AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
Powered by AMiner. Clicking this button will take you away from SciOpen.
Home Journal of Advanced Ceramics Article
PDF (3.8 MB)
Cite
EndNote(RIS) BibTeX
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article | Open Access

New class of high-entropy pseudobrookite titanate with excellent thermal stability, low thermal expansion coefficient, and low thermal conductivity

Jinyu WU, Xiaohui MA, Xiaoxia HU, Liwen YAN, Feng HOU, Jiachen LIU, Anran GUO( )
School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin University, Tianjin 300072, China
Show Author Information

Graphical Abstract

Abstract

As a type of titanate, the pseudobrookite (MTi2O5/M2TiO5) exhibits a low thermal expansion coefficient and thermal conductivity, as well as excellent dielectric and solar spectrum absorption properties. However, the pseudobrookite is unstable and prone to decomposing below 1200 ℃, which limits the practical application of the pseudobrookite. In this paper, the high-entropy pseudobrookite ceramic is synthesized for the first time. The pure high-entropy (Mg,Co,Ni,Zn)Ti2O5 with the pseudobrookite structure and the biphasic high-entropy ceramic composed of the high-entropy pseudobrookite (Cr,Mn,Fe,Al,Ga)2TiO5 and the high-entropy spinel (Cr,Mn,Fe,Al,Ga,Ti)3O4 are successfully prepared by the in-situ solid-phase reaction method. The comparison between the theoretical crystal structure of the pseudobrookite and the aberration-corrected scanning transmission electron microscopy (AC-STEM) images of high-entropy (Mg,Co,Ni,Zn)Ti2O5 shows that the metal ions (M and Ti ions) are disorderly distributed at the A site and the B site in high-entropy (Mg,Co,Ni,Zn)Ti2O5, leading to an unprecedentedly high configurational entropy of high-entropy (Mg,Co,Ni,Zn)Ti2O5. The bulk high-entropy (Mg,Co,Ni,Zn)Ti2O5 ceramics exhibit a low thermal expansion coefficient of 6.35×10−6 K−1 in the temperature range of 25–1400 ℃ and thermal conductivity of 1.840 W·m−1·K−1 at room temperature, as well as the excellent thermal stability at 200, 600, and 1400 ℃. Owing to these outstanding properties, high-entropy (Mg,Co,Ni,Zn)Ti2O5 is expected to be the promising candidate for high-temperature thermal insulation. This work has further extended the family of different crystal structures of high-entropy ceramics reported to date.

Keywords

high-entropy pseudobrookite(Mg,Co,Ni,Zn)Ti2O5(Cr,Mn,Fe,Al,Ga)2TiO5high conformational entropythermal expansion coefficientthermal conductivity

