Tailoring high-energy storage NaNbO3-based materials from antiferroelectric to relaxor states

Mao-Hua Zhang; Hui Ding; Sonja Egert; Changhao Zhao; Lorenzo Villa; Lovro Fulanović; Pedro B Groszewicz; Gerd Buntkowsky; Hans-Joachim Kleebe; Karsten Albe; Andreas Klein; Jurij Koruza

doi:10.1038/s41467-023-37060-4

Tailoring high-energy storage NaNbO₃-based materials from antiferroelectric to relaxor states

Nat Commun. 2023 Mar 18;14(1):1525. doi: 10.1038/s41467-023-37060-4.

Authors

Mao-Hua Zhang^{1

2}, Hui Ding³, Sonja Egert⁴, Changhao Zhao⁵, Lorenzo Villa⁶, Lovro Fulanović⁵, Pedro B Groszewicz⁷, Gerd Buntkowsky⁴, Hans-Joachim Kleebe⁸, Karsten Albe⁶, Andreas Klein⁹, Jurij Koruza^{10

11}

Affiliations

¹ Non-metallic Inorganic Materials, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany. maohua.zhang.10@gmail.com.
² Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, 16802, USA. maohua.zhang.10@gmail.com.
³ Advanced Electron Microscopy, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany.
⁴ Eduard Zintl Institute for Inorganic and Physical Chemistry, Technical University of Darmstadt, Darmstadt, 64287, Germany.
⁵ Non-metallic Inorganic Materials, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany.
⁶ Materials Modeling Division, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany.
⁷ Department of Radiation Science and Technology, Delft University of Technology, 2600AA, Delft, The Netherlands.
⁸ Institute of Applied Geosciences, Geomaterial Science, Technical University of Darmstadt, Darmstadt, 64287, Germany.
⁹ Electronic Structure of Materials, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany.
¹⁰ Non-metallic Inorganic Materials, Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt, 64287, Germany. jurij.koruza@tugraz.at.
¹¹ Institute for Chemistry and Technology of Materials, Graz University of Technology, Graz, 8010, Austria. jurij.koruza@tugraz.at.

Abstract

Reversible field-induced phase transitions define antiferroelectric perovskite oxides and lay the foundation for high-energy storage density materials, required for future green technologies. However, promising new antiferroelectrics are hampered by transition´s irreversibility and low electrical resistivity. Here, we demonstrate an approach to overcome these problems by adjusting the local structure and defect chemistry, delivering NaNbO₃-based antiferroelectrics with well-defined double polarization loops. The attending reversible phase transition and structural changes at different length scales are probed by in situ high-energy X-ray diffraction, total scattering, transmission electron microcopy, and nuclear magnetic resonance spectroscopy. We show that the energy-storage density of the antiferroelectric compositions can be increased by an order of magnitude, while increasing the chemical disorder transforms the material to a relaxor state with a high energy efficiency of 90%. The results provide guidelines for efficient design of (anti-)ferroelectrics and open the way for the development of new material systems for a sustainable future.