Excellent hardening effect in lead-free piezoceramics by embedding local Cu-doped defect dipoles in phase boundary engineering

Piezoceramics for high-power applications require both high piezoelectric coefficient (d<sub>33</sub>) and mechanical quality factor (Q<sub>m</sub>). However, the trade-off between them poses a significant challenge in achieving high values simultaneously, which is more prominent in lead-free piezoceramics. Here, we propose a new strategy, local Cu-acceptor defect dipoles embedded orthorhombic-tetragonal phase boundary engineering (O-T PBE), to balance d<sub>33</sub> and Q<sub>m</sub> in potassium sodium niobate piezoceramics. This is validated in 0.95(K<sub>0.48</sub>Na<sub>0.52</sub>)NbO<sub>3</sub>-0.05(Bi<sub>0.5</sub>Na<sub>0.5</sub>)HfO<sub>3</sub>-0.2%molFe<sub>2</sub>O<sub>3</sub>-xmol%CuO ceramics. Our strategy simultaneously maintains the O-T PBE and introduces local dimeric <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow><mml:mrow><mml:mo>(</mml:mo> <mml:mrow> <mml:msubsup><mml:mrow><mml:mi>C</mml:mi> <mml:mi>u</mml:mi></mml:mrow> <mml:mrow><mml:mi>N</mml:mi> <mml:mi>b</mml:mi></mml:mrow> <mml:mrow><mml:mo>″</mml:mo> <mml:mo>'</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:mrow> <mml:mo>)</mml:mo></mml:mrow> </mml:mrow> <mml:mrow><mml:mo>'</mml:mo></mml:mrow> </mml:msup> </mml:math> and trimeric <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow> <mml:mfenced> <mml:mrow> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>C</mml:mi> <mml:mi>u</mml:mi></mml:mrow> <mml:mrow><mml:mi>N</mml:mi> <mml:mi>b</mml:mi></mml:mrow> <mml:mrow><mml:mo>″</mml:mo> <mml:mo>'</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:mrow> </mml:mfenced> </mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> defects. The dimeric defects form defect dipole polarization that pins domain wall motion, while the trimeric ones introduce the local structural heterogeneity that leads to nano-scale multi-phase coexistence and abundant nano-domains. Encouragingly, for the Cu-doped sample with x = 1, Q<sub>m</sub> increases by a factor of 4, but d<sub>33</sub> only decreases by 1/5 (i.e., achieving a d<sub>33</sub> of 340 pC/N and a Q<sub>m</sub> of 256). Our research provides a new paradigm for balancing d<sub>33</sub> and Q<sub>m</sub> in lead-free piezoceramics, which holds promise for high-power applications.

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Journal
Nature Communications
Published
2025-03-25
DOI
https://doi.org/10.1038/s41467-025-58269-5
Citations
20
Primary Topic
Ferroelectric and Piezoelectric Materials
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article
Field-Weighted Citation Impact
9.84
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article

Excellent hardening effect in lead-free piezoceramics by embedding local Cu-doped defect dipoles in phase boundary engineering

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20 citations
Nature Communications
Ferroelectric and Piezoelectric Materials
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article

Excellent hardening effect in lead-free piezoceramics by embedding local Cu-doped defect dipoles in phase boundary engineering

Jiagang Wu, Chao Wu, Xinyue Qiu, Xiang Lv, Xixiang Zhang, Zhi Tan, Yinchang Ma, Junwei Zhang, Chen Liu, Daniel Q. Tan, Zhipeng Wang, Ruihong Liang, Shiyang Wei
article en
20 citations

Abstract

Piezoceramics for high-power applications require both high piezoelectric coefficient (d<sub>33</sub>) and mechanical quality factor (Q<sub>m</sub>). However, the trade-off between them poses a significant challenge in achieving high values simultaneously, which is more prominent in lead-free piezoceramics. Here, we propose a new strategy, local Cu-acceptor defect dipoles embedded orthorhombic-tetragonal phase boundary engineering (O-T PBE), to balance d<sub>33</sub> and Q<sub>m</sub> in potassium sodium niobate piezoceramics. This is validated in 0.95(K<sub>0.48</sub>Na<sub>0.52</sub>)NbO<sub>3</sub>-0.05(Bi<sub>0.5</sub>Na<sub>0.5</sub>)HfO<sub>3</sub>-0.2%molFe<sub>2</sub>O<sub>3</sub>-xmol%CuO ceramics. Our strategy simultaneously maintains the O-T PBE and introduces local dimeric <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow><mml:mrow><mml:mo>(</mml:mo> <mml:mrow> <mml:msubsup><mml:mrow><mml:mi>C</mml:mi> <mml:mi>u</mml:mi></mml:mrow> <mml:mrow><mml:mi>N</mml:mi> <mml:mi>b</mml:mi></mml:mrow> <mml:mrow><mml:mo>