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Journal of Advanced Ceramics 2024, 13(2): 198-206 https://doi.org/10.26599/JAC.2024.9220841
Research Article | Open Access | Issue | Published: 08 March 2024

Simultaneously achieving high energy density and responsivity in submicron BaTiO3 film capacitors integrated on Si

Show Author's Information Jun Ouyang1,2,3( ),  Yinxiu Xue1,  Chuanqi Song1,  Meiling Yuan3,4,  Kun Wang3,5,  Yuyao Zhao3,  Hongbo Cheng1,3,  Hanfei Zhu1,3,  Chao Liu1
Institute of Advanced Energy Materials and Chemistry, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
Key Laboratory of Key Film Materials & Application for Equipment, School of Material Sciences and Engineering, Xiangtan University, Xiangtan 411105, China
School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Academic Affairs Office, Civil Aviation University of China, Tianjin 300300, China
China Tobacco Shandong Industrial Co., Ltd., Jinan 250014, China
Keywords:
energy density, energy storage, BaTiO3, Si, responsivity, dielectric capacitor
Cite this article:
Ouyang J, Xue Y, Song C, et al. Simultaneously achieving high energy density and responsivity in submicron BaTiO3 film capacitors integrated on Si. Journal of Advanced Ceramics, 2024, 13(2): 198-206. https://doi.org/10.26599/JAC.2024.9220841
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Abstract Full text About this article

In the research field of energy storage dielectrics, the “responsivity” parameter, defined as the recyclable/recoverable energy density per unit electric field, has become critically important for a comprehensive evaluation of the energy storage capability of a dielectric. In this work, high recyclable energy density and responsivity, i.e., Wrec = 161.1 J·cm–3 and ξ = 373.8 J·(kV·m2)–1, have been simultaneously achieved in a prototype perovskite dielectric, BaTiO3, which is integrated on Si at 500 ℃ in the form of a submicron thick film. This ferroelectric film features a multi-scale polar structure consisting of ferroelectric grains with different orientations and inner-grain ferroelastic domains. A LaNiO3 buffer layer is used to induce a {001} textured, columnar nanograin microstructure, while an elevated deposition temperature promotes lateral growth of the nanograins (in-plane diameter increases from ~10–20 nm at lower temperatures to ~30 nm). These preferably oriented and periodically regulated nanograins have resulted in a small remnant polarization and a delayed polarization saturation in the film’s P–E behavior, leading to a high recyclable energy density. Meanwhile, an improved polarizability/dielectric constant of the BaTiO3 film has produced a much larger maximum polarization than those deposited at lower temperatures at the same electric field, leading to a record-breaking responsivity for this simple perovskite.


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About this article

Simultaneously achieving high energy density and responsivity in submicron BaTiO3 film capacitors integrated on Si

Show Author's information Jun Ouyang1,2,3( ), Yinxiu Xue1, Chuanqi Song1, Meiling Yuan3,4, Kun Wang3,5, Yuyao Zhao3, Hongbo Cheng1,3, Hanfei Zhu1,3, Chao Liu1
Institute of Advanced Energy Materials and Chemistry, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
Key Laboratory of Key Film Materials & Application for Equipment, School of Material Sciences and Engineering, Xiangtan University, Xiangtan 411105, China
School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Academic Affairs Office, Civil Aviation University of China, Tianjin 300300, China
China Tobacco Shandong Industrial Co., Ltd., Jinan 250014, China

Abstract

In the research field of energy storage dielectrics, the “responsivity” parameter, defined as the recyclable/recoverable energy density per unit electric field, has become critically important for a comprehensive evaluation of the energy storage capability of a dielectric. In this work, high recyclable energy density and responsivity, i.e., Wrec = 161.1 J·cm–3 and ξ = 373.8 J·(kV·m2)–1, have been simultaneously achieved in a prototype perovskite dielectric, BaTiO3, which is integrated on Si at 500 ℃ in the form of a submicron thick film. This ferroelectric film features a multi-scale polar structure consisting of ferroelectric grains with different orientations and inner-grain ferroelastic domains. A LaNiO3 buffer layer is used to induce a {001} textured, columnar nanograin microstructure, while an elevated deposition temperature promotes lateral growth of the nanograins (in-plane diameter increases from ~10–20 nm at lower temperatures to ~30 nm). These preferably oriented and periodically regulated nanograins have resulted in a small remnant polarization and a delayed polarization saturation in the film’s P–E behavior, leading to a high recyclable energy density. Meanwhile, an improved polarizability/dielectric constant of the BaTiO3 film has produced a much larger maximum polarization than those deposited at lower temperatures at the same electric field, leading to a record-breaking responsivity for this simple perovskite.