References

[1]
Cantor B, Chang ITH, Knight P, et al. Microstructural development in equiatomic multicomponent alloys. Mater Sci Eng A 2004, 375–377: 213-218.
Crossref Google Scholar
[2]
Yeh JW, Chen SK, Lin SJ, et al. Nanostructured high-entropy alloys with multiple principal elements: Novel alloy design concepts and outcomes. Adv Eng Mater 2004, 6: 299-303.
Crossref Google Scholar
[3]
Rost CM, Sachet E, Borman T, et al. Entropy-stabilized oxides. Nat Commun 2015, 6: 8485.
Crossref Google Scholar
[4]
Oses C, Toher C, Curtarolo S. High-entropy ceramics. Nat Rev Mater 2020, 5: 295-309.
Crossref Google Scholar
[5]
Xiang HM, Xing Y, Dai FZ, et al. High-entropy ceramics: Present status, challenges, and a look forward. J Adv Ceram 2021, 10: 385–441.
Crossref Google Scholar
[6]
Zhang WM, Zhao B, Xiang HM, et al. One-step synthesis and electromagnetic absorption properties of high entropy rare earth hexaborides (HE REB6) and high entropy rare earth hexaborides/borates (HE REB6/HE REBO3) composite powders. J Adv Ceram 2021, 10: 62-77.
Crossref Google Scholar
[7]
Li F, Zhou L, Liu JX, et al. High-entropy pyrochlores with low thermal conductivity for thermal barrier coating materials. J Adv Ceram 2019, 8: 576-582.
Crossref Google Scholar
[8]
Jiang SC, Hu T, Gild J, et al. A new class of high-entropy perovskite oxides. Scripta Mater 2018, 142: 116-120.
Crossref Google Scholar
[9]
Liu SY, Zhang SX, Liu SY, et al. Stability and mechanical properties of single-phase quinary high-entropy metal carbides: First-principles theory and thermodynamics. J Eur Ceram Soc 2022, 42: 3089-3098.
Crossref Google Scholar
[10]
Strauss F, Lin J, Duffiet M, et al. High-entropy polyanionic lithium superionic conductors. ACS Mater Lett 2022, 4: 418-423.
Crossref Google Scholar
[11]
Xue Y, Zhao XQ, An YL, et al. High-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Ce2O7: A potential thermal barrier material with improved thermo-physical properties. J Adv Ceram 2022, 11: 615-628.
Google Scholar
[12]
Wright AJ, Luo J. A step forward from high-entropy ceramics to compositionally complex ceramics: A new perspective. J Mater Sci 2020, 55: 9812-9827.
Crossref Google Scholar
[13]
Qin MD, Vega H, Zhang DW, et al. 21-Component compositionally complex ceramics: Discovery of ultrahigh-entropy weberite and fergusonite phases and a pyrochlore–weberite transition. J Adv Ceram 2022, 11: 641-655.
Crossref Google Scholar
[14]
Qin Y, Liu JX, Li F, et al. A high entropy silicide by reactive spark plasma sintering. J Adv Ceram 2019, 8: 148-152.
Crossref Google Scholar
[15]
Gild J, Braun J, Kaufmann K, et al. A high-entropy silicide: (Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2. J Materiomics 2019, 5: 337-343.
Google Scholar
[16]
Liu JX, Shen XQ, Wu Y, et al. Mechanical properties of hot-pressed high-entropy diboride-based ceramics. J Adv Ceram 2020, 9: 503-510.
Crossref Google Scholar
[17]
Gild J, Zhang YY, Harrington T, et al. High-entropy metal diborides: A new class of high-entropy materials and a new type of ultrahigh temperature ceramics. Sci Rep 2016, 6: 37946.
Crossref Google Scholar
[18]
Chen H, Xiang HM, Dai FZ, et al. Porous high entropy (Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)B2: A novel strategy towards making ultrahigh temperature ceramics thermal insulating. J Mater Sci Technol 2019, 35: 2404-2408.
Crossref Google Scholar
[19]
Xirouchakis DM. Pseudobrookite-group oxide solutions and basaltic melts. Lithos 2007, 95: 1-9.
Crossref Google Scholar
[20]
Yang HX, Hazen RM. Crystal chemistry of cation order–disorder in pseudobrookite-type MgTi2O5. J Solid State Chem 1998, 138: 238-244.
Crossref Google Scholar
[21]
Xirouchakis D, Smirnov A, Woody K, et al. Thermodynamics and stability of pseudobrookite-type MgTi2O5 (karrooite). Am Mineral 2002, 87: 658-667.
