journal article·2021-11

Comparative study of phase structure, dielectric properties and electrocaloric effect in novel high-entropy ceramics

Wei Liu, Feng Li, Guohua Chen, Guohui Li, Hongwei Shi, Li Li, Youmin Guo, Jiwei Zhai, Chunchang Wang

Journal of Materials Science· Volume 56· Issue 33
Publisher page

Abstract

Unique structure and performance in prominent high-entropy ceramics (HECs) have attracted enormous attentions recently. In this work, we have successfully synthesized pure-phase (Bi1/6Na1/6Sr1/6Ba1/6Pb1/6Ca1/6)TiO3 (BNSBPC) and (Bi1/6La1/6Na1/6K1/6Sr1/6Ba1/6)TiO3 (BLNKSB) HECs by conventional solid-state method. Rietveld refinement results show that BNSBPC composition possesses tetragonal phase (P4mm) while the BLNKSB one exhibits cubic phase (Pm $$\overline{3}$$ m). Dielectric characterization reveals distinct relaxation behaviors between BNSBPC and BLNKSB compositions. Relaxor-like nature in BNSBPC and Debye medium in BLNKSB one are verified by dielectric, ferroelectric and Raman spectra characterizations. Maximal electrocaloric effect (ECE, ΔTmax) reaches 0.63 K with relatively narrow temperature span (ΔTspan) of ~ 20 K at 60 kV cm−1 for BNSBPC ceramic, while the BLNKSB one possesses superior temperature stability (ΔTspan = 100 K) with ΔTmax = 0.14 K. Room-temperature ECE is also obtained by home-made adiabatic calorimeter, which indicates a positive ECE for both compositions. Finally, phase structure, dielectric properties and ECE in two high-entropy compositions are comparatively discussed to explore structure–ECE relationships in HECs. The superior thermal stability of ECE in BLNKSB samples provides a broad prospect for designing solid-state refrigeration.
Source: openaire · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Ferroelectric and Piezoelectric Materials · Thermal Expansion and Ionic Conductivity · Magnetic and transport properties of perovskites and related materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (55)

Show source-provided references
1. Ma RJ, Zhang ZY, Tong KW, Huber D, Kornbluh R, Ju YS, Pei QB (2017) Highly efficient electrocaloric cooling with electrostatic actuation. Science 357(6356):1130–113410.1126/science.aan5980 ↗
2. Valant M (2012) Electrocaloric materials for future solid-state refrigeration technologies. Prog Mater Sci 57(6):980–100910.1016/j.pmatsci.2012.02.001 ↗
3. Mischenko AS, Zhang Q, Scott JF, Whatmore RW, Mathur ND (2006) Giant electrocaloric effect in thin-film PbZr0.95Ti0.05O3. Science 311(5765):1270–127110.1126/science.1123811 ↗
4. Hagberg J, Uusimaki A, Jantunen H (2008) Electrocaloric characteristics in reactive sintered 0.87Pb(Mg1/3Nb2/3)O3-0.13PbTiO3. Appl Phys Lett 92(13):13290910.1063/1.2905296 ↗
5. Lu B, Jian XD, Lin XW, Yao YB, Tao T, Liang B, Luo HS, Lu SG (2020) Enhanced electrocaloric effect in single crystals via direct measurement 0.73Pb(Mg1/3Nb2/3)O3-0.27PbTiO3. Curr Comput-Aided Drug Des 10(6):451
6. Jian XD, Lu B, Li DD, Yao Y-B, Tao T, Liang B, Guo JH, Zeng Y-J, Chen JL, Lu SG (2018) Direct measurement of large electrocaloric effect in Ba(ZrxTi1–x)O3 Ceramics. ACS Appl Mater Interfaces 10(5):4801–480710.1021/acsami.7b15933 ↗
7. Li JN, Zhang DW, Qin SQ, Li TY, Wu M, Wang D, Bai Y, Lou XJ (2016) Large room-temperature electrocaloric effect in lead-free BaHfxTi1-xO3 ceramics under low electric field. Acta Mater 115:58–6710.1016/j.actamat.2016.05.044 ↗
