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Journal of Advanced Ceramics 2023, 12(1): 196-206 https://doi.org/10.26599/JAC.2023.9220678
Research Article | Open Access | Issue | Published: 19 December 2022

Achieving a high energy storage density in Ag(Nb,Ta)O3 antiferroelectric films via nanograin engineering

Show Author's Information Hongbo CHENGa,b,†,  Xiao ZHAIc,†,  Jun OUYANGa( ),  Limei ZHENGc( ),  Nengneng LUOd,  Jinpeng LIUa,  Hanfei ZHUa,  Yingying WANGe,  Lanxia HAOe,  Kun WANGf
Institute of Advanced Energy Materials and Chemistry, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
College of Electronic and Optical Engineering, Nanjing University of Posts and Telecommunications, Nanjing 210023, China
School of Physics, Shandong University, Jinan 250100, China
Guangxi Key Laboratory of Processing for Non-ferrous Metallic and Featured Materials, School of Resources, Environment and Materials; Center on Nanoenergy Research, School of Physical Science and Technology, Guangxi University, Nanning 530004, China
Key Laboratory for Liquid-Solid Structure Evolution and Processing of Materials (Ministry of Education), School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Jinan Cigarette Factory, China Tobacco Shandong Industrial Co., Ltd., Jinan 250104, China

† Hongbo Cheng and Xiao Zhai contributed equally to this work.

Keywords:
energy storage, antiferroelectrics (AFE), AgNbO3, Ag(Nb,Ta)O3, film capacitors, nanograin engineering
Cite this article:
CHENG H, ZHAI X, OUYANG J, et al. Achieving a high energy storage density in Ag(Nb,Ta)O3 antiferroelectric films via nanograin engineering. Journal of Advanced Ceramics, 2023, 12(1): 196-206. https://doi.org/10.26599/JAC.2023.9220678
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Abstract Full text About this article

Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization (Pmax) and a small remnant polarization (Pr), AgNbO3-based antiferroelectrics (AFEs) have attracted extensive research interest for electric energy storage applications. However, a low dielectric breakdown field (Eb) limits an energy density and its further development. In this work, a highly efficient method was proposed to fabricate high-energy-density Ag(Nb,Ta)O3 capacitor films on Si substrates, using a two-step process combining radio frequency (RF)-magnetron sputtering at 450 ℃ and post-deposition rapid thermal annealing (RTA). The RTA process at 700 ℃ led to sufficient crystallization of nanograins in the film, hindering their lateral growth by employing short annealing time of 5 min. The obtained Ag(Nb,Ta)O3 films showed an average grain size (D) of ~14 nm (obtained by Debye–Scherrer formula) and a slender room temperature (RT) polarization–electric field (P–E) loop (Pr ≈ 3.8 μC·cm−2 and Pmax ≈ 38 μC·cm−2 under an electric field of ~3.3 MV·cm−1), the P–E loop corresponding to a high recoverable energy density (Wrec) of ~46.4 J·cm−3 and an energy efficiency (η) of ~80.3%. Additionally, by analyzing temperature-dependent dielectric property of the film, a significant downshift of the diffused phase transition temperature (TM2–M3) was revealed, which indicated the existence of a stable relaxor-like AFE phase near the RT. The downshift of the TM2–M3 could be attributed to a nanograin size and residual tensile strain of the film, and it led to excellent temperature stability (20–240 ℃) of the energy storage performance of the film. Our results indicate that the Ag(Nb,Ta)O3 film is a promising candidate for electrical energy storage applications.


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About this article

Achieving a high energy storage density in Ag(Nb,Ta)O3 antiferroelectric films via nanograin engineering

Show Author's information Hongbo CHENGa,b,†, Xiao ZHAIc,†, Jun OUYANGa( ), Limei ZHENGc( ), Nengneng LUOd, Jinpeng LIUa, Hanfei ZHUa, Yingying WANGe, Lanxia HAOe, Kun WANGf
Institute of Advanced Energy Materials and Chemistry, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
College of Electronic and Optical Engineering, Nanjing University of Posts and Telecommunications, Nanjing 210023, China
School of Physics, Shandong University, Jinan 250100, China
Guangxi Key Laboratory of Processing for Non-ferrous Metallic and Featured Materials, School of Resources, Environment and Materials; Center on Nanoenergy Research, School of Physical Science and Technology, Guangxi University, Nanning 530004, China
Key Laboratory for Liquid-Solid Structure Evolution and Processing of Materials (Ministry of Education), School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Jinan Cigarette Factory, China Tobacco Shandong Industrial Co., Ltd., Jinan 250104, China

† Hongbo Cheng and Xiao Zhai contributed equally to this work.

Abstract

Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization (Pmax) and a small remnant polarization (Pr), AgNbO3-based antiferroelectrics (AFEs) have attracted extensive research interest for electric energy storage applications. However, a low dielectric breakdown field (Eb) limits an energy density and its further development. In this work, a highly efficient method was proposed to fabricate high-energy-density Ag(Nb,Ta)O3 capacitor films on Si substrates, using a two-step process combining radio frequency (RF)-magnetron sputtering at 450 ℃ and post-deposition rapid thermal annealing (RTA). The RTA process at 700 ℃ led to sufficient crystallization of nanograins in the film, hindering their lateral growth by employing short annealing time of 5 min. The obtained Ag(Nb,Ta)O3 films showed an average grain size (D) of ~14 nm (obtained by Debye–Scherrer formula) and a slender room temperature (RT) polarization–electric field (P–E) loop (Pr ≈ 3.8 μC·cm−2 and Pmax ≈ 38 μC·cm−2 under an electric field of ~3.3 MV·cm−1), the P–E loop corresponding to a high recoverable energy density (Wrec) of ~46.4 J·cm−3 and an energy efficiency (η) of ~80.3%. Additionally, by analyzing temperature-dependent dielectric property of the film, a significant downshift of the diffused phase transition temperature (TM2–M3) was revealed, which indicated the existence of a stable relaxor-like AFE phase near the RT. The downshift of the TM2–M3 could be attributed to a nanograin size and residual tensile strain of the film, and it led to excellent temperature stability (20–240 ℃) of the energy storage performance of the film. Our results indicate that the Ag(Nb,Ta)O3 film is a promising candidate for electrical energy storage applications.

Keywords: energy storage, antiferroelectrics (AFE), AgNbO3, Ag(Nb,Ta)O3, film capacitors, nanograin engineering

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Acknowledgements
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Publication history

Received: 05 July 2022
Revised: 15 October 2022
Accepted: 16 October 2022
Published: 19 December 2022
Issue date: January 2023

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© The Author(s) 2022.

Acknowledgements

The authors are deeply grateful for the financial support from the National Natural Science Foundation of China (Grant Nos. 51772175, 52072218, and 52002192), Natural Science Foundation of Shandong Province (Grant Nos. ZR2020QE042, ZR2022ZD39, and ZR2022ME031), 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). Hongbo Cheng acknowledges the support from the Jiangsu Province NSFC (Grant No. BK20180764). Limei Zheng acknowledges the support from the National Key R&D Program of China (Grant No. 2021YFB3601504) and Natural Science Foundation of Shandong Province (Grant No. ZR2020KE019).

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