Keywords: energy density, energy storage, BaTiO3, Si, responsivity, dielectric capacitor

References(49)

[1]

Li JL, Li F, Xu Z, et al. Multilayer lead-free ceramic capacitors with ultrahigh energy density and efficiency. Adv Mater 2018, 30: 1802155.
DOI Google Scholar
[2]

Li DX, Zeng XJ, Li ZP, et al. Progress and perspectives in dielectric energy storage ceramics. J Adv Ceram 2021, 10: 675–703.
DOI Google Scholar
[3]

Yao FZ, Yuan QB, Wang Q, et al. Multiscale structural engineering of dielectric ceramics for energy storage applications: From bulk to thin films. Nanoscale 2020, 12: 17165–17184.
DOI Google Scholar
[4]

Palneedi H, Peddigari M, Hwang GT, et al. High-performance dielectric ceramic films for energy storage capacitors: Progress and outlook. Adv Funct Materials 2018, 28: 1803665.
DOI Google Scholar
[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.
DOI Google Scholar
[6]

Liang ZS, Ma CR, Shen LK, et al. Flexible lead-free oxide film capacitors with ultrahigh energy storage performances in extremely wide operating temperature. Nano Energy 2019, 57: 519–527.
DOI Google Scholar
[7]
Peddigari M, Park JH, Han JH, et al. Flexible self-charging, ultrafast, high-power-density ceramic capacitor system. ACS Energy Lett 2021: 1383–1391.
DOI
[8]

Yang LT, Kong X, Li F, et al. Perovskite lead-free dielectrics for energy storage applications. Prog Mater Sci 2019, 102: 72–108.
DOI Google Scholar
[9]

Zhao PY, Wang HX, Wu LW, et al. High-performance relaxor ferroelectric materials for energy storage applications. Adv Energy Mater 2019, 9: 1803048.
DOI Google Scholar
[10]
Huang YL, Zhao CL, Wu B, et al. Multifunctional BaTiO3-based relaxor ferroelectrics toward excellent energy storage performance and electrostrictive strain benefiting from crossover region. ACS Appl Mater Interfaces 2020, 12 : 23885–23895.
DOI
[11]

Tong S, Ma BH, Narayanan M, et al. Lead lanthanum zirconate titanate ceramic thin films for energy storage. ACS Appl Mater Interfaces 2013, 5: 1474–1480.
DOI Google Scholar
[12]

Huang Y, Shu L, Zhang SW, et al. Simultaneously achieved high-energy storage density and efficiency in (K,Na)NbO3-based lead-free ferroelectric films. J Am Ceram Soc 2021, 104: 4119–4130.
DOI Google Scholar
[13]

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.
DOI Google Scholar
[14]

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.
DOI Google Scholar
[15]
Yuan QB, Li G, Yao FZ, et al. Simultaneously achieved temperature-insensitive high energy density and efficiency in domain engineered BaTiO3–Bi(Mg0.5Zr0.5)O3 lead-free relaxor ferroelectrics, Nano Energy 2018, 52 : 203–210.
DOI
[16]

Li Y, Sun NN, Li XW, et al. Multiple electrical response and enhanced energy storage induced by unusual coexistent-phase structure in relaxor ferroelectric ceramics. Acta Mater 2018, 146: 202–210.
DOI Google Scholar
[17]

Sun NN, Li Y, Liu XJ, et al. High energy-storage density under low electric field in lead-free relaxor ferroelectric film based on synergistic effect of multiple polar structures. J Power Sources 2020, 448: 227457.
DOI Google Scholar
[18]

Peng BL, Zhang Q, Li X, et al. Giant electric energy density in epitaxial lead-free thin films with coexistence of ferroelectrics and antiferroelectrics. Adv Elect Materials 2015, 1: 1500052.
DOI Google Scholar
[19]

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.
DOI Google Scholar
[20]

Pan H, Li F, Liu Y, et al. Ultrahigh-energy density lead-free dielectric films via polymorphic nanodomain design. Science 2019, 365: 578–582.
DOI Google Scholar
[21]

Pan H, Lan S, Xu SQ, et al. Ultrahigh energy storage in superparaelectric relaxor ferroelectrics. Science 2021, 374: 100–104.
DOI Google Scholar
[22]

Kim J, Saremi S, Acharya M, et al. Ultrahigh capacitive energy density in ion-bombarded relaxor ferroelectric films. Science 2020, 369: 81–84.
DOI Google Scholar
[23]

Zhang YL, Li WL, Wang ZY, et al. Perovskite Sr1− x (Na0.5Bi0.5) x Ti0.99Mn0.01O3 thin films with defect dipoles for high energy-storage and electrocaloric performance. ACS Appl Mater Interfaces 2019, 11: 37947–37954.
DOI Google Scholar
[24]

Song BJ, Wu SH, Yan H, et al. Fatigue-less relaxor ferroelectric thin films with high energy storage density via defect engineer. J Mater Sci Technol 2021, 77: 178–186.
DOI Google Scholar
[25]

Sun ZX, Ma CR, Liu M, et al. Ultrahigh energy storage performance of lead-free oxide multilayer film capacitors via interface engineering. Adv Mater 2017, 29: 1604427.
DOI Google Scholar
[26]

