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

Sun, Zheng; Zhang, Ji; Luo, Huajie; Yao, Yonghao; Wang, Na; Chen, Liang; Li, Tianyu; Hu, Changzheng; Qi, He; Deng, Shiqing; Gallington, Leighanne C.; Zhang, Yuanpeng; Neuefeind, Joerg C.; Liu, Hui; Chen, Jun

doi:10.1021/jacs.2c12200

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

Journal Article · Thu Mar 09 00:00:00 EST 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c12200· OSTI ID:1965228

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

University of Science and Technology, Beijing (China)
Nanjing University of Science and Technology (China)
Guilin University of Technology (China)
Argonne National Laboratory (ANL), Lemont, IL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Chemical design of lead-free relaxors with simultaneously high energy density (W_rec) 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 W_recof 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Lemont, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Central Universities, China; China Postdoctoral Science Foundation; Fundamental Research Funds for the Central Universities; National Natural Science Foundation of China; National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1965228

Alternate ID(s):: OSTI ID: 2404499

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 11 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (54)

Ultrahigh Energy‐Storage Density in NaNbO ₃ ‐Based Lead‐Free Relaxor Antiferroelectric Ceramics with Nanoscale Domains Qi, He; Zuo, Ruzhong; Xie, Aiwen Advanced Functional Materials, Vol. 29, Issue 35 https://doi.org/10.1002/adfm.201903877	journal	July 2019
Improved Energy Storage Properties Achieved in (K, Na)NbO ₃ ‑Based Relaxor Ferroelectric Ceramics via a Combinatorial Optimization Strategy Li, Da; Zhou, Di; Wang, Dong Advanced Functional Materials, Vol. 32, Issue 15 https://doi.org/10.1002/adfm.202111776	journal	December 2021
Homogeneous/Inhomogeneous-Structured Dielectrics and their Energy-Storage Performances Yao, Zhonghua; Song, Zhe; Hao, Hua Advanced Materials, Vol. 29, Issue 20 https://doi.org/10.1002/adma.201601727	journal	February 2017
Lead-Free Antiferroelectric Silver Niobate Tantalate with High Energy Storage Performance Zhao, Lei; Liu, Qing; Gao, Jing Advanced Materials, Vol. 29, Issue 31 https://doi.org/10.1002/adma.201701824	journal	June 2017
Multilayer Lead-Free Ceramic Capacitors with Ultrahigh Energy Density and Efficiency Li, Jinglei; Li, Fei; Xu, Zhuo Advanced Materials, Vol. 30, Issue 32 https://doi.org/10.1002/adma.201802155	journal	June 2018
Supercritical Relaxor Nanograined Ferroelectrics for Ultrahigh‐Energy‐Storage Capacitors Xie, Aiwen; Fu, Jian; Zuo, Ruzhong Advanced Materials, Vol. 34, Issue 34 https://doi.org/10.1002/adma.202204356	journal	July 2022
Local Diverse Polarization Optimized Comprehensive Energy‐Storage Performance in Lead‐Free Superparaelectrics Chen, Liang; Wang, Na; Zhang, Zhifei Advanced Materials, Vol. 34, Issue 44 https://doi.org/10.1002/adma.202205787	journal	October 2022
High‐Performance Relaxor Ferroelectric Materials for Energy Storage Applications Zhao, Peiyao; Wang, Hongxian; Wu, Longwen Advanced Energy Materials, Vol. 9, Issue 17 https://doi.org/10.1002/aenm.201803048	journal	March 2019
Superior Energy‐Storage Capacitors with Simultaneously Giant Energy Density and Efficiency Using Nanodomain Engineered BiFeO ₃ ‐BaTiO ₃ ‐NaNbO ₃ Lead‐Free Bulk Ferroelectrics Qi, He; Xie, Aiwen; Tian, Ao Advanced Energy Materials, Vol. 10, Issue 6 https://doi.org/10.1002/aenm.201903338	journal	December 2019
Progress on Emerging Ferroelectric Materials for Energy Harvesting, Storage and Conversion Wei, Xian‐Kui; Domingo, Neus; Sun, Young Advanced Energy Materials, Vol. 12, Issue 24 https://doi.org/10.1002/aenm.202201199	journal	May 2022
