4.8 Article

Enhancing Comprehensive Energy Storage Properties in Tungsten Bronze Sr0.53Ba0.47Nb2O6-Based Lead-free Ceramics by B-Site Doping and Relaxor Tuning

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c06889

Keywords

tungsten bronze structure; energy storage; Sb doping in B-sites; relaxor; charge-discharge; dielectric capacitors

Funding

  1. National Natural Science Foundation of China [52172125, 51701149, 11272248]
  2. CSS project [YK2015-0602006]
  3. Major Science and Technology Project of Ordos City [2021EEDSCXQDFZ014]
  4. Ordos Science and Technol-ogy Program, Shaanxi Province Science and Technology Innovation Team Project [2020TD-001]
  5. Fundamen-tal Research Funds for the Central Universities
  6. World-Class Universities
  7. Characteristic Development Guidance Funds for the Central Universities

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In this study, a lead-free Sb-modified tungsten bronze ceramic was designed and fabricated to enhance the relaxor characteristics. The incorporation of Sb induced structural distortion and order-disorder distribution, resulting in improved breakdown strength and remarkable energy storage performance at high power and current density.
Dielectric ceramics with relaxor characteristics are promising candidates to meet the demand for capacitors of next-generation pulse devices. Herein, a lead-free Sb-modified (Sr0.515Ba0.47Gd0.01) (Nb1.9-xTa0.1Sbx)O-6 (SBGNT-based) tungsten bronze ceramic is designed and fabricated for high-density energy storage capacitors. Using a B-site engineering strategy to enhance the relaxor characteristics, Sb incorporation could induce the structural distortion of the polar unit BO6 and order-disorder distribution of B-site cations as well as the modulation of polarization in the SBGNT-based tungsten bronze ceramic. More importantly, benefiting from the effective inhibition of abnormal growth of non-equiaxed grains, Sb introduction into SBGNT-based ceramics could effectively suppress the conductivity and leakage current density, enhancing the breakdown strength, as proved by the electrical impedance spectra. Consequently, a remarkable comprehensive performance via balancing recoverable energy density (similar to 3.26 J/cm(3)) and efficiency (91.95%) is realized simultaneously at 380 kV/cm, which surpasses that of the pristine sample without the Sb dopant (2.75 J/cm(3) and 80.5%, respectively). The corresponding ceramics display superior stability in terms of fatigue (10(5) cycles), frequency (1 similar to 200 Hz), and temperature (20 similar to 140 degrees C). Further charge-discharge analysis indicates that a high power density (89.57 MW/cm(3)) and an impressive current density (1194.27 A/cm(2)) at 150 kV/cm are achieved simultaneously. All of the results demonstrate that the tungsten bronze relaxors are indeed gratifying lead-free candidate materials for dielectric energy storage applications.

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