Environment protection and human health concern is the driving force to eliminate the lead from commercial piezoelectric materials. In 2004, Saito et al. [ Saito et al., Nature , 2004 , 432 , 84 . ] developed an alkali niobate-based perovskite solid solution with a peak piezoelectric constant d33 of 416 pC/N when prepared in the textured polycrystalline form, intriguing the enthusiasm of developing high-performance lead-free piezoceramics. Although much attention has been paid on the alkali niobate-based system in the past ten years, no significant breakthrough in its d33 has yet been attained. Here, we report an alkali niobate-based lead-free piezoceramic with the largest d33 of ∼490 pC/N ever reported so far using conventional solid-state method. In addition, this material system also exhibits excellent integrated performance with d33∼390-490 pC/N and TC∼217-304 °C by optimizing the compositions. This giant d33 of the alkali niobate-based lead-free piezoceramics is ascribed to not only the construction of a new rhombohedral-tetragonal phase boundary but also enhanced dielectric and ferroelectric properties. Our finding may pave the way for "lead-free at last".

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The structural origin of enhanced piezoelectric performance and stability in KNN-based ceramics can be attributed to the hierarchical nanodomain architecture with phase coexistence.

For potassium-sodium niobate, poor piezoelectric properties always perplex most researchers, and then it becomes important to attain a giant piezoelectricity. Here we reported a giant piezoelectric constant in (1-x)(K0.48Na0.52)(Nb0.95Sb0.05)O3-xBi0.5Ag0.5ZrO3 lead-free ceramics. The rhombohedral-tetragonal phase boundary was shown in the ceramics with 0.04

The obvious conflicts between large piezoelectricity and high strain could be solved by developing new phase boundaries in potassium–sodium niobate materials.

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The inherent disadvantage of lead-free potassium sodium niobate (KNN)based ceramics is the severe temperature instability of piezoelectric charge coefficient (d 33 ) caused by the polymorphic phase boundary. Herein, a new concept of structural gradient is proposed by designing compositionally graded multilayer composites with multiple successive phase transitions, to solve the challenge of the inferior temperature stability. The structural gradient ceramics exhibit a superior temperature reliability (d 33 remains almost unchanged in the temperature range of 25-100 °C), far outperforming the previously reported KNN counterparts with d 33 variation above 27% over the same temperature range. The synergistic contribution of the continuous phase transition, the strain gradient, and the complementary effect of each constituent layer leads to the excellent temperature stability, which is also confirmed by phase-field simulation. These findings are expected to provide a new paradigm for functional material design with outstanding temperature stability.

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