Bias-field-regulated phase evolution and pyroelectric energy harvesting in antiferroelectric Pb(Mg0.9W0.9Sc0.1Ta0.1)0.5O3 multilayer ceramic capacitors

Ferroelectric and antiferroelectric materials exhibit polarization changes in response to temperature and electric field, making them promising for pyroelectric energy harvesting and solid-state refrigeration. B-site complex perovskites Pb(B′0.5B″0.5)O3 have attracted considerable attention in energy storage and conversion owing to their flexible B-site tunability and rich phase-transition behavior. In this work, we report antiferroelectric Pb(Mg0.9W0.9Sc0.1Ta0.1)0.5O3 multilayer ceramic capacitors with dielectric and pyroelectric properties that are strongly dependent on the direct-current (DC)-bias-field. The incorporation of Sc3+ and Ta5+ into the B-site lattice creates a chemically disordered local environment, which facilitates field-induced polarization and phase transition. The DC-bias dielectric spectra reveal that the applied electric field regulates the relative stability of the antiferroelectric, field-induced ferroelectric, and paraelectric phases. Consequently, pronounced positive and negative pyroelectric responses are achieved. More importantly, the Olsen cycle delivers a high pyroelectric energy-harvesting density of 2.33 J cm−3 over −20 to 50 °C, while maintaining a stable output of approximately 2.3 J cm−3 over a broad initial temperature range from −50 to −10 °C. These results demonstrate that combining B-site compositional regulation with a multilayer architecture provides an effective route for developing antiferroelectric materials for high-energy-density thermal energy harvesting.