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Lead scandium tantalate (PbSc0.5Ta0.5O3 (PST)) is one of the most promising ferroelectric materials for electrocaloric (EC) refrigeration because of its large enthalpy change (ΔH) at room temperature (RT), whose properties are determined by the ordering arrangement of two kinds of heterovalent ions at B-sites. This work continuously adjusts the ordering degree (Ω) for PST ceramics on a large scale from 0.51 to 1 via multiple heat treatment processes. For the PST sample with Ω = 1, large ΔH = 1.06 J/g and very large EC adiabatic temperature change ΔTmax = 4.26 K@60 kV/cm are obtained because of the highly ordered arrangement of the Sc3+ and Ta5+ ions. With decreasing Ω, the Curie temperature (TC) gradually shifts from RT to below 0 °C, and the phase transition is diffused. A fairly large ΔTmax = 1.57 K is obtained at a rather low temperature of 0 °C in the ceramic with Ω = 0.51. This work proves that lattice ordering is another efficient route to modify ferroelectric features, and the achieved large ΔTmax in a wide temperature range near/below RT facilitates high-performance cooling devices with a cascade design toward the most urgent market needs.
Greco A, Masselli C. Electrocaloric cooling: A review of the thermodynamic cycles, materials, models, and devices. Magnetochemistry 2020, 6: 67–99.
Wang G, Lu Z, Li Y, et al. Electroceramics for high-energy density capacitors: Current status and future perspectives. Chem Rev 2021, 121: 6124–6172.
Lheritier P, Torelló A, Usui T, et al. Large harvested energy with non-linear pyroelectric modules. Nature 2022, 609: 718–721.
Hanani Z, Merselmiz S, Danine A, et al. Enhanced dielectric and electrocaloric properties in lead-free rod-like BCZT ceramics. J Adv Ceram 2020, 9: 210–219.
Ali F, Abbas A, Wu G, et al. Novel fluorite-structured materials for solid-state refrigeration. Small 2022, 18: 2200133.
Tao H, Yin J, Zhao CL, et al. Large electrocaloric effect under electric field behavior in potassium sodium niobate ceramics with incompletely overlapped phase boundaries. J Mater Chem A 2022, 10: 5262–5272.
Wei XK, Prokhorenko S, Wang BX, et al. Ferroelectric phase-transition frustration near a tricritical composition point. Nat Commun 2021, 12: 5322–5329.
Wang ZJ, Meng YZ, Tang SL, et al. Simultaneous achievement of large electrocaloric effect and ultra-wide operating temperature range in BaTiO3-based lead-free ceramic. J Adv Ceram 2024, 13: 1234–1241.
Marlton FP, Nayak S, Venkateshwarlu S, et al. Broad distribution of local polar states generates large electrothermal properties in Pb-free relaxor ferroelectrics. Chem Mater 2021, 33: 8844–8853.
Huang F, Tian H, Meng XD, et al. Large room temperature electrocaloric effect in KTa1–xNbxO3 single crystal. Phys Status Solidi-R 2019, 13: 1800515.
Patel S, Chauhan A, Vaish R. Multiple caloric effects in (Ba0.865Ca0.135Zr0.1089Ti0.8811Fe0.01)O3 ferroelectric ceramic. Appl Phys Lett 2015, 107: 042902.
Niu X, Jian XD, Chen XY, et al. Enhanced electrocaloric effect at room temperature in Mn2+ doped lead-free (BaSr)TiO3 ceramics via a direct measurement. J Adv Ceram 2021, 10: 482–492.
Hagberg J, Uusimäki A, Jantunen H. Electrocaloric characteristics in reactive sintered 0.87Pb(Mg1∕3Nb2∕3)O3–0.13PbTiO3. Appl Phys Lett 2008, 92: 132909.
Moya X, Stern-Taulats E, Crossley S, et al. Giant electrocaloric strength in single-crystal BaTiO3. Adv Mater 2013, 25: 1360–1365.
Han F, Bai Y, Qiao LJ, et al. A systematic modification of the large electrocaloric effect within a broad temperature range in rare-earth doped BaTiO3 ceramics. J Mater Chem C 2016, 4: 1842–1849.
Vales-Castro P, Faye R, Vellvehi M, et al. Origin of large negative electrocaloric effect in antiferroelectric PbZrO3. Phys Rev B 2021, 103: 054112.
