Harnessing Multisite High-Entropy Architecture for Ultrahigh Energy Storage Multilayer Capacitors
High energy density lead-free dielectric capacitors play a pivotal role in state-of-the-art electrical and electronic systems. Nevertheless, the low energy storage capacities have persistently posed a significant impediment to the ongoing trend toward the miniaturization and integration of electronic devices. Here, we report an equimolar high-entropy relaxor ferroelectric multilayer capacitor that demonstrates exceptional energy storage performance by harnessing flexible multisite tetragonal tungsten bronze (TTB) high-entropy architecture. Our findings reveal that the equimolar high-entropy design results in NbO<sub>6</sub> octahedra distortion, disrupting long-range ferroelectric order while preserving strong off-center displacements along the polar axis at a local scale. This unique structure characteristic of high-entropy TTB not only enhances its relaxor feature, reducing hysteresis, but also maintains high polarizability under applied electric fields. Consequently, our high-entropy TTB multilayer ceramic capacitors achieved an unprecedented recoverable energy density of 20.2 J·cm<sup>-3</sup>, accompanied by a notably enhanced efficiency of 93.8%. This approach opens the door for the development of innovative functional ceramics and devices with prominent energy storage capability by designing flexible multisite high-entropy architecture.
Authors
- Tiantian Wu (ORCID: https://orcid.org/0000-0001-6048-2345)
- Fangfang Xu (ORCID: https://orcid.org/0000-0002-5570-4289)
- Cheng Yang (ORCID: https://orcid.org/0000-0002-2497-7014)
- Junhao Chu (ORCID: https://orcid.org/0000-0003-1867-9296)
- Haonan Peng (ORCID: https://orcid.org/0000-0002-3814-2237)
- Wanbiao Hu (ORCID: https://orcid.org/0000-0003-0180-9648)
- T. Honda (ORCID: https://orcid.org/0000-0003-4121-8957)
- Yonghong Chen (ORCID: https://orcid.org/0000-0001-9552-1308)
- Teng Lü (ORCID: https://orcid.org/0000-0002-7866-1859)
- Zhengqian Fu (ORCID: https://orcid.org/0000-0001-9402-9549)
- Zhen Liu (ORCID: https://orcid.org/0000-0003-4895-0948)
- Yun Liu (ORCID: https://orcid.org/0000-0002-5404-3909)
- Shujun J. Zhang (ORCID: https://orcid.org/0000-0001-6139-6887)
- Jiyang Xie
- Zhisheng Lin
- Zhichao Hong
- Genshui Wang (ORCID: https://orcid.org/0000-0002-5077-6574)
Institutions
- Tokyo Electron (Japan) (JP)
- Australian National University (AU)
- High Energy Accelerator Research Organization (JP)
- Yunnan University (CN)
- Chinese Academy of Sciences (CN)
- University of Wollongong (AU)
- The 180th Hospital of PLA (CN)
- Shanghai Institute of Technical Physics (CN)
- Advanced Materials and Devices (United States) (US)
- Superconducting Systems (United States) (US)
- Shanghai Institute of Ceramics (CN)
- University of Chinese Academy of Sciences (CN)
- Institute of Materials Structure Science (JP)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-10-29
- DOI
- https://doi.org/10.1021/jacs.5c12566
- Citations
- 1
- Primary Topic
- Ferroelectric and Piezoelectric Materials
- Type
- article
- Field-Weighted Citation Impact
- 0.52