Design of superior electrostriction in BaTiO ₃ ‐based lead‐free relaxors via the formation of polarization nanoclusters Wang, Lu; Qi, He; Deng, Shiqing InfoMat, Vol. 5, Issue 1 https://doi.org/10.1002/inf2.12362	journal	September 2022
Effects of Sintering Method and BiAlO₃Dopant on Dielectric Relaxation and Energy Storage Properties of BaTiO₃–BiYbO₃Ceramics Yi, Xin; Ji, Cong; Chen, Gang physica status solidi (a), Vol. 217, Issue 2 https://doi.org/10.1002/pssa.201900721	journal	December 2019
Underneath the Bragg Peaks Egami, T.; Billinge, S. J. L. Materials Today, Vol. 6, Issue 6 https://doi.org/10.1016/S1369-7021(03)00635-7	journal	June 2003
Optimization the energy density and efficiency of BaTiO3-based ceramics for capacitor applications Hu, Di; Pan, Zhongbin; Tan, Xiaoyan Chemical Engineering Journal, Vol. 409 https://doi.org/10.1016/j.cej.2020.127375	journal	April 2021
Excellent energy storage and hardness performance of Sr0.7Bi0.2TiO3 ceramics fabricated by solution combustion-synthesized nanopowders Zuo, Chengyang; Yang, Shilin; Cao, Zhiqin Chemical Engineering Journal, Vol. 442 https://doi.org/10.1016/j.cej.2022.136330	journal	August 2022
Combining high energy efficiency and fast charge-discharge capability in novel BaTiO3-based relaxor ferroelectric ceramic for energy-storage Zhou, Mingxing; Liang, Ruihong; Zhou, Zhiyong Ceramics International, Vol. 45, Issue 3 https://doi.org/10.1016/j.ceramint.2018.11.018	journal	February 2019
Significantly enhanced energy storage density and efficiency of BNT-based perovskite ceramics via A-site defect engineering Yan, Fei; Huang, Kaiwei; Jiang, Tao Energy Storage Materials, Vol. 30 https://doi.org/10.1016/j.ensm.2020.05.026	journal	September 2020
Giant energy density and high efficiency achieved in silver niobate-based lead-free antiferroelectric ceramic capacitors via domain engineering Li, Song; Hu, Tengfei; Nie, Hengchang Energy Storage Materials, Vol. 34 https://doi.org/10.1016/j.ensm.2020.09.021	journal	January 2021
Ultrahigh energy density in short-range tilted NBT-based lead-free multilayer ceramic capacitors by nanodomain percolation Ji, Hongfen; Wang, Dawei; Bao, Weichao Energy Storage Materials, Vol. 38 https://doi.org/10.1016/j.ensm.2021.01.023	journal	June 2021
Enhanced electric resistivity and dielectric energy storage by vacancy defect complex Pan, Hao; Feng, Nan; Xu, Xing Energy Storage Materials, Vol. 42 https://doi.org/10.1016/j.ensm.2021.08.027	journal	November 2021
Ultrahigh energy storage density in lead-free relaxor antiferroelectric ceramics via domain engineering Jiang, Jie; Meng, Xiangjun; Li, Ling Energy Storage Materials, Vol. 43 https://doi.org/10.1016/j.ensm.2021.09.018	journal	December 2021
Significant increase in comprehensive energy storage performance of potassium sodium niobate-based ceramics via synergistic optimization strategy Zhang, Miao; Yang, Haibo; Lin, Ying Energy Storage Materials, Vol. 45 https://doi.org/10.1016/j.ensm.2021.12.037	journal	March 2022
Enhanced energy storage and fast discharge properties of BaTiO3 based ceramics modified by Bi(Mg1/2Zr1/2)O3 Jiang, Xuewen; Hao, Hua; Zhang, Shujun Journal of the European Ceramic Society, Vol. 39, Issue 4 https://doi.org/10.1016/j.jeurceramsoc.2018.11.025	journal	April 2019
Achieve ultrahigh energy storage performance in BaTiO3–Bi(Mg1/2Ti1/2)O3 relaxor ferroelectric ceramics via nano-scale polarization mismatch and reconstruction Hu, Qingyuan; Tian, Ye; Zhu, Qingshan Nano Energy, Vol. 67 https://doi.org/10.1016/j.nanoen.2019.104264	journal	January 2020
