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Superior Capacitive Energy-Storage Performance in Pb-Free Relaxors with a Simple Chemical Composition

  • Zheng Sun
    Zheng Sun
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    School of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, China
    More by Zheng Sun
  • Ji Zhang
    Ji Zhang
    School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, Jiangsu 210094, China
    More by Ji Zhang
  • Huajie Luo
    Huajie Luo
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by Huajie Luo
  • Yonghao Yao
    Yonghao Yao
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by Yonghao Yao
  • Na Wang
    Na Wang
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by Na Wang
  • Liang Chen
    Liang Chen
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by Liang Chen
  • Tianyu Li
    Tianyu Li
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by Tianyu Li
  • Changzheng Hu
    Changzheng Hu
    College of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, China
  • He Qi
    He Qi
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    More by He Qi
  • Shiqing Deng
    Shiqing Deng
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    School of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, China
    More by Shiqing Deng
  • Leighanne C. Gallington
    Leighanne C. Gallington
    X-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
  • Yuanpeng Zhang
    Yuanpeng Zhang
    Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Joerg C. Neuefeind
    Joerg C. Neuefeind
    Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Hui Liu*
    Hui Liu
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    School of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, China
    *Email: [email protected]
    More by Hui Liu
  • , and 
  • Jun Chen*
    Jun Chen
    Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
    School of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, China
    Department of Physical Chemistry, University of Science and Technology Beijing, Beijing 100083, China
    *Email: [email protected]
    More by Jun Chen
Cite this: J. Am. Chem. Soc. 2023, 145, 11, 6194–6202
Publication Date (Web):March 9, 2023
https://doi.org/10.1021/jacs.2c12200
Copyright © 2023 American Chemical Society

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    Abstract

    Abstract Image

    Chemical design of lead-free relaxors with simultaneously high energy density (Wrec) and high efficiency (η) for capacitive energy-storage has been a big challenge for advanced electronic systems. The current situation indicates that realizing such superior energy-storage properties requires highly complex chemical components. Herein, we demonstrate that, via local structure design, an ultrahigh Wrec of 10.1 J/cm3, concurrent with a high η of 90%, as well as excellent thermal and frequency stabilities can be achieved in a relaxor with a very simple chemical composition. By introducing 6s2 lone pair stereochemical active Bi into the classical BaTiO3 ferroelectric to generate a mismatch between A- and B-site polar displacements, a relaxor state with strong local polar fluctuations can be formed. Through advanced atomic-resolution displacement mapping and 3D reconstructing the nanoscale structure from neutron/X-ray total scattering, it is revealed that the localized Bi enhances the polar length largely at several perovskite unit cells and disrupts the long-range coherent Ti polar displacements, resulting in a slush-like structure with extremely small size polar clusters and strong local polar fluctuations. This favorable relaxor state exhibits substantially enhanced polarization, and minimized hysteresis at a high breakdown strength. This work offers a feasible avenue to chemically design new relaxors with a simple composition for high-performance capacitive energy-storage.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c12200.

    • Experimental section for materials synthesis, electrical property measurements, and structure characterization including STEM, neutron–/X-ray-total scattering, and detailed big-box RMC refinement analysis (PDF)

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    Cited By

    This article is cited by 8 publications.

    1. Zheng Sun, Hui Liu, Ji Zhang, Huajie Luo, Yonghao Yao, Yuanpeng Zhang, Laijun Liu, Joerg C. Neuefeind, Jun Chen. Strong Local Polarization Fluctuations Enabled High Electrostatic Energy Storage in Pb-Free Relaxors. Journal of the American Chemical Society 2024, 146 (19) , 13467-13476. https://doi.org/10.1021/jacs.4c02868
    2. Botao Gao, Zhengyang Zhou, Shiqing Deng, Koomok Lee, Masayuki Fukuda, Lei Hu, Masaki Azuma, Hui Liu, Jun Chen. Emergent Three-Dimensional Electric Dipole Sinewave in Bulk Perovskite Oxides. Nano Letters 2024, 24 (10) , 3118-3124. https://doi.org/10.1021/acs.nanolett.3c04957
    3. Hui Liu, Zheng Sun, Ji Zhang, Huajie Luo, Yuanpeng Zhang, Andrea Sanson, Manuel Hinterstein, Laijun Liu, Joerg C. Neuefeind, Jun Chen. Chemical Framework to Design Linear-like Relaxors toward Capacitive Energy Storage. Journal of the American Chemical Society 2024, 146 (5) , 3498-3507. https://doi.org/10.1021/jacs.3c13405
    4. Huajie Luo, Zheng Sun, Ji Zhang, Hailong Xie, Yonghao Yao, Tianyu Li, Chenjie Lou, Huashan Zheng, Na Wang, Shiqing Deng, Li-Feng Zhu, Jue Liu, Joerg C. Neuefeind, Matthew G. Tucker, Mingxue Tang, Hui Liu, Jun Chen. Outstanding Energy-Storage Density Together with Efficiency of above 90% via Local Structure Design. Journal of the American Chemical Society 2024, 146 (1) , 460-467. https://doi.org/10.1021/jacs.3c09805
    5. Kaibiao Xi, Yudong Hou, Xiaole Yu, Mupeng Zheng, Mankang Zhu. Optimizing Output Power Density in Lead-Free Energy-Harvesting Piezoceramics with an Entropy-Increasing Polymorphic Phase Transition Structure. ACS Applied Materials & Interfaces 2023, 15 (44) , 51330-51338. https://doi.org/10.1021/acsami.3c10426
    6. Ziming Cai, Hang Yang, Chaoqiong Zhu, Shiheng Li, Bingcheng Luo, Aoyu Li, Xinheng Li, Zhaobo Tian, Peizhong Feng. Local Heterogeneous Polarization Enhanced Superior Low-Field Energy Storage Performance in Lead-Free Relaxor Ferroelectric Ceramics. ACS Sustainable Chemistry & Engineering 2023, 11 (37) , 13729-13735. https://doi.org/10.1021/acssuschemeng.3c03618
    7. Hui Liu, Zheng Sun, Ji Zhang, Huajie Luo, Yonghao Yao, Xingcheng Wang, He Qi, Shiqing Deng, Jue Liu, Leighanne C. Gallington, Yuanpeng Zhang, Joerg C. Neuefeind, Jun Chen. Local Chemical Clustering Enabled Ultrahigh Capacitive Energy Storage in Pb-Free Relaxors. Journal of the American Chemical Society 2023, 145 (35) , 19396-19404. https://doi.org/10.1021/jacs.3c06912
    8. Hui Liu, Zheng Sun, Ji Zhang, Huajie Luo, Qinghua Zhang, Yonghao Yao, Shiqing Deng, He Qi, Jue Liu, Leighanne C. Gallington, Joerg C. Neuefeind, Jun Chen. Chemical Design of Pb-Free Relaxors for Giant Capacitive Energy Storage. Journal of the American Chemical Society 2023, 145 (21) , 11764-11772. https://doi.org/10.1021/jacs.3c02811

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