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The ferroelectric material usually exhibits temperature dependent spontaneouspolarization, known as pyroelectricity, which can be used to directly convertthermal energy to electricity from ambient low-grade waste heat. When utilizingthe structural phase transformations of the material, the conversion capabilitycan be magnified, consequently the device performance can be strongly boostedby orders of magnitude. However, common ferroelectric oxides suffer themechanical fatigue and functional degradation over cyclic phasetransformations, hindering widespread applications of the energy conversiondevice. In this paper, we investigate the mechanical and functionalreversibility of the material by lattice tuning and grain coarsening. Wediscover the lead-free compoundBa(Ce$_{0.005}$Zr$_{0.005}$)Ti$_{0.99}$O3-0.10(Ba$_{0.7}$Ca$_{0.3}$)TiO$_3$(BCZT-0.10BCT) satisfying the compatibility condition among all present phasesby its lattice parameters, making the phase transformations highly reversible.We demonstrated that the energy conversion device with the equiaxial coarsegrains exhibits exceptional fatigue-resistance, with stable pyroelectriccurrent output at 4$\mu$A/cm$^2$ over 3,000 energy conversion cycles. Our workopens a new way to fabricate high-performance material that advances thepyroelectric energy conversion for practical application in engineering.

Enhanced functional reversibility in lead-free ferroelectric material over long cycle pyroelectric energy conversion