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
PDF (7.3 MB)
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Open Access

Dielectric ultracapacitors based on columnar nano-grained ferroelectric oxide films with gradient phases along the growth direction

Chuanqi Song1Feifan Zheng1Yuan Zhang2Hongbo Cheng1( )Long Teng1,3Kun Wang4Hanfei Zhu1Chao Liu1Li Wang1Zhengyan Liang1Jun Ouyang1,3( )
Institute of Advanced Energy Materials and Chemistry, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Key Laboratory of Key Film Materials & Application for Equipment (Hunan Province), School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
China Tobacco Shandong Industrial Co., Ltd., Jinan 250104, China
Show Author Information

Graphical Abstract

Abstract

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.

References

[1]

Burn I, Smyth DM. Energy storage in ceramic dielectrics. J Mater Sci 1972, 7: 339–343.

[2]

Kim J, Saremi S, Acharya M, et al. Ultrahigh capacitive energy density in ion-bombarded relaxor ferroelectric films. Science 2020, 369: 81–84.

[3]

Yang LT, Kong X, Li F, et al. Perovskite lead-free dielectrics for energy storage applications. Prog Mater Sci 2019, 102: 72–108.

[4]

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.

[5]

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.

[6]

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.

[7]

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.

[8]

Zhao PY, Wang HX, Wu LW, et al. High-performance relaxor ferroelectric materials for energy storage applications. Adv Energy Mater 2019, 9: 1803048.

[9]

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.

[10]

Pan H, Li F, Liu Y, et al. Ultrahigh-energy density lead-free dielectric films via polymorphic nanodomain design. Science 2019, 365: 578–582.

[11]

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.

[12]

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.

[13]

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.

[14]

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.

[15]

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.

[16]

Wang JJ, Su YJ, Wang B, et al. Strain engineering of dischargeable energy density of ferroelectric thin-film capacitors. Nano Energy 2020, 72: 104665.

[17]

Peng W, Zorn JA, Mun J, et al. Constructing polymorphic nanodomains in BaTiO3 films via epitaxial symmetry engineering. Adv Funct Mater 2020, 30: 1910569.

[18]

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.

[19]

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.

[20]

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.

[21]

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.

[22]

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.

[23]

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.

[24]

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.

[25]

Dong L, Stone DS, Lakes RS. Enhanced dielectric and piezoelectric properties of xBaZrO3–(1− x)BaTiO3 ceramics. J Appl Phys 2012, 111: 084107.

[26]

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.

[27]

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.

[28]

Roytburd AL, Ouyang J, Artemev A. Polydomain structures in ferroelectric and ferroelastic epitaxial films. J Phys: Condens Matter 2017, 29: 163001.

[29]

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.

[30]

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.

[31]

Zhang W, Gao YQ, Kang LM, et al. Space-charge dominated epitaxial BaTiO3 heterostructures. Acta Mater 2015, 85: 207–215.

[32]

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.

[33]

Choi KJ, Biegalski M, Li YL, et al. Enhancement of ferroelectricity in strained BaTiO3 thin films. Science 2004, 306: 1005–1009.

[34]

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.

[35]

Uchino K, Nomura S. Critical exponents of the dielectric constants in diffused-phase-transition crystals. Ferroelectr Lett Sect 1982, 44: 55–61.

[36]

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.

Journal of Advanced Ceramics
Pages 1072-1079
Cite this article:
Song C, Zheng F, Zhang Y, et al. Dielectric ultracapacitors based on columnar nano-grained ferroelectric oxide films with gradient phases along the growth direction. Journal of Advanced Ceramics, 2024, 13(7): 1072-1079. https://doi.org/10.26599/JAC.2024.9220920

1198

Views

226

Downloads

2

Crossref

2

Web of Science

2

Scopus

0

CSCD

Altmetrics

Received: 09 April 2024
Revised: 08 May 2024
Accepted: 30 May 2024
Published: 30 July 2024
© The Author(s) 2024.

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/).

Return