Mechanism of enhanced energy storage density in AgNbO3-based lead-free antiferroelectrics Lu, Zhilun; Bao, Weichao; Wang, Ge Nano Energy, Vol. 79 https://doi.org/10.1016/j.nanoen.2020.105423	journal	January 2021
Perovskite lead-free dielectrics for energy storage applications Yang, Letao; Kong, Xi; Li, Fei Progress in Materials Science, Vol. 102 https://doi.org/10.1016/j.pmatsci.2018.12.005	journal	May 2019
Electroceramics for High-Energy Density Capacitors: Current Status and Future Perspectives Wang, Ge; Lu, Zhilun; Li, Yong Chemical Reviews, Vol. 121, Issue 10 https://doi.org/10.1021/acs.chemrev.0c01264	journal	April 2021
Multifunctional BaTiO₃-Based Relaxor Ferroelectrics toward Excellent Energy Storage Performance and Electrostrictive Strain Benefiting from Crossover Region Huang, Yanli; Zhao, Chunlin; Wu, Bo ACS Applied Materials & Interfaces, Vol. 12, Issue 21 https://doi.org/10.1021/acsami.0c03677	journal	April 2020
Novel BaTiO ₃ -Based, Ag/Pd-Compatible Lead-Free Relaxors with Superior Energy Storage Performance Yang, Huijing; Lu, Zhilun; Li, Linhao ACS Applied Materials & Interfaces, Vol. 12, Issue 39 https://doi.org/10.1021/acsami.0c13057	journal	September 2020
Slush-like polar structures in single-crystal relaxors Takenaka, Hiroyuki; Grinberg, Ilya; Liu, Shi Nature, Vol. 546, Issue 7658 https://doi.org/10.1038/nature22068	journal	June 2017
Constructing phase boundary in AgNbO3 antiferroelectrics: pathway simultaneously achieving high energy density and efficiency Luo, Nengneng; Han, Kai; Cabral, Matthew J. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-18665-5	journal	September 2020
Atomic scale symmetry and polar nanoclusters in the paraelectric phase of ferroelectric materials Bencan, Andreja; Oveisi, Emad; Hashemizadeh, Sina Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23600-3	journal	June 2021
Giant energy-storage density with ultrahigh efficiency in lead-free relaxors via high-entropy design Chen, Liang; Deng, Shiqing; Liu, Hui Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30821-7	journal	June 2022
Grain-orientation-engineered multilayer ceramic capacitors for energy storage applications Li, Jinglei; Shen, Zhonghui; Chen, Xianghua Nature Materials, Vol. 19, Issue 9 https://doi.org/10.1038/s41563-020-0704-x	journal	June 2020
High-entropy enhanced capacitive energy storage Yang, Bingbing; Zhang, Yang; Pan, Hao Nature Materials, Vol. 21, Issue 9 https://doi.org/10.1038/s41563-022-01274-6	journal	June 2022
Ultrahigh energy storage density lead-free multilayers by controlled electrical homogeneity Wang, Ge; Li, Jinglei; Zhang, Xun Energy & Environmental Science, Vol. 12, Issue 2 https://doi.org/10.1039/C8EE03287D	journal	January 2019
Enhanced antiferroelectric phase stability in La-doped AgNbO₃: perspectives from the microstructure to energy storage properties Gao, Jing; Zhang, Yichi; Zhao, Lei Journal of Materials Chemistry A, Vol. 7, Issue 5 https://doi.org/10.1039/C8TA09353A	journal	January 2019
High temperature lead-free BNT-based ceramics with stable energy storage and dielectric properties Zhu, Chaoqiong; Cai, Ziming; Luo, Bingcheng Journal of Materials Chemistry A, Vol. 8, Issue 2 https://doi.org/10.1039/C9TA10347C	journal	January 2020
Ultra-high energy storage performance in lead-free multilayer ceramic capacitors via a multiscale optimization strategy Zhao, Peiyao; Cai, Ziming; Chen, Lingling Energy & Environmental Science, Vol. 13, Issue 12 https://doi.org/10.1039/D0EE03094E	journal	January 2020
Multiscale structural engineering of dielectric ceramics for energy storage applications: from bulk to thin films Yao, Fang-Zhou; Yuan, Qibin; Wang, Qing Nanoscale, Vol. 12, Issue 33 https://doi.org/10.1039/D0NR04479B	journal	January 2020