8. Luo ZD, Zhang DW, Liu Y, Zhou D, Yao YG, Liu CQ, Dkhil B, Ren XB, Lou XJ (2014) Enhanced electrocaloric effect in lead-free BaTi1-xSnxO3 ceramics near room temperature. Appl Phys Lett 105(10):10290410.1063/1.4895615 ↗
9. Bai Y, Han X, Ding K, Qiao LJ (2013) Combined effects of diffuse phase transition and microstructure on the electrocaloric effect Ba1-xSrxTiO3 in ceramics. Appl Phys Lett 103(16):16290210.1063/1.4825266 ↗
10. Han F, Bai Y, Qiao LJ, Guo D (2016) A systematic modification of the large electrocaloric effect within a broad temperature range in rare-earth doped BaTiO3 ceramics. J Mater Chem C 4(9):1842–184910.1039/C5TC04209G ↗
11. Weyland F, Eisele T, Steiner S, Fromling T, Rossetti GA, Rodel J, Novak N (2018) Long term stability of electrocaloric response in barium zirconate titanate. J Eur Ceram Soc 38(2):551–55610.1016/j.jeurceramsoc.2017.09.018 ↗
12. Hanani Z, Merselmiz S, Danine A, Stein N, Mezzane D, Mb A, Lahcini M, Gagou Y, Spreitzer M, Vengust D, Kutnjak Z, El Marssi M, Luk’yanchuk IA, Gouné M (2020) Enhanced dielectric and electrocaloric properties in lead-free rod-like BCZT ceramics. J Adv Ceram 9(2):210–21910.1007/s40145-020-0361-1 ↗
13. Li JT, Bai Y, Qin SQ, Fu J, Zuo RZ, Qiao LJ (2016) Direct and indirect characterization of electrocaloric effect in (Na, K)NbO3 based lead-free ceramics. Appl Phys Lett 109(16):16290210.1063/1.4965707 ↗
14. Yang JL, Zhao Y, Lou XJ, Wu JG, Hao XH (2020) Synergistically optimizing electrocaloric effects and temperature span in KNN-based ceramics utilizing a relaxor multiphase boundary. J Mater Chem C 8(12):4030–403910.1039/C9TC06443E ↗
15. Wang XJ, Wu JG, Dkhil B, Xu BX, Wang XP, Dong GH, Yang G, Lou XJ (2017) Enhanced electrocaloric effect near polymorphic phase boundary in lead-free potassium sodium niobate ceramics. Appl Phys Lett 110(6):06390410.1063/1.4976026 ↗
16. Tao H, Yang JL, Lv X, Hao XH, Wu JG (2019) Electrocaloric behavior and piezoelectric effect in relaxor NaNbO3-based ceramics. J Am Ceram Soc 102(5):2578–258610.1111/jace.16074 ↗
17. Yu Y, Gao F, Weyland F, Du HL, Jin L, Hou L, Yang ZT, Novak N, Qu SB (2019) Significantly enhanced room temperature electrocaloric response with superior thermal stability in sodium niobate-based bulk ceramics. J Mater Chem A 7(19):11665–1167210.1039/C9TA00713J ↗
18. Turki O, Slimani A, Seveyrat L, Sebald G, Perrin V, Sassi Z, Khemakhem H, Lebrun L (2016) Structural, dielectric, ferroelectric, and electrocaloric properties of 2% Gd2O3 doping (Na0.5Bi0.5)(0.94)Ba0.06TiO3 ceramics. J Appl Phys 120(5):05410210.1063/1.4960141 ↗
19. Weyland F, Acosta M, Koruza J, Breckner P, Rodel J, Novak N (2016) Criticality: concept to enhance the piezoelectric and electrocaloric properties of ferroelectrics. Adv Func Mater 26(40):7326–733310.1002/adfm.201602368 ↗
20. Li F, Li J, Zhai J, Shen B, Li S, Zhou M, Zhao K, Zeng H (2018) Influence of structural evolution on electrocaloric effect in Bi0.5Na0.5TiO3-SrTiO3 ferroelectric ceramics. J Appl Phys 124(16):16410810.1063/1.5050826 ↗
21. Miracle DB, Senkov ON (2017) A critical review of high entropy alloys and related concepts. Acta Mater 122:448–51110.1016/j.actamat.2016.08.081 ↗
22. Oses C, Toher C, Curtarolo S (2020) High-entropy ceramics. Nat Rev Mater 5(4):295–30910.1038/s41578-019-0170-8 ↗
23. Djenadic R, Sarkar A, Clemens O, Loho C, Botros M, Chakravadhanula VSK, Kubel C, Bhattacharya SS, Gandhif AS, Hahn H (2017) Multicomponent equiatomic rare earth oxides. Mater Res Lett 5(2):102–10910.1080/21663831.2016.1220433 ↗
