Discover the SciOpen Platform and Achieve Your Research Goals with Ease.
Search articles, authors, keywords, DOl and etc.
In this work, dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies. These ultracapacitors are based on submicron-thick Ba(Zr0.2Ti0.8)O3 ferroelectric films sputter-deposited on Si at 500 °C. With a composition near a polymorphic phase boundary (PPB), a compressive strain, and a high nucleation rate due to the lowered deposition temperature, these films exhibit a columnar nanograined microstructure with gradient phases along the growth direction. Such a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale, thereby significantly delaying the saturation of the overall electric polarization. Consequently, a pseudolinear, ultraslim polarization (P)–electric field (E) hysteresis loop was obtained, featuring a high maximum applicable electric field (~5.7 MV/cm), low remnant polarization (~5.2 μC/cm2) and high maximum polarization (~92.1 μC/cm2). This P–E loop corresponds to a high recyclable energy density (Wrec ~208 J/cm3) and charge‒discharge efficiency (~88%). An in-depth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal (T) and rhombohedral (R) polymorphs along the growth direction of the film. The T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the surface. These films also exhibited a high Curie temperature of ~460 °C and stable capacitive energy storage up to 200 °C. These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.
Burn I, Smyth DM. Energy storage in ceramic dielectrics. J Mater Sci 1972, 7: 339–343.
Kim J, Saremi S, Acharya M, et al. Ultrahigh capacitive energy density in ion-bombarded relaxor ferroelectric films. Science 2020, 369: 81–84.
Yang LT, Kong X, Li F, et al. Perovskite lead-free dielectrics for energy storage applications. Prog Mater Sci 2019, 102: 72–108.
Ouyang J, Xue YX, Song CQ, et al. Simultaneously achieving high energy density and responsivity in submicron BaTiO3 film capacitors integrated on Si. J Adv Ceram 2024, 13: 198–206.
Yang CH, Lv PP, Qian J, et al. Fatigue-free and bending-endurable flexible Mn-doped Na0.5Bi0.5TiO3–BaTiO3–BiFeO3 film capacitor with an ultrahigh energy storage performance. Adv Energy Mater 2019, 9: 1803949.
Lu ZL, Wang G, Bao WC, et al. Superior energy density through tailored dopant strategies in multilayer ceramic capacitors. Energy Environ Sci 2020, 13: 2938–2948.
Bhattarai MK, Mishra KK, Instan AA, et al. Enhanced energy storage density in Sc3+ substituted Pb(Zr0.53Ti0.47)O3 nanoscale films by pulse laser deposition technique. Appl Surf Sci 2019, 490: 451–459.
Zhao PY, Wang HX, Wu LW, et al. High-performance relaxor ferroelectric materials for energy storage applications. Adv Energy Mater 2019, 9: 1803048.
Pan H, Ma J, Ma J, et al. Giant energy density and high efficiency achieved in bismuth ferrite-based film capacitors via domain engineering. Nat Commun 2018, 9: 1813.
Pan H, Li F, Liu Y, et al. Ultrahigh-energy density lead-free dielectric films via polymorphic nanodomain design. Science 2019, 365: 578–582.
Zhao YY, Ouyang J, Wang K, et al. Achieving an ultra-high capacitive energy density in ferroelectric films consisting of superfine columnar nanograins. Energy Storage Mater 2021, 39: 81–88.
Wang K, Ouyang J, Wuttig M, et al. Superparaelectric (Ba0.95,Sr0.05)(Zr0.2,Ti0.8)O3 ultracapacitors. Adv Energy Mater 2020, 10: 2001778.
Cheng HB, Zhai X, Ouyang J, et al. Achieving a high energy storage density in Ag(Nb,Ta)O3 antiferroelectric films via nanograin engineering. J Adv Ceram 2023, 12: 196–206.
Han GF, Ryu J, Yoon WH, et al. Stress-controlled Pb(Zr0.52Ti0.48)O3 thick films by thermal expansion mismatch between substrate and Pb(Zr0.52Ti0.48)O3 film. J Appl Phys 2011, 110: 124101.
Akedo J, Park JH, Kawakami Y. Piezoelectric thick film fabricated with aerosol deposition and its application to piezoelectric devices. Jpn J Appl Phys 2018, 57: 07LA02.
