Chemical Framework to Design Linear-like Relaxors toward Capacitive Energy Storage

Liu, Hui; Sun, Zheng; Zhang, Ji; Luo, Huajie; Zhang, Yuanpeng; Sanson, Andrea; Hinterstein, Manuel; Liu, Laijun; Neuefeind, Joerg C.; Chen, Jun

doi:10.1021/jacs.3c13405

Chemical Framework to Design Linear-like Relaxors toward Capacitive Energy Storage

Journal Article · Mon Jan 22 23:00:00 EST 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c13405· OSTI ID:2573471

^[1]; Sun, Zheng ^[1]; ^[2]; Luo, Huajie ^[1]; ^[3]; ^[4]; ^[5]; ^[6]; ^[3]; ^[7]

University of Science and Technology Beijing (China)
Nanjing Univ. of Information Science and Technology (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of Padova (Italy)
Fraunhofer Institute for Mechanics of Materials IWM, Freiburg (Germany)
Guilin University of Technology (China)
University of Science and Technology Beijing (China); Hainan University (China)

ABO₃-type perovskite relaxor ferroelectrics (RFEs) have emerged as the preferred option for dielectric capacitive energy storage. However, the compositional design of RFEs with high energy density and efficiency poses significant challenges owing to the vast compositional space and the absence of general rules. Here, we present an atomic-level chemical framework that captures inherent characteristics in terms of radius and ferroelectric activity of ions. By categorizing A/B-site ions as host framework, rattling, ferroelectrically active, and blocking ions and assembling these four types of ions with specific criteria, linear-like relaxors with weak locally correlated and highly extendable unit-cell polarization vectors can be constructed. As example, we demonstrate two new compositions of Bi_0.5K_0.5TiO_3-based and BaTiO_3-based relaxors, showing extremely high recoverable energy densities of 17.3 and 12.1 J cm^–3, respectively, both with a high efficiency of about 90%. Further, the role of different types of ions in forming heterogeneous polar structures is identified through element-specific local structure analysis using neutron total scattering combined with reverse Monte Carlo modeling. Further, our work not only opens up new avenues toward rational compositional design of high energy storage performance lead-free RFEs but also sheds light on atomic-level manipulation of functional properties in compositionally complex ferroelectrics.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); China Postdoctoral Science Foundation

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573471

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 146; ISSN 0002-7863; ISSN 1520-5126

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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