24. Rost CM, Sachet E, Borman T, Moballegh A, Dickey EC, Hou D, Jones JL, Curtarolo S, Maria JP (2015) Entropy-stabilized oxides. Nat Commun 6:848510.1038/ncomms9485 ↗
25. Dabrowa J, Stygar M, Mikula A, Knapik A, Mroczka K, Tejchman W, Danielewski M, Martin M (2018) Synthesis and microstructure of the (Co, Cr, Fe, Mn, Ni)3O4 high entropy oxide characterized by spinel structure. Mater Lett 216:32–3610.1016/j.matlet.2017.12.148 ↗
26. Chen K, Pei X, Tang L, Cheng H, Li Z, Li C, Zhang X, An L (2018) A five-component entropy-stabilized fluorite oxide. J Eur Ceram Soc 38(11):4161–416410.1016/j.jeurceramsoc.2018.04.063 ↗
27. Ge PZ, Tang XG, Liu QX, Jiang YP, Li WH, Luo J (2018) Energy storage properties and electrocaloric effect of Ba0.65Sr0.35TiO3 ceramics near room temperature. J Mater Sci-Mater Electron 29(2):1075–108110.1007/s10854-017-8008-x ↗
28. Bérardan D, Franger S, Dragoe D, Meena AK, Dragoe N (2016) Colossal dielectric constant in high entropy oxides. Physica Status Solidi (RRL) Rapid Res Lett 10(4):328–33310.1002/pssr.201600043 ↗
29. Bérardan D, Franger S, Meena AK, Dragoe N (2016) Room temperature lithium superionic conductivity in high entropy oxides. J Mat Chem A 4(24):9536–954110.1039/C6TA03249D ↗
30. Chen H, Fu J, Zhang P, Peng H, Abney CW, Jie K, Liu X, Chi M, Dai S (2018) Entropy-stabilized metal oxide solid solutions as CO oxidation catalysts with high-temperature stability. J Mater Chem A 6(24):11129–1113310.1039/C8TA01772G ↗
31. Zhai S, Rojas J, Ahlborg N, Lim K, Toney MF, Jin H, Chueh WC, Majumdar A (2018) The use of poly-cation oxides to lower the temperature of two-step thermochemical water splitting. Energy Environ Sci 11(8):2172–217810.1039/C8EE00050F ↗
32. Pu Y, Zhang Q, Li R, Chen M, Du X, Zhou S (2019) Dielectric properties and electrocaloric effect of high-entropy (Na0.2Bi0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic. Appl Phys Lett 115:22390110.1063/1.5126652 ↗
33. Du Q, Yan JH, Zhang XY, Li JS, Liu XY, Zhang JR, Qi XW (2020) Phase evolution and dielectric properties of Ba(Ti1/6Sn1/6Zr1/6Hf1/6Nb1/6Ga1/6)O3 high-entropy perovskite ceramics. J Mater Sci-Mater Electron 31(10):7760–776510.1007/s10854-020-03313-x ↗
34. Xiang HM, Xing Y, Dai FZ, Wang HJ, Su L, Miao L, Zhang GJ, Wang YG, Qi XW, Yao L, Wang HL, Zhao B, Li JQ, Zhou YC (2021) High-entropy ceramics: Present status, challenges, and a look forward. J Adv Ceram 10(3):385–44110.1007/s40145-021-0477-y ↗
35. Li F, Chen GR, Liu X, Zhai JW, Shen B, Zeng HR, Li SD, Li P, Yang K, Yan HX (2017) Phase-composition and temperature dependence of electrocaloric effect in lead-free Bi0.5Na0.5TiO3-BaTiO3-(Sr0.7Bi0.2□0.1)TiO3 ceramics. J Eur Ceram Soc 37(15):4732–474010.1016/j.jeurceramsoc.2017.06.033 ↗
36. Li F, Li J, Zhai J, Shen B, Li S, Zeng H (2019) Phase formation and electrocaloric effect in nonstoichiometric 0.94Bi0.5+xNa0.5TiO3-0.06BaTiO3 ceramics. J Mater Sci-Mater Electron 30(4):3465–347110.1007/s10854-018-00622-0 ↗
37. Jiang S, Hu T, Gild J, Zhou N, Nie J, Qin M, Harrington T, Vecchio K, Luo J (2018) A new class of high-entropy perovskite oxides. Scripta Mater 142:116–12010.1016/j.scriptamat.2017.08.040 ↗
38. Goldschmidt VM (1926) Die Gesetze der Krystallochemie. Naturwissenschaften 14(21):477–48510.1007/BF01507527 ↗
39. Shvartsman VV, Kleemann W, Dec J, Xu ZK, Lu SG (2006) Diffuse phase transition in BaTi1-xSnxO3 ceramics: An intermediate state between ferroelectric and relaxor behavior. J Appl Phys 99(12):12411110.1063/1.2207828 ↗