Wang JJ, Su YJ, Wang B, et al. Strain engineering of dischargeable energy density of ferroelectric thin-film capacitors. Nano Energy 2020, 72: 104665.
Peng W, Zorn JA, Mun J, et al. Constructing polymorphic nanodomains in BaTiO3 films via epitaxial symmetry engineering. Adv Funct Mater 2020, 30: 1910569.
Cheng HB, Ouyang J, Zhang YX, et al. Demonstration of ultra-high recyclable energy densities in domain-engineered ferroelectric films. Nat Commun 2017, 8: 1999.
Zhu HF, Liu ML, Zhang YX, et al. Increasing energy storage capabilities of space-charge dominated ferroelectric thin films using interlayer coupling. Acta Mater 2017, 122: 252–258.
Chen XY, Peng BL, Ding MJ, et al. Giant energy storage density in lead-free dielectric thin films deposited on Si wafers with an artificial dead-layer. Nano Energy 2020, 78: 105390.
Chen HY, Liu L, Yan ZN, et al. Ultrahigh energy storage density in superparaelectric-like Hf0.2Zr0.8O2 electrostatic supercapacitors. Adv Sci 2023, 10: e2300792.
Fan QL, Liu M, Ma CR, et al. Significantly enhanced energy storage density with superior thermal stability by optimizing Ba(Zr0.15Ti0.85)O3/Ba(Zr0.35Ti0.65)O3 multilayer structure. Nano Energy 2018, 51: 539–545.
Chen JY, Tang ZH, Yang B, et al. Ultra-high energy storage performances regulated by depletion region engineering sensitive to the electric field in PNP-type relaxor ferroelectric heterostructural films. J Mater Chem A 2020, 8: 8010–8019.
Ren YH, Cheng HB, Ouyang J, et al. Bimodal polymorphic nanodomains in ferroelectric films for giant energy storage. Energy Storage Mater 2022, 48: 306–313.
Dong L, Stone DS, Lakes RS. Enhanced dielectric and piezoelectric properties of xBaZrO3–(1− x)BaTiO3 ceramics. J Appl Phys 2012, 111: 084107.
Yu Z, Ang C, Guo RY, et al. Piezoelectric and strain properties of Ba(Ti1− x Zr x )O3 ceramics. J Appl Phys 2002, 92: 1489–1493.
Kalyani AK, Senyshyn A, Ranjan R. Polymorphic phase boundaries and enhanced piezoelectric response in extended composition range in the lead free ferroelectric BaTi1– x Zr x O3. J Appl Phys 2013, 114: 014102.
Roytburd AL, Ouyang J, Artemev A. Polydomain structures in ferroelectric and ferroelastic epitaxial films. J Phys: Condens Matter 2017, 29: 163001.
Wakiya N, Azuma T, Shinozaki K, et al. Low-temperature epitaxial growth of conductive LaNiO3 thin films by RF magnetron sputtering. Thin Solid Films 2002, 410: 114–120.
Ren YH, Maity P, Ascienzo D, et al. Second harmonic generation studies of interfacial strain engineering in BaZr0.2Ti0.8O3. Adv Electron Materials 2023, 9: 2300497.
Zhang W, Gao YQ, Kang LM, et al. Space-charge dominated epitaxial BaTiO3 heterostructures. Acta Mater 2015, 85: 207–215.
Wang K, Zhu HF, Ouyang J, et al. Significantly improved energy storage stabilities in nanograined ferroelectric film capacitors with a reduced dielectric nonlinearity. Appl Surf Sci 2022, 581: 152400.
Choi KJ, Biegalski M, Li YL, et al. Enhancement of ferroelectricity in strained BaTiO3 thin films. Science 2004, 306: 1005–1009.
Harrington SA, Zhai JY, Denev S, et al. Thick lead-free ferroelectric films with high Curie temperatures through nanocomposite-induced strain. Nat Nanotechnol 2011, 6: 491–495.
Uchino K, Nomura S. Critical exponents of the dielectric constants in diffused-phase-transition crystals. Ferroelectr Lett Sect 1982, 44: 55–61.
Zhao Z, Buscaglia V, Viviani M, et al. Grain-size effects on the ferroelectric behavior of dense nanocrystalline BaTiO3 ceramics. Phys Rev B 2004, 70: 024107.
1198
Views
226
Downloads
2
Crossref
2
Web of Science
2
Scopus
0
CSCD
Altmetrics
This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).