High-performance lead-free bulk ceramics for electrical energy storage applications: design strategies and challenges Yang, Zetian; Du, Hongliang; Jin, Li Journal of Materials Chemistry A, Vol. 9, Issue 34 https://doi.org/10.1039/D1TA04504K	journal	January 2021
Superior energy storage properties in NaNbO₃-based ceramics via synergistically optimizing domain and band structures Yang, Weiwei; Zeng, Huarong; Yan, Fei Journal of Materials Chemistry A, Vol. 10, Issue 21 https://doi.org/10.1039/D2TA02534E	journal	January 2022
Simultaneous achievement of ultrahigh energy storage density and high efficiency in BiFeO₃-based relaxor ferroelectric ceramics via a highly disordered multicomponent design Cui, Tao; Zhang, Ji; Guo, Jian Journal of Materials Chemistry A, Vol. 10, Issue 27 https://doi.org/10.1039/D2TA02893J	journal	January 2022
Designing pseudocubic perovskites with enhanced nanoscale polarization Levin, I.; Laws, W. J.; Wang, D. Applied Physics Letters, Vol. 111, Issue 21 https://doi.org/10.1063/1.5007700	journal	November 2017
Dielectric and pyroelectric properties in the Pb(Mg _1/3 Nb _2/3 )O ₃ -PbTiO ₃ system Choi, S. W.; Shrout, R. T. R.; Jang, S. J. Ferroelectrics, Vol. 100, Issue 1 https://doi.org/10.1080/00150198908007897	journal	December 1989
Total scattering and the pair distribution function in crystallography Keen, David A. Crystallography Reviews, Vol. 26, Issue 3 https://doi.org/10.1080/0889311X.2020.1797708	journal	July 2020
RMCProfile: reverse Monte Carlo for polycrystalline materials Tucker, Matthew G.; Keen, David A.; Dove, Martin T. Journal of Physics: Condensed Matter, Vol. 19, Issue 33 https://doi.org/10.1088/0953-8984/19/33/335218	journal	July 2007
Local structure in BaTi O 3 − BiSc O 3 dipole glasses Levin, I.; Krayzman, V.; Woicik, J. C. Physical Review B, Vol. 93, Issue 10 https://doi.org/10.1103/PhysRevB.93.104106	journal	March 2016
Emergence of Long-Range Order in BaTiO 3 from Local Symmetry-Breaking Distortions Senn, M. S.; Keen, D. A.; Lucas, T. C. A. Physical Review Letters, Vol. 116, Issue 20 https://doi.org/10.1103/PhysRevLett.116.207602	journal	May 2016
Current Understanding of Structure–Processing–Property Relationships in BaTiO ₃ –Bi( M )O ₃ Dielectrics Beuerlein, Michaela A.; Kumar, Nitish; Usher, Tedi‐Marie Journal of the American Ceramic Society, Vol. 99, Issue 9 https://doi.org/10.1111/jace.14472	journal	September 2016
Revisiting the temperature-dependent dielectric permittivity of Ba(Ti_1−x Zr_x )O₃ Liu, Laijun; Ren, Shaokai; Zhang, Jie Journal of the American Ceramic Society, Vol. 101, Issue 6 https://doi.org/10.1111/jace.15410	journal	January 2018
Ultrahigh–energy density lead-free dielectric films via polymorphic nanodomain design Pan, Hao; Li, Fei; Liu, Yao Science, Vol. 365, Issue 6453 https://doi.org/10.1126/science.aaw8109	journal	August 2019
Ultrahigh capacitive energy density in ion-bombarded relaxor ferroelectric films Kim, Jieun; Saremi, Sahar; Acharya, Megha Science, Vol. 369, Issue 6499 https://doi.org/10.1126/science.abb0631	journal	July 2020
Ultrahigh energy storage in superparaelectric relaxor ferroelectrics Pan, Hao; Lan, Shun; Xu, Shiqi Science, Vol. 374, Issue 6563 https://doi.org/10.1126/science.abi7687	journal	October 2021

Similar Records

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

Journal Article · Mon Aug 21 20:00:00 EDT 2023 · Journal of the American Chemical Society · OSTI ID:2404941

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

Journal Article · Thu May 18 20:00:00 EDT 2023 · Journal of the American Chemical Society · OSTI ID:2404847

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ceramics
chemical composition
cluster chemistry
insulators
polarization

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

Citation Formats

References (54)

Similar Records

Related Subjects