Crossref Google Scholar
[22]
Wu JY, Xu XJ, Xiong YL, et al. Preparation and structure control of a scalelike MoSi2–borosilicate glass coating with improved contact damage and thermal shock resistance. Ceram Int 2020, 46: 7178-7186.
Crossref Google Scholar
[23]
Suzuki Y, Shinoda Y. Magnesium dititanate (MgTi2O5) with pseudobrookite structure: A review. Sci Technol Adv Mater 2011, 12: 034301.
Crossref Google Scholar
[24]
Kornaus K, Rutkowski P, Lach R, et al. Effect of microstructure on thermal and mechanical properties of solid solutions Al2TiO5–MgTi2O5. J Eur Ceram Soc 2021, 41: 1498-1505.
Crossref Google Scholar
[25]
Nakagoshi Y, Suzuki Y. Pseudobrookite-type MgTi2O5 water purification filter with controlled particle morphology. J Asian Ceram Soc 2015, 3: 334-338.
Crossref Google Scholar
[26]
Regue M, Ahmet IY, Bassi PS, et al. Zn-doped Fe2TiO5 pseudobrookite-based photoanodes grown by aerosol-assisted chemical vapor deposition. ACS Appl Energ Mater 2020, 3: 12066-12077.
Crossref Google Scholar
[27]
Platt NJ, Kaye KM, Limburn GJ, et al. Order of magnitude increase in photocatalytic rate for hierarchically porous anatase thin films synthesized from zinc titanate coatings. Dalton Trans 2017, 46: 1975-1985.
Crossref Google Scholar
[28]
Xiong K, Wang KZ, Chen L, et al. Heterostructured ZnFe2O4/Fe2TiO5/TiO2 composite nanotube arrays with an improved photocatalysis degradation efficiency under simulated sunlight irradiation. Nano-Micro Lett 2018, 10: 17.
Google Scholar
[29]
Ehsan MA, Naeem R, McKee V, et al. MgTi2O5 thin films from single molecular precursor for photoelectrochemical water splitting. Sol Energ Mat Sol C 2017, 161: 328-337.
Crossref Google Scholar
[30]
Zhang N, Zhang KF, Zhou W, et al. Pure phase orthorhombic MgTi2O5 photocatalyst for H2 production. RSC Adv 2015, 5: 106151-106155.
Crossref Google Scholar
[31]
Chen C, Giovannelli F, Duclère JR, et al. Thermoelectric properties of Fe2(Ti1−xNbx)O5 pseudobrookite ceramics with low thermal conductivity. J Eur Ceram Soc 2017, 37: 4681-4685.
Crossref Google Scholar
[32]
Djuric ZZ, Aleksic OS, Nikolic MV, et al. Structural and electrical properties of sintered Fe2O3/TiO2 nanopowder mixtures. Ceram Int 2014, 40: 15131-15141.
Crossref Google Scholar
[33]
Nikolic MV, Vasiljevic ZZ, Lukovic MD, et al. Humidity sensing properties of nanocrystalline pseudobrookite (Fe2TiO5) based thick films. Sensor Actuat B-Chem 2018, 277: 654-664.
Crossref Google Scholar
[34]
Sarwanto Y, Adi WA. Modification of pseudobrookite Fe2−xMnxTiO5 with solid state reaction method using a mechanical milling. IOP Conf Ser Mater Sci Eng 2017, 202: 012073.
Crossref Google Scholar
[35]
Perry NH, Stevanovic V, Lim LY, et al. Discovery of a ternary pseudobrookite phase in the earth-abundant Ti–Zn–O system. Dalton Trans 2016, 45: 1572-1581.
Crossref Google Scholar
[36]
Cerro S, Gargori C, Llusar M, et al. Orthorhombic (Fe2TiO5)–monoclinic (Cr2TiO5) solid solution series: Synthesis by gel routes, coloring and NIR reflectivity evaluation. Ceram Int 2018, 44: 13349-13359.
Crossref Google Scholar
[37]
Llusar M, García E, García MT, et al. Synthesis, stability and coloring properties of yellow–orange pigments based on Ni-doped karrooite (Ni,Mg)Ti2O5. J Eur Ceram Soc 2015, 35: 357-376.
Crossref Google Scholar
[38]
Llusar M, Bermejo T, Primo JE, et al. Karrooite green pigments doped with Co and Zn: Synthesis, color properties and stability in ceramic glazes. Ceram Int 2017, 43: 9133-9144.
Crossref Google Scholar
[39]
Matteucci F, Cruciani G, Dondi M, et al. Crystal structure, optical properties and colouring performance of karrooite MgTi2O5 ceramic pigments. J Solid State Chem 2007, 180: 3196-3210.
Crossref Google Scholar
[40]
