Preparation and Property of High Entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 Perovskite Ceramics

doi:10.15541/jim20200500

Abstract

Abstract:

High entropy ceramic is a kind of ceramic developed based on the high entropy alloy in recent years. The appearance of high entropy ceramics provides a new concept and route for developing non-metallic materials with excellent properties. In present work, a series of high-entropy ceramics with a molar ratio of A site—(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ were successfully synthesized by solid state reaction. The effects of sintering temperature on phase, microstructure and electric properties were investigated. Results show that the high-entropy ceramics sintered at current temperatures are of cubic perovskite structure, and exhibit excellent insulation, with low leakage current density of J value around 10^-8-10^-6 A/cm². Although the grain size increases with the increase of sintering temperature, the correlation between microstructure and dielectric properties of (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ ceramics is not significant. The dielectric constant reaches its maximum value at 1350 ℃, with the value of 230 at the frequency of 100 Hz. Meanwhile, this high-entropy ceramic has relaxation behavior, and the relaxation peak of the permittivity moves towards high temperature with the increase of frequency.

Key words: high-entropy ceramics, perovskite, dielectric property

CLC Number:

TQ174

ZHANG Xiaoyan, LIU Xinyue, YAN Jinhua, GU Yaohang, QI Xiwei. Preparation and Property of High Entropy (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ Perovskite Ceramics[J]. Journal of Inorganic Materials, 2021, 36(4): 379-385.

Figures/Tables 8

Fig. 1 XRD patterns of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2) TiO3 ceramic sintered at different temperatures

Fig. 2 HRTEM image of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2) TiO3 ceramic sintered at 1350 ℃

Fig. 3 SEM images of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at different temperatures (a) 1250 ℃; (b) 1300 ℃; (c) 1350 ℃; (d)1400 ℃; (e) 1450 ℃; (f) 1500 ℃

Fig. 4 Variation of density and relative density of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at different temperatures

Fig. 5 (a) Ti2p and (b) O1s XPS spectra of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic

Fig. 6 Frequency dependences of dielectric constant εr (a) and dielectric loss tanδ (b) of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic

Fig. 7 Temperature dependence of dielectric constant and dielectric loss of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at 1350 ℃

Fig. 8 Leakage current density of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramics sintered at different temperatures (a) J-E curves; (b) lnJ-lnE curves

