Local Chemical Clustering Enabled Ultrahigh Capacitive Energy Storage in Pb-Free Relaxors

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

doi:10.1021/jacs.3c06912

Local Chemical Clustering Enabled Ultrahigh Capacitive Energy Storage in Pb-Free Relaxors

Journal Article · Tue Aug 22 04:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c06912· OSTI ID:2404941

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

Univ. of Science and Technology, Beijing (China)
Nanjing Univ. of Science and Technology (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. of Science and Technology, Beijing (China); Hainan University (China)

Designing Pb-free relaxors with both a high capacitive energy density (W_rec) and high storage efficiency (η) remains a remarkable challenge for cutting-edge pulsed power technologies. Local compositional heterogeneity is crucial for achieving complex polar structure in solid solution relaxors, but its role in optimizing energy storage properties is often overlooked. Here, in this paper, we report that an exceptionally high W_rec of 15.2 J cm^–3 along with an ultrahigh η of 91% can be achieved through designing local chemical clustering in Bi_0.5Na_0.5TiO₃–BaTiO₃-based relaxors. A three-dimensional atomistic model derived from neutron/X-ray total scattering combined with reverse Monte Carlo method reveals the presence of subnanometer scale clustering of Bi, Na, and Ba, which host differentiated polar displacements, and confirming the prediction by density functional theory calculations. This leads to a polar state with small polar clusters and strong length and direction fluctuations in unit-cell polar vectors, thus manifesting improved high-field polarizability, steadily reduced hysteresis, and high breakdown strength macroscopically. The favorable polar structure features also result in a unique field-increased η, excellent stability, and superior discharge capacity. Our work demonstrates that the hidden local chemical order exerts a significant impact on the polarization characteristic of relaxors, and can be exploited for accessing superior energy storage performance.

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). Scientific User Facilities (SUF); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2404941

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 35 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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