Dondi M, Lyubenova TS, Carda JB, et al. M-doped Al2TiO5 (M = Cr, Mn, Co) solid solutions and their use as ceramic pigments. J Am Ceram Soc 2009, 92: 1972-1980.
Crossref Google Scholar
[41]
Kornaus K, Lach R, Szumera M, et al. Synthesis of aluminium titanate by means of isostructural heterogeneous nucleation. J Eur Ceram Soc 2019, 39: 2535-2544.
Crossref Google Scholar
[42]
Jantzen T, Hack K, Yazhenskikh E, et al. Addition of TiO2 and Ti2O3 to the Al2O3–FeO–Fe2O3–MgO system. Calphad 2018, 62: 187-200.
Crossref Google Scholar
[43]
Jaromin AL, Edwards DD. Subsolidus phase relationships in the Ga2O3–Al2O3–TiO2 system. J Am Ceram Soc 2005, 88: 2573-2577.
Crossref Google Scholar
[44]
Korim T. Effect of Mg2+- and Fe3+-ions on formation mechanism of aluminium titanate. Ceram Int 2009, 35: 1671-1675.
Crossref Google Scholar
[45]
Anderson KP, Giri AK, Vinci RP, et al. Single crystal growth of CoTi2O5 by solid state reaction synthesis. J Am Ceram Soc 2019, 102: 5050-5062.
Crossref Google Scholar
[46]
Deng YF, Zhang HL, Hong QM, et al. Titanium-based mixed oxides from a series of titanium(IV) citrate complexes. J Solid State Chem 2007, 180: 3152-3159.
Crossref Google Scholar
[47]
Liou YC, Yang SL. Calcium-doped MgTiO3–MgTi2O5 ceramics prepared using a reaction-sintering process. Mater Sci Eng B 2007, 142: 116-120.
Crossref Google Scholar
[48]
Giordano L, Viviani M, Bottino C, et al. Microstructure and thermal expansion of Al2TiO5–MgTi2O5 solid solutions obtained by reaction sintering. J Eur Ceram Soc 2002, 22: 1811-1822.
Crossref Google Scholar
[49]
Minouei H, Kheradmandfard M, Rizi MS, et al. Formation mechanism of high-entropy spinel thin film and its mechanical and magnetic properties: Linking high-entropy alloy to high-entropy ceramic. Appl Surf Sci 2022, 576: 151719.
Crossref Google Scholar
[50]
Stygar M, Dąbrowa J, Moździerz M, et al. Formation and properties of high entropy oxides in Co–Cr–Fe–Mg–Mn–Ni–O system: Novel (Cr,Fe,Mg,Mn,Ni)3O4 and (Co,Cr,Fe,Mg,Mn)3O4 high entropy spinels. J Eur Ceram Soc 2020, 40: 1644-1650.
Crossref Google Scholar
[51]
Parida T, Karati A, Guruvidyathri K, et al. Novel rare-earth and transition metal-based entropy stabilized oxides with spinel structure. Scripta Mater 2020, 178: 513-517.
Crossref Google Scholar
[52]
Marik S, Singh D, Gonano B, et al. Enhanced magnetic frustration in a new high entropy diamond lattice spinel oxide. Scripta Mater 2020, 186: 366-369.
Crossref Google Scholar
[53]
Fracchia M, Manzoli M, Anselmi-Tamburini U, et al. A new eight-cation inverse high entropy spinel with large configurational entropy in both tetrahedral and octahedral sites: Synthesis and cation distribution by X-ray absorption spectroscopy. Scripta Mater 2020, 188: 26-31.
Crossref Google Scholar
[54]
Lin CC, Chang CW, Kaun CC, et al. Stepwise evolution of photocatalytic spinel-structured (Co,Cr,Fe,Mn,Ni)3O4 high entropy oxides from first-principles calculations to machine learning. Crystals 2021, 11: 1035.
Crossref Google Scholar
[55]
Mittal VK, Chandramohan P, Bera S, et al. Cation distribution in NixMg1−xFe2O4 studied by XPS and Mössbauer spectroscopy. Solid State Commun 2006, 137: 6-10.
Crossref Google Scholar
[56]
Kim JG, Pugmire DL, Battaglia D, et al. Analysis of the NiCo2O4 spinel surface with Auger and X-ray photoelectron spectroscopy. Appl Surf Sci 2000, 165: 70-84.
Crossref Google Scholar
[57]
Nesbitt HW, Legrand D, Bancroft GM. Interpretation of Ni2p XPS spectra of Ni conductors and Ni insulators. Phys Chem Miner 2000, 27: 357-366.
Crossref Google Scholar
[58]
Sakamoto K, Hayashi F, Sato K, et al. XPS spectral analysis for a multiple oxide comprising NiO, TiO2, and NiTiO3. Appl Surf Sci 2020, 526: 146729.
Crossref Google Scholar
[59]
Biesinger MC, Payne BP, Grosvenor AP, et al. Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni. Appl Surf Sci 2011, 257: 2717-2730.
