Large Energy Capacitive High-Entropy Lead-Free Ferroelectrics

Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market. Here, an ultrahigh energy storage density of ~ 13.8 J cm(−3) and a large efficiency of ~ 82.4% are achieved in high-entropy lead-free relaxor ferroelectrics by increasing configuration entropy, named high-entropy strategy, realizing nearly ten times growth of energy storage density compared with low-entropy material. Evolution of energy storage performance and domain structure with increasing configuration entropy is systematically revealed for the first time. The achievement of excellent energy storage properties should be attributed to the enhanced random field, decreased nanodomain size, strong multiple local distortions, and improved breakdown field. Furthermore, the excellent frequency and fatigue stability as well as charge/discharge properties with superior thermal stability are also realized. The significantly enhanced comprehensive energy storage performance by increasing configuration entropy demonstrates that high entropy is an effective but convenient strategy to design new high-performance dielectrics, promoting the development of advanced capacitors [Image: see text]. SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01036-2.