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Large Energy Density, Excellent Thermal Stability and High Cycling Endurance of Lead-Free BaZr0.2Ti0.8O3 Film Capacitors Zixiong Sun, Chunrui Ma, Xi Wang, Ming Liu, Lu Lu, Ming Wu, Xiaojie Lou, Hong Wang, and Chun-Lin Jia ACS Appl. Mater. Interfaces, Just Accepted Manuscript • Publication Date (Web): 04 May 2017 Downloaded from http://pubs.acs.org on May 6, 2017

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ACS Applied Materials & Interfaces

Large Energy Density, Excellent Thermal Stability and High Cycling Endurance of Lead-Free BaZr0.2Ti0.8O3 Film Capacitors

Zixiong Sun,†,‡ Chunrui Ma,‡∗ Xi Wang,& Ming Liu,†,‡∗ Lu Lu,†,‡ Ming Wu,# Xiaojie Lou,# Hong Wang,†,‡ Chun-Lin Jia†,‡,₤



State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, P. R. China



School of Microelectronics, Xi’an Jiaotong University, Xi’an 710049, China

&

School of Mathermatics and Physics, Handan College, Handan, 056005, China

#

Frontier Institute of Science and Technology, Xi’an Jiaotong University, Xi’an 710049, China



Peter Grünberg Institute and Ernst Ruska Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich, D-52425 Jülich, Germany

Keywords: Lead-free Ceramic, Dielectrics, Thin Films, Energy Storage Density, Thermal Stability.

∗ Electronic address: [email protected]; [email protected] 1

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Abstract: Large energy storage density (ESD) of 30.4 J/cm3 and high energy efficiency of 81.7% under electrical field of 3 MV/cm was achieved at room temperature by the fabrication of environment-friendly lead-free BaZr0.2Ti0.8O3 epitaxial thin films on Nb doped SrTiO3 (001) substrates by using radio frequency magnetron sputtering system. Moreover, the BZT film capacitors exhibit great thermal stability of the ESD from 16.8 J/cm3 to 14.0 J/cm3 with efficiency of beyond 67.4% and high fatigue endurance (up to 106 cycles) in wide temperature range from RT to 125 oC. Compared to other BaTiO3-based energy storage capacitor materials and even Pb-based systems, BaZr0.2Ti0.8O3 thin film capacitors show either high ESD or great energy efficiency. All these excellent results revealed that the BaZr0.2Ti0.8O3 film capacitors have huge potential in the application of modern electronic, such as locomotive and pulse power, in harsh working environment.

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ACS Applied Materials & Interfaces

Introduction Dielectric materials play a key role in modern electronics such as in charges controlling and electric energy harvesting/storing. Due to the increasing serious energy crisis, devices based on dielectric energy storage materials have attracted increasing attention by scientists and technicians. Among them, power electronics has been widely used in the last few decades in either the industrial manufacture or daily life, which could provide faster charging-discharging, better storage efficiency and higher storage energy density compared with Li-ion batteries, super-capacitors, and fuel cells.[1][2][3] The rapid development of solid-state devices with high integration, lightweight and wearability provides more chances and possibilities for the thick/thin film materials. Not only the low-dimensional scale but also lots of superior performances than bulk materials, such as higher electrical breakdown strength, larger energy storage density have attracted more and more attentions.[4][5][6][7][8][9][10][11][12] Pb-based antiferroelectric thin films have been deeply investigated for its good energy storage density (ESD) in a broad temperature range

[13][14][15][16]

. However, the harm of Pb to environment and human-beings will

inevitably limit its applications. Therefore, the research on lead-free materials has become very important and urgent. As one of the most potential systems for replacing Pb-based materials, BaTiO3-based (BT-based) systems exhibit much more superior in energy storage. Puli et al. and Kwon et al. have reported the BT-based thin film capacitors of (Ba0.955Ca0.045)(Zr0.17Ti0.83)O3

and

0.88BaTiO3-0.12Bi(Mg,Ti)O3

systems,

respectively.[17][18] The (Ba0.955Ca0.045)(Zr0.17Ti0.83)O3 film capacitor can achieve high energy storage density (ESD) of 39.1 J/cm3 at room temperature (RT), but the energy storage efficiency (η) is very low,