4.6 Article

Aliovalent A-site engineered AgNbO3 lead-free antiferroelectric ceramics toward superior energy storage density

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 7, Issue 23, Pages 14118-14128

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta02053e

Keywords

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Funding

  1. National Natural Science Foundation of China [11864004]
  2. Guangxi Natural Science Foundation [2017GXNSFBA198132, 2016GXNSFCB380006, 2016GXNSFAA380214, 2017GXNSFFA198015]
  3. Science and Technology Major Project of Guangxi [AA17204100]
  4. funds of the State Key Laboratory of New Ceramics and Fine Processing, Tsinghua University, Beijing, China

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Lead-free dielectric capacitors with high energy storage density and temperature-insensitive performance are pivotal to pulsed power systems. In this work, a pronounced recoverable energy storage density (W-rec) was achieved in AgNbO3-based lead-free antiferroelectric ceramics, by aliovalent A-site Sm mediation. The Sm modification was found to alter the crystal structure and enhance the interaction among the ions by affecting the electronic structure, leading to improved antiferroelectricity. The Sm0.03Ag0.91NbO3 solid solution exhibited a superior W-rec of 5.2 J cm(-3) with a high energy storage efficiency (eta) of 68.5% at an applied electric field of 290 kV cm(-1). Excellent temperature stability of W-rec with a minimal variation of less than 4% from room temperature up to 140 degrees C was also observed. Meanwhile, the Sm0.03Ag0.91NbO3 ceramic also exhibited an ultrafast discharge speed (similar to 20 mu s) and high discharge energy density (4.2 J cm(-3)). Ginzburg-Landau-Devonshire (GLD) phenomenology revealed that the significantly stabilized antiferroelectricity and the cation disorder were responsible for the ultrahigh W-rec and eta. The extraordinary energy storage performance indicates the SmxAg1-3xNbO3 system a promising candidate for advanced pulsed power capacitors. More importantly, the results show that aliovalent A-site engineering is an effective way to achieve high energy storage density.

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