<p>A critical challenge for the application of lead-free antiferroelectrics in energy storage systems is their poor thermal stability and low efficiency when the superior energy storage density is attained, primarily due to the inherent first-order nature and narrow temperature window of antiferroelectric-to-ferroelectric transitions. Here, we elucidate a unique percolating interaction between antipolar regions in antiferroelectrics and engineered defect pairs using density functional theory and phase field calculations. Strategic distribution of the strongly coupled Li-Ta pairs in AgNbO<sub>3</sub> fosters a percolating interaction that facilitates antipolar rotations, enabling a pronounced polarization change with minimal hysteresis. Guided by theoretical calculations, a large recoverable energy storage density of 12.8 J/cm<sup>3</sup>, with a high efficiency of 90%, is achieved at room temperature in Ag<sub>0.95</sub>Li<sub>0.05</sub>Nb<sub>0.35</sub>Ta<sub>0.65</sub>O<sub>3</sub> ceramics. Moreover, the superior energy storage performance can remain stable within a wide temperature range from −70 to 170 °C, which paves the way for application in advanced energy capacitors.</p>

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Ultrahigh energy storage density and efficiency in AgNbO3-based ceramics by percolating interaction between antipolar regions and defect pairs

  • Liqiang He,
  • Le Zhang,
  • Yating Ran,
  • Cunle Bo,
  • Kaiyun Chen,
  • Yao Liu,
  • Chen Zhang,
  • Zihao Zheng,
  • Jinming Guo,
  • Danyang Wang,
  • Shujun Zhang,
  • Sen Yang,
  • Xiaobing Ren,
  • Zibin Chen,
  • Dong Wang

摘要

A critical challenge for the application of lead-free antiferroelectrics in energy storage systems is their poor thermal stability and low efficiency when the superior energy storage density is attained, primarily due to the inherent first-order nature and narrow temperature window of antiferroelectric-to-ferroelectric transitions. Here, we elucidate a unique percolating interaction between antipolar regions in antiferroelectrics and engineered defect pairs using density functional theory and phase field calculations. Strategic distribution of the strongly coupled Li-Ta pairs in AgNbO3 fosters a percolating interaction that facilitates antipolar rotations, enabling a pronounced polarization change with minimal hysteresis. Guided by theoretical calculations, a large recoverable energy storage density of 12.8 J/cm3, with a high efficiency of 90%, is achieved at room temperature in Ag0.95Li0.05Nb0.35Ta0.65O3 ceramics. Moreover, the superior energy storage performance can remain stable within a wide temperature range from −70 to 170 °C, which paves the way for application in advanced energy capacitors.