light i.e. 440–480 nm. Emission is in the form of characteristic broad band of Sn2+ covering nUV and almost entire regions of visible spectrum i.e. 400–650 nm. The XRD pattern of prepared phosphor well matches with International Center for Diffraction Data. Synthesized phosphor particles are of different sizes, with smooth surfaces, from less than 1 micron to few microns. The chromaticity coordinates of synthesized phosphors have been calculated from its corresponding emission spectra monitored at their excitation wavelengths. They observed to falls in white region of CIE diagram. These points are close to standard white point D65, corresponding to daylight with correlated color temperature (CCT) 6500 °K, indicating better color purity of the synthesized phosphor and they are promising material for a color converter using blue LED as the primary light (pumping) source in phosphor converted white LED (pc wLED) for solid state lighting.

A comparative study of ultrasonic-assisted methods to synthesise spinel (CoAl2O4) nanoparticles

In this study, a spinel form of cobalt aluminate (CoAl2O4) was successfully synthesized using different experimental procedures assisted by ultrasonics. The effects of ultrasonic treatment with co-precipitation and hydrothermal experimental methods were compared with traditional techniques. The results indicated that enhanced chromatic features resulted from the experimental procedures modified by ultrasonic treatment. In chromatic analyses, the lowest b* value of −47.19 was observed in the sample synthesized by the ultrasonic-assisted co-precipitation method. This synthesized phase was identified as “Spinel” with the chemical formula of CoAl2O4 according to Powder Diffraction File number (PDF no.) 01-0820-2251 from XRD analyses. The optimum samples were determined to be UC-8 and UH-9 for the modified methods. For these samples the particle sizes were measured between 62 and 83 nm, whereas crystallite sizes were estimated to be in the range from 33 to 43 nm. The thermal analyses results proved the stability of the sample structure up to 1000 °C.