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.
DOI Google Scholar
[27]

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.
DOI Google Scholar
[28]

McMillen M, Douglas AM, Correia TM, et al. Increasing recoverable energy storage in electroceramic capacitors using “dead-layer” engineering. Appl Phys Lett 2012, 101: 242909.
DOI Google Scholar
[29]

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.
DOI Google Scholar
[30]

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.
DOI Google Scholar
[31]

Peddigari M, Palneedi H, Hwang GT, et al. Boosting the recoverable energy density of lead-free ferroelectric ceramic thick films through artificially induced quasi-relaxor behavior. ACS Appl Mater Interfaces 2018, 10: 20720–20727.
DOI Google Scholar
[32]

Peddigari M, Wang B, Wang R, et al. Giant energy density via mechanically tailored relaxor ferroelectric behavior of PZT thick film. Adv Mater 2023, 35: e2302554.
DOI Google Scholar
[33]

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.
DOI Google Scholar
[34]

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.
DOI Google Scholar
[35]

Yan J, Wang YL, Wang CM, et al. Boosting energy storage performance of low-temperature sputtered CaBi2Nb2O9 thin film capacitors via rapid thermal annealing. J Adv Ceram 2021, 10: 627–635.
DOI Google Scholar
[36]

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.
DOI Google Scholar
[37]

Wang JJ, Su YJ, Wang B, et al. Strain engineering of dischargeable energy density of ferroelectric thin-film capacitors. Nano Energy 2020, 72: 104665.
DOI Google Scholar
[38]

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.
DOI Google Scholar
[39]

Peng W, Zorn JA, Mun J, et al. Constructing polymorphic nanodomains in BaTiO3 films via epitaxial symmetry engineering. Adv Funct Materials 2020, 30: 1910569.
DOI Google Scholar
[40]

Zhu HF, Zhao YY, Ouyang J, et al. Achieving a record-high capacitive energy density on Si with columnar nanograined ferroelectric films. ACS Appl Mater Interfaces 2022, 14: 7805–7813.
DOI Google Scholar
[41]

Li F, Zhai JW, Shen B, et al. Simultaneously high-energy storage density and responsivity in quasi-hysteresis-free Mn-doped Bi0.5Na0.5TiO3–BaTiO3–(Sr0.7Bi0.2□0.1)TiO3 ergodic relaxor ceramics. Mater Res Lett 2018, 6: 345–352.
DOI Google Scholar
[42]
Ouyang J, Teng XM, Yuan ML, et al. Grain engineering of high energy density BaTiO3 thick films integrated on Si. Microstructures 2023: 2023027.
DOI
[43]

Wang YY, Ouyang J, Cheng HB, et al. High performance LaNiO3-buffered, (001)-oriented PZT piezoelectric films integrated on (111) Si. Appl Phys Lett 2022, 121: 182902.
DOI Google Scholar
[44]

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.
DOI Google Scholar
[45]

Scott JF. Ferroelectrics go bananas. J Phys: Condens Matter 2008, 20: 021001.
DOI Google Scholar
[46]

Ederer C, Spaldin NA. Effect of epitaxial strain on the spontaneous polarization of thin film ferroelectrics. Phys Rev Lett 2005, 95: 257601.
DOI Google Scholar
[47]

Liu ML, Zhu HF, Zhang YX, et al. Energy storage characteristics of BiFeO₃/BaTiO₃ Bi-layers integrated on Si. Materials 2016, 9: 935.
DOI Google Scholar
[48]

Choi KJ, Biegalski M, Li YL, et al. Enhancement of ferroelectricity in strained BaTiO3 thin films. Science 2004, 306: 1005–1009.
DOI Google Scholar
[49]

Chu BJ, Zhou X, Ren KL, et al. A dielectric polymer with high electric energy density and fast discharge speed. Science 2006, 313: 334–336.
DOI Google Scholar
Publication history
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Publication history

Received: 25 October 2023
Revised: 02 December 2023
Accepted: 12 December 2023
Published: 08 March 2024
Issue date: February 2024

Copyright

© The Author(s) 2024.

Acknowledgements

Acknowledgements

The authors are deeply grateful for the financial support from the National Natural Science Foundation of China (Grant Nos. 51772175 and 52002192), Natural Science Foundation of Shandong Province (Grant Nos. ZR2022ZD39, ZR2022ME075, ZR2020QE042, ZR2022ME031, and ZR2022QB138), and the Science, Education and Industry Integration Pilot Projects of Qilu University of Technology (Shandong Academy of Sciences) (Grant Nos. 2022GH018 and 2022PY055). Jun Ouyang acknowledges the support from the Jinan City Science and Technology Bureau (Grant No. 2021GXRC055), and the Education Department of Hunan Province/Xiangtan University (Grant No. KZ0807969), as well as the seed funding for top talents at Qilu University of Technology (Shandong Academy of Sciences).

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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/).

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