40. Bokov AA, Ye ZG (2006) Recent progress in relaxor ferroelectrics with perovskite structure. J Mater Sci 41(1):31–5210.1007/s10853-005-5915-7 ↗
41. Sharma P, Kumar P, Kundu RS, Juneja JK, Ahlawat N, Punia R (2015) Structural and dielectric properties of substituted barium titanate ceramics for capacitor applications. Ceram Int 41(10):13425–1343210.1016/j.ceramint.2015.07.131 ↗
42. Sharma P, Berwal N, Ahlawat N, Maan AS, Punia R (2019) Study of structural, dielectric, ferroelectric and magnetic properties of vanadium doped BCT ceramics. Ceram Int 45(16):20368–2037810.1016/j.ceramint.2019.07.013 ↗
43. Xiong W, Zhang H, Cao S, Gao F, Svec P, Dusza J, Reece MJ, Yan H (2021) Low-loss high entropy relaxor-like ferroelectrics with A-site disorder. J Eur Ceram Soc 41(4):2979–298510.1016/j.jeurceramsoc.2020.11.030 ↗
44. Viehland D, Jang SJ, Cross LE, Wuttig M (1990) Freezing of the polarization fluctuations in lead magnesium niobate relaxors. J Appl Phys 68(6):2916–292110.1063/1.346425 ↗
45. Cheng ZY, Zhang LY, Yao X (1996) Investigation of glassy behavior of lead magnesium niobate relaxors. J Appl Phys 79(11):8615–861910.1063/1.362685 ↗
46. Barick BK, Mishra KK, Arora AK, Choudhary RNP, Pradhan DK (2011) Impedance and Raman spectroscopic studies of (Na0.5Bi0.5)TiO3. J Phys D-Appl Phys 44(35):8615–861910.1088/0022-3727/44/35/355402 ↗
47. Jiang XJ, Wang BY, Luo LH, Li WP, Zhou J, Chen HB (2014) Electrical properties of (1–x)(Bi0.5Na0.5)TiO3-xKNbO3 lead-free ceramics. J Solid State Chem 213:72–7810.1016/j.jssc.2014.01.022 ↗
48. Schutz D, Deluca M, Krauss W, Feteira A, Jackson T, Reichmann K (2012) Lone-pair-induced covalency as the cause of temperature- and field-induced instabilities in bismuth sodium titanate. Adv Func Mater 22(11):2285–229410.1002/adfm.201102758 ↗
49. Haumont R, Gemeiner P, Dkhil B, Kiat JM, Bulou A (2006) Polar and chemical states at a nanometer scale in a PbSc1/2Nb1/2O3-PbTiO3 system investigated by Raman spectroscopy. Phys Rev B 73(10):10410610.1103/PhysRevB.73.104106 ↗
50. Li J, Li J, Qin S, Su X, Qiao L, Wang Y, Lookman T, Bai Y (2019) Effects of long- and short-range ferroelectric order on the electrocaloric effect in relaxor ferroelectric ceramics. Phys Rev Appl 11(4):04403210.1103/PhysRevApplied.11.044032 ↗
51. Wang JF, Yang TQ, Chen SC, Li G, Zhang QF, Yao X (2013) Nonadiabatic direct measurement electrocaloric effect in lead-free Ba, Ca(Zr, Ti)O3 ceramics. J Alloy Compd 550:561–56310.1016/j.jallcom.2012.10.144 ↗
52. Zhang L, Zhao C, Zheng T, Wu J (2021) Large electrocaloric response with superior temperature stability in NaNbO3-based relaxor ferroelectrics benefiting from the crossover region. J Mater Chem A 9(5):2806–281410.1039/D0TA11423E ↗
53. Li F, Li K, Long MS, Wang CC, Chen GH, Zhai JW (2021) Ferroelectric-relaxor crossover induce large electrocaloric effect with ultrawide temperature span in NaNbO3-based lead-free ceramics. Appl Phys Lett 118(4):04390210.1063/5.0038506 ↗
54. Lu SG, Li DD, Lin XW, Jian XD, Zhao XB, Yao YB, Tao T, Liang B (2020) Influence of electric field on the phenomenological coefficient and electrocaloric strength in ferroelectrics. Acta Physica Sinica 69(12):12770110.7498/aps.69.20200296 ↗
55. Lu SG, Lin XW, Li J, Li DD, Yao YB, Tao T, Liang B (2021) Enhanced electrocaloric strengths at room temperature in (SrxBa1-x)(Sn0.05Ti0.95)O3 (lead-free ceramics. J Alloys Compd 871:15951910.1016/j.jallcom.2021.159519 ↗