References 38

[1]	YEH J W, CHEN S K, LIN S J, et al. Nanostructured high-entropy alloys with multiple principal elements: novel alloy design concepts and outcomes. Advanced Engineering Materials, 2004,6(5):299-303.
[2]	CANTOR B, CHANG I T H, KNIGHT P, et al. Microstructural development in equiatomic multicomponent alloys. Materials Science Engineering A, 2004, 375-377(1):213-218.
[3]	RANGANATHAN. Alloyed pleasures: multimetallic cocktails. Current Science, 2003,85(5):1404-1406.
[4]	王晓鹏, 孔凡涛. 高熵合金及其他高熵材料研究新进展. 航空材料学报, 2019,39(6):1-19.
[5]	ZHOU Y J, ZHANG Y, WANG Y L, et al. Solid solution alloys of AlCoCrFeNiTi_x with excellent room-temperature mechanical properties. Applied Physics Letters, 2007,90(18):181904-1-3. DOI URL
[6]	ZHOU W, FU L M, LIU P, et al. Deformation stimulated precipitation of a single-phase CoCrFeMnNi high entropy alloy. Intermetallics, 2017,85:90-97.
[7]	SZKLARZ Z, LEKKI J, BOBROWSKI P, et al. The effect of SiC nanoparticles addition on the electrochemical response of mechanically alloyed CoCrFeMnNi high entropy alloy. Materials Chemistry and Physics, 2018,215:385-392.
[8]	王睿鑫, 唐宇, 李永彦, 等. NbZrTiTa高熵合金的高温氧化行为. 稀有金属材料与工程, 2020,49(7):2417-2424.
[9]	MISHRA K, SAHAY RAJESH P P, ROHIT R S. Alloying, magnetic and corrosion behavior of AlCrFeMnNiTi high entropy alloy. Journal of Materials Science, 2019,54(5):4433-4443.
[10]	陈克丕, 李泽民, 马金旭, 等. 高熵陶瓷材料研究进展与展望. 陶瓷学报, 2020,41(2):157-163.
[11]	顾俊峰, 邹冀, 张帆, 等. 高熵陶瓷材料研究进展. 中国材料进展, 2019,38(9):855-865.
[12]	CHEN H, XIANG H M, DAI F Z, et al. High porosity and low thermal conductivity high entropy (Zr_0.2Hf_0.2Ti_0.2Nb_0.2Ta_0.2)C. Journal of Materials Science & Technology, 2019,35(8):1700-1705.
[13]	GILD J, BRAUN J, KAUFMANN K, et al. A high-entropy silicide: (Mo_0.2Nb_0.2Ta_0.2Ti_0.2W_0.2)Si₂. Journal of Materiomics, 2019,5(3):337-343.
[14]	QIN Y, LIU J X, LI F, et al. A high entropy silicide by reactive spark plasma sintering. Journal of Advanced Ceramics, 2019,8(1):148-152.
[15]	LIU J X, SHEN X Q, WU Y, et al. Mechanical properties of hot-pressed high-entropy diboride-based ceramics. Journal of Advanced Ceramics, 2020,9(4):503-510.
[16]	ROST C M, SACHET E, BORMAN T, et al. Entropy-stabilized oxides. Nature Communications, 2015,6:8485. URL PMID
[17]	SARKAR A, DJENADIC R, WANG D, et al. Rare earth and transition metal based entropy stabilised perovskite type oxides. Journal of the European Ceramic Society, 2018,38(5):2318-2327.
[18]	CHEN K P, PEI X T, TANG L, et al. A five-component entropy-stabilized fluorite oxide. Journal of the European Ceramic Society, 2018,38(11):4161-4164.
[19]	DABROWA J, STYGAR M, MIKUŁA A, et al. Synthesis and microstructure of the (Co, Cr, Fe, Mn, Ni)₃O₄ high entropy oxide characterized by spinel structure. Materials Letters, 2018,216:32-36.
[20]	JIANG S C, HU T, GILD J, et al. A new class of high-entropy perovskite oxides. Scripta Materialia, 2018,142:116-120.
[21]	DONG Y, REN K, LU Y H, et al. High-entropy environmental barrier coating for the ceramic matrix composites. Journal of the European Ceramic Society, 2019,39(7):2574-2579.
[22]	LI F, ZHOU L, LIU J X, et al. High-entropy pyrochlores with low thermal conductivity for thermal barrier coating materials. Journal of Advanced Ceramics, 2019,8(4):576-582.
[23]	ZHANG M, ZHANG X, DAS S, et al. High remanent polarization and temperature-insensitive ferroelectric remanent polarization in BiFeO₃-based lead-free perovskite. Journal of Materials Chemistry C, 2019,7(34):10551-10560.
[24]	ZHANG M, ZHANG X Y, QI X W, et al. Enhanced ferroelectric, magnetic and magnetoelectric properties of multiferroic BiFeO₃-BaTiO₃-LaFeO₃ ceramics. Ceramics International, 2018,44(17):21269-21276.
[25]	DONG G X, MA S W, DU J, et al. Dielectric properties and energy storage density in ZnO-doped Ba_0.3Sr_0.7TiO₃ ceramics. Ceramics International, 2009,35(5):2069-2075.
[26]	KREUER K D. Proton-conducting oxides. Annual Review of Materials Research, 2003,33(1):333-359.
[27]	WRIGHTON M S, MORSE D L, ELLIS A B, et al. Photoassisted electrolysis of water by ultraviolet irradiation of an antimony doped stannic oxide electrode. ChemInform, 1976,7(13):44-48.
[28]	JI L, MCDANIEL M D, WANG S J, et al. A silicon-based photocathode for water reduction with an epitaxial SrTiO₃ protection layer and a nanostructured catalyst. Nature Nanotechnology, 2015,10(1):84-90.
[29]	BIESUZ M, FU S, DONG J, et al. High entropy Sr((Zr_0.94Y_0.06)_0.2Sn_0.2Ti_0.2Hf_0.2Mn_0.2)O_3-x perovskite synthesis by reactive spark plasma sintering. Journal of Asian Ceramic Societies, 2019,7(2):127-132.
[30]	ZHOU S Y, PU Y P, ZHANG Q W, et al. Microstructure and dielectric properties of high entropy Ba(Zr_0.2Ti_0.2Sn_0.2Hf_0.2Me_0.2)O₃ perovskite oxides. Ceramics International, 2020,46(6):7430-7437.
[31]	BÉRARDAN D, FRANGER S, MEENA A K, et al. Room temperature lithium superionic conductivity in high entropy oxides. Journal of Materials Chemistry A, 2016,4(24):9536-9541.
[32]	ZHANG Y, YANG X, LIAW P K. Alloy design and properties optimization of high-entropy alloys. JOM, 2012,64(7):830-838.
[33]	SHANNON R D. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides . Acta Crystallographica Section A, Foundations of Crystallography, 1976,A32(5):751-767.
[34]	PAN W G, CAO M H, HAO H, et al. Defect engineering toward the structures and dielectric behaviors of (Nb, Zn) co-doped SrTiO₃ ceramics. Journal of the European Ceramic Society, 2020,40(1):49-55.
[35]	MERINO N A, BARBERO B P, ELOY P, et al. La_1-xCa_xCoO₃ perovskite-type oxides: identification of the surface oxygen species by XPS. Applied Surface Science, 2006,253(3):1489-1493.
[36]	OSENCIAT N, BÉRARDAN D, DRAGOE D, et al. Charge compensation mechanisms in Li-substituted high-entropy oxides and influence on Li superionic conductivity. Journal of the American Ceramic Society, 2019,102(10):6156-6162.
[37]	WU J G, WANG J. Ferroelectric and impedance behavior of La- and Ti-codoped BiFeO₃ thin films. Journal of the American Ceramic Society, 2010,93(9):2795-2803.
[38]	BAI Y L, ZHAO H, CHEN J, et al. Strong magnetoelectric coupling effect of BiFeO₃/Bi₅Ti₃FeO₁₅ bilayer composite films. Ceramics International, 2016,42(8):10304-10309.

Preparation and Property of High Entropy (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ Perovskite Ceramics

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