Buixaderas E, Nuzhnyy D, Veljko S, et al. Broad-band dielectric spectroscopy of tetragonal PLZTx/40/60. Phase Transit 2006, 79: 415–426.
Nouchokgwe Y, Lheritier P, Hong CH, et al. Giant electrocaloric materials energy efficiency in highly ordered lead scandium tantalate. Nat Commun 2021, 12: 3298–3304.
Li JJ, Wu HH, Li JT, et al. Room-temperature symmetric giant positive and negative electrocaloric effect in PbMg0.5W0.5O3 antiferroelectric ceramic. Adv Funct Mater 2021, 31: 2101176.
Nair B, Usui T, Crossley S, et al. Large electrocaloric effects in oxide multilayer capacitors over a wide temperature range. Nature 2019, 575: 468–472.
Chu F, Setter N, Tagantsev AK. The spontaneous relaxor-ferroelectric transition of Pb(Sc0.5Ta0.5)O3. J Appl Phys 1993, 74: 5129–5134.
Setter N, Cross LE. The role of B-site cation disorder in diffuse phase transition behavior of perovskite ferroelectrics. J Appl Phys 1980, 51: 4356–4360.
Chu F, Reaney IM, Setter N. Role of defects in the ferroelectric relaxor lead scandium tantalate. J Am Ceram Soc, 1995, 78: 1947–1952.
Yang LH, Li Q. Preparation, dielectric relaxation, and X-ray diffraction at various temperatures of Pb(Sc1/2Ta1/2)O3 ceramics. Aip Adv 2021, 11: 125313.
Merz WJ. Double hysteresis loop of BaTiO3 at the curie point. Phys Rev 1953, 91: 513–517.
Shebanovs L, Sternberg A, Lawless WN, et al. Isomorphous ion substitutions and order–disorder phenomena in highly electrocaloric lead-scandium tantalate solid solutions. Ferroelectrics 1996, 184: 239–242.
Crossley S, Nair B, Whatmore RW, et al. Electrocaloric cooling cycles in lead scandium tantalate with true regeneration via field variation. Phys Rev X 2019, 9: 041002.
Bai Y, Han X, Ding K, et al. Combined effects of diffuse phase transition and microstructure on the electrocaloric effect in Ba1−xSrxTiO3 ceramics. Appl Phys Lett 2013, 103: 162902.
Molin C, Sanlialp M, Shvartsman VV, et al. Effect of dopants on the electrocaloric effect of 0.92Pb(Mg1/3Nb2/3)O3–0.08PbTiO3 ceramics. J Eur Ceram Soc 2015, 35: 2065–2071.
Qian XS, Ye HJ, Zhang YT, et al. Giant electrocaloric response over A broad temperature range in modified BaTiO3 ceramics. Adv Funct Mater 2014, 24: 1300–1305.
Bai Y, Ding K, Zheng GP, et al. The electrocaloric effect around the orthorhombic-tetragonal first-order phase transition in BaTiO3. Aip Adv 2012, 2: 022162.
Li F, Ji XL, Wang XJ, et al. Superior electrocaloric performance enabled by highly robust monomorphic ferrodistortion in NaNbO3-based relaxor. Adv Funct Mater 2025, 35: 2418534.
Luo ZD, Zhang DW, Liu Y, et al. Enhanced electrocaloric effect in lead-free BaTi1−xSnxO3 ceramics near room temperature. Appl Phys Lett 2014, 105: 102904
Li F, Jin L, Xu Z, et al. Electrostrictive effect in ferroelectrics: An alternative approach to improve piezoelectricity. Appl Phys Rev 2014, 1: 011103.
Li JJ, Li JT, Wu HH, et al. Giant electrocaloric effect and ultrahigh refrigeration efficiency in antiferroelectric ceramics by morphotropic phase boundary design. ACS Appl Mater Inter 2020, 12: 45005–45014.
Li JJ, Yin RW, Xiong Z, et al. Manipulating Zr/Ti ratio based on phase diagram for large electrocaloric effects with multiple target operation temperatures in PLZT ceramics. J Adv Ceram 2024, 13: 1422–1431.
Wei SY, Chen X, Dong GZ, et al. Large electrocaloric effect in two-step-SPS processed Pb(Sc0.25In0.25Nb0.25Ta0.25)O3 medium-entropy ceramics. Ceram Int 2022, 48: 15640–15646.
