Chemical Design of Pb-Free Relaxors for Giant Capacitive Energy Storage

Liu, Hui; Sun, Zheng; Zhang, Ji; Luo, Huajie; Zhang, Qinghua; Yao, Yonghao; Deng, Shiqing; Qi, He; Liu, Jue; Gallington, Leighanne C.; Neuefeind, Joerg C.; Chen, Jun

doi:10.1021/jacs.3c02811

Chemical Design of Pb-Free Relaxors for Giant Capacitive Energy Storage

Journal Article · Fri May 19 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c02811· OSTI ID:2404847

^[1]; Sun, Zheng ^[1]; ^[2]; Luo, Huajie ^[1]; Zhang, Qinghua ^[3]; Yao, Yonghao ^[1]; ^[1]; ^[1]; ^[4]; ^[5]; Neuefeind, Joerg C. ^[4]; ^[6]

University of Science and Technology Beijing (China)
Nanjing University of Science and Technology (China)
Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
University of Science and Technology Beijing (China); Hainan University, Haikou (China)

Dielectric capacitors have captured substantial attention for advanced electrical and electronic systems. Developing dielectrics with high energy density and high storage efficiency is challenging owing to the high compositional diversity and the lack of general guidelines. Herein, we propose a map that captures the structural distortion ($$\delta$$) and tolerance factor (t) of perovskites to design Pb-free relaxors with extremely high capacitive energy storage. Our map shows how to select ferroelectric with large $$\delta$$ and paraelectric components to form relaxors with a t value close to 1 and thus obtaining eliminated hysteresis and large polarization under a high electric breakdown. Taking the Bi_0.5Na_0.5TiO₃-based solid solution as an example, we demonstrate that composition-driven predominant order-disorder characteristic of local atomic polar displacements endows the relaxor with a slushlike structure and strong local polar fluctuations at several nanoscale. This leads to a giant recoverable energy density of 13.6 J cm^-3, along with an ultrahigh efficiency of 94%, which is far beyond the current performance boundary reported in Pb-free bulk ceramics. In conclusion, our work provides a solution through rational chemical design for obtaining Pb-free relaxors with outstanding energy-storage properties.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (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:: AC02-06CH11357

OSTI ID:: 2404847

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 21 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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