Gaur Anand P S, Choudhary Renu, Liu Binzhi, Mudryk Yaroslav, Johnson Duane D, Cui Jun, Tan Xiaoli
Department of Materials Science and Engineering, Iowa State University, Ames, IA, 50011, USA.
U.S. DOE Ames National Laboratory, Ames, IA, 50011, USA.
Adv Mater. 2024 Aug;36(31):e2312856. doi: 10.1002/adma.202312856. Epub 2024 Jun 2.
Antiferroelectric ceramics, via the electric-field-induced antiferroelectric (AFE)-ferroelectric (FE) phase transitions, show great promise for high-energy-density capacitors. Yet, currently, only 70-80% energy release is found during a charge-discharge cycle. Here, for PbZrO-based oxides, geometric nonlinear theory of martensitic phase transitions is applied (first used to guide supercompatible shape-memory alloys) to predict the reversibility of the AFE-FE transition by using density-functional theory to assess AFE/FE interfacial lattice-mismatch strain that assures ultralow electric hysteresis and extended fatigue lifetime. A good correlation of mismatch strain with electric hysteresis, hence, with energy efficiency of AFE capacitors is observed. Guided by theory, high-throughput material search is conducted and AFE compositions with a near-perfect charge-discharge energy efficiency (98.2%), i.e., near-zero hysteresis are discovered. And the fatigue life of the capacitor reaches 79.5 million charge-discharge cycles, a factor of 80 enhancement over AFE ceramics with large electric hysteresis.
反铁电陶瓷通过电场诱导的反铁电（AFE）-铁电（FE）相变，在高能量密度电容器方面展现出巨大潜力。然而，目前在充放电循环中仅发现70 - 80%的能量释放。在此，对于基于PbZrO的氧化物，应用马氏体相变的几何非线性理论（首次用于指导超相容性形状记忆合金），通过使用密度泛函理论评估AFE/FE界面晶格失配应变来预测AFE - FE转变的可逆性，该应变确保了超低的电滞和延长的疲劳寿命。观察到失配应变与电滞之间存在良好的相关性，进而与AFE电容器的能量效率存在良好相关性。在理论指导下，进行了高通量材料搜索，发现了具有近乎完美的充放电能量效率（98.2%），即近乎零滞后的AFE成分。并且该电容器的疲劳寿命达到7950万次充放电循环，比具有大电滞的AFE陶瓷提高了80倍。