Sun HC, Meng YZ, Han FF, et al. Simultaneously achieved large electrocaloric effect and broad working temperature range in transparent Sm-doped 0.88Pb(Mg1/3Nb2/3)O3–0.12PbTiO3 ceramics at low electric field. Ceram Int 2024, 50: 19237–19244.
Huang Y, Zhao C, Zhong S, et al. Highly tunable multifunctional BaTiO3-based ferroelectrics via site selective doping strategy. Acta Mater 2021, 209: 116792.
Li JN, Zhang DW, Qin SQ, et al. Large room-temperature electrocaloric effect in lead-free BaHfxTi1−xO3 ceramics under low electric field. Acta Mater 2016, 115: 58–67.
Zhao CL, Yang JL, Huang YL, et al. Broad-temperature-span and large electrocaloric effect in lead-free ceramics utilizing successive and metastable phase transitions. J Mater Chem A 2019, 7: 25526–25536.
Hanani Z, Merselmiz S, Mezzane D, et al. Thermally-stable high energy storage performances and large electrocaloric effect over a broad temperature span in lead-free BCZT ceramic. RSC Adv 2020, 10: 30746–30755.
Wei XW, Zhao CL, Zheng T, et al. Understanding the enhanced electrocaloric effect in BaTiO3-based ferroelectrics at critical state. Acta Mater 2022, 227: 117735.
Du FH, Song ZW, Xu YT, et al. Multi-element B-site substituted perovskite ferroelectrics exhibit enhanced electrocaloric effect. Sci China Technol Sc 2023, 66: 1119–1128.
Wang XJ, Tian F, Zhao CL, et al. Giant electrocaloric effect in lead-free Ba0.94Ca0.06Ti1−xSnxO3 ceramics with tunable Curie temperature. Appl Phys Lett 2015, 107: 252905.
Li J, Chang Y, Yang S, et al. Lead-free bilayer thick films with giant electrocaloric effect near room temperature. ACS Appl Mater Inter 2019, 11: 23346–23352.
Liu XQ, Chen TT, Wu YJ, et al. Enhanced electrocaloric effects in spark plasma-sintered Ba0.65Sr0.35TiO3-based ceramics at room temperature. J Am Ceram Soc 2013, 96: 1021–1023.
Lin MM, Luo ZH, Sun HC, et al. Enhanced room-temperature electrocaloric performance by both multiphase coexistence and diffused phase transition in (Ba0.65Sr0.3Ca0.05)(SnxTi1−x)O3 ferroelectric ceramics. J Mater Chem C 2025, 13: 1713–1723.
Meng YZ, Tang SL, Wang ZJ, et al. Significantly enhanced electrocaloric effect by composition modulation in lead-free BaTiO3-based ceramics. J Materiomics 2025, 11: 100903.
Meng YZ, Wang ZJ, Tang SL, et al. Significantly enhanced electrocaloric performance in lead-free BaTiO3 ceramics by introducing high-entropy component. Sustain Mater Technol 2025, 43: 01235.
Li F, Chen GR, Liu X, et al. Phase-composition and temperature dependence of electrocaloric effect in lead-free Bi0.5Na0.5TiO3–BaTiO3–(Sr0.7Bi0.2
Le Goupil F, Baker A, Tonus F, et al. Direct measurement of electrocaloric effect in lead-free (Na0.5Bi0.5)TiO3-based multilayer ceramic capacitors. J Eur Ceram Soc 2019, 39: 3315–3319.
Li JT, Bai Y, Qin SQ, et al. Direct and indirect characterization of electrocaloric effect in (Na,K)NbO3 based lead-free ceramics. Appl Phys Lett 2016, 109: 162902.
Wang XJ, Wu JG, Dkhil B, et al. Enhanced electrocaloric effect near polymorphic phase boundary in lead-free potassium sodium niobate ceramics. Appl Phys Lett 2017, 110: 063904.
Yang JL, Zhao Y, Zhu LP, et al. Enhanced electrocaloric effect of relaxor potassium sodium niobate lead-free ceramic via multilayer structure. Scripta Mater 2021, 193: 97–102.
Zhao Y, Du J, Yang J, et al. Large room-temperature electrocaloric response realized in potassium-sodium niobate by a relaxor enhancement effect and multilayer ceramic construct. ACS Appl Mater Interf 2022, 14: 11626–11635.
Zhang L, Zhao CL, Zheng T, et al. Large electrocaloric response with superior temperature stability in NaNbO3-based relaxor ferroelectrics benefiting from the crossover region. J Mater Chem A 2021, 9: 2806–2814.
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