Crossref Google Scholar
[60]
Tang K, Wang CA, Xu XL, et al. A study on powder X-ray diffraction of Ti3SiC2. Mater Lett 2002, 55: 50-54.
Crossref Google Scholar
[61]
Shi WT, Sun DL, Chen JQ, et al. Hydrothermal synthesis of aluminum-doped zincophosphate large single crystal with different morphology. J Cryst Growth 2019, 507: 189-195.
Crossref Google Scholar
[62]
Inoue M, Hirasawa I. The relationship between crystal morphology and XRD peak intensity on CaSO4·2H2O. J Cryst Growth 2013, 380: 169-175.
Crossref Google Scholar
[63]
Matos CRS, Xavier MJ, Barreto LS, et al. Principal component analysis of X-ray diffraction patterns to yield morphological classification of brucite particles. Anal Chem 2007, 79: 2091-2095.
Crossref Google Scholar
[64]
Heidarpour A, Aghamohammadi H, Jamshidi R, et al. The shape evolution of TiCx prepared by mechanical alloying of Ti–Al–C system after HF treatment. Ceram Int 2019, 45: 4653-4660.
Crossref Google Scholar
[65]
Sun ZQ, Zhou YC, Wang JY, et al. Thermal properties and thermal shock resistance of γ-Y2Si2O7. J Am Ceram Soc 2008, 91: 2623-2629.
Crossref Google Scholar
[66]
Cao XQ, Vassen R, Stoever D. Ceramic materials for thermal barrier coatings. J Eur Ceram Soc 2004, 24: 1-10.
Crossref Google Scholar
[67]
Zhao M, Ren XR, Yang J, et al. Thermo-mechanical properties of ThO2-doped Y2O3 stabilized ZrO2 for thermal barrier coatings. Ceram Int 2016, 42: 501-508.
Crossref Google Scholar
[68]
Zhao ZF, Xiang HM, Dai FZ, et al. (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7: A novel high-entropy ceramic with low thermal conductivity and sluggish grain growth rate. J Mater Sci Technol 2019, 35: 2647-2651.
Google Scholar
[69]
Zhu JT, Meng XY, Zhang P, et al. Dual-phase rare-earth-zirconate high-entropy ceramics with glass-like thermal conductivity. J Eur Ceram Soc 2021, 41: 2861-2869.
Crossref Google Scholar
[70]
Zhao ZF, Chen H, Xiang HM, et al. High-entropy (Y0.2Nd0.2Sm0.2Eu0.2Er0.2)AlO3: A promising thermal/ environmental barrier material for oxide/oxide composites. J Mater Sci Technol 2020, 47: 45-51.
Crossref Google Scholar
[71]
Zhao ZF, Xiang HM, Chen H, et al. High-entropy (Nd0.2Sm0.2Eu0.2Y0.2Yb0.2)4Al2O9 with good high temperature stability, low thermal conductivity, and anisotropic thermal expansivity. J Adv Ceram 2020, 9: 595-605.
Google Scholar
[72]
Chen H, Zhao ZF, Xiang HM, et al. High entropy (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12: A novel high temperature stable thermal barrier material. J Mater Sci Technol 2020, 48: 57-62.
Google Scholar
[73]
Qin MD, Yan QZ, Liu Y, et al. A new class of high-entropy M3B4 borides. J Adv Ceram 2021, 10: 166-172.
Crossref Google Scholar
[74]
Zhang Y, Sun SK, Guo WM, et al. Optimal preparation of high-entropy boride–silicon carbide ceramics. J Adv Ceram 2021, 10: 173-180.
Crossref Google Scholar
[75]
Wang MC, Bu FX, Zhou CJ, et al. Bonding performance and mechanism of a heat-resistant composite precursor adhesive (RT–1000 ℃) for TC4 titanium alloy. J Micromech Mol Phys 2020, 5: 2050016.
Crossref Google Scholar
Journal of Advanced Ceramics
Volume 11 Issue 10,
October 2022
Pages 1654-1670
DOI: 10.1007/s40145-022-0638-7
Cite this article:
WU J, MA X, HU X, et al. New class of high-entropy pseudobrookite titanate with excellent thermal stability, low thermal expansion coefficient, and low thermal conductivity. Journal of Advanced Ceramics, 2022, 11(10): 1654-1670. https://doi.org/10.1007/s40145-022-0638-7

1335

Views

197

Downloads

12

Crossref

12

Web of Science

13

Scopus

0

CSCD

Altmetrics
Received: 31 May 2022
Revised: 31 July 2022
Accepted: 09 August 2022
Published: 11 October 2022
© The Author(s) 2022.

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
Return