Synergistically Optimizing Pressure-Driven Energy Conversion and Energy-Harvesting Application via Modulating an Antiferroelectric-to-Ferroelectric Overlap Zone in Antiferroelectric Ceramics

Dielectric ceramics with ultrahigh polarization and energy density are the core components used in next-generation pulse power generators based on explosive energy conversion. However, the low polarization of ferroelectric materials and high depolarized pressure hinder their development toward miniaturization, light weight, and integration, while antiferroelectric materials possessing larger nonlinear saturated polarization and rich phase structure are neglected in pulse power energy conversion. Here, an effective strategy of constructing antiferroelectric-to-ferroelectric overlap zone is achieved in binary system (1 – x)(Pb,La)(Zr,Ti)O3–xBa(Al1/2Nb1/2)O3 antiferroelectric ceramics to realize an excellent polarization of 41 μC/cm2 and a large depolarization efficiency of >99% under 150 MPa as well as a record high energy harvesting density of 2.5 J/cm3 under 400 MPa. The excellent comprehensive energy conversion and energy harvesting performance is mainly attributed to the strategy of antiferroelectric-to-ferroelectric overlap zone and improved microdomain density, at which orthorhombic-to-rhombohedral structure evolution is confirmed by transmission electron microscopy, piezo-response force microscopy, and Raman spectrum, resulting in substantially enhanced remanent polarization compared to ferroelectric ceramics. Besides, excellent temperature stability (∼180 °C) and optimized depolarization pressure also support that this binary system is a candidate for energy conversion and energy harvesting application. This work demonstrates that antiferroelectric-to-ferroelectric overlap based on antiferroelectric materials is an excellent strategy to develop dielectric materials with excellent depolarized polarization and energy harvesting density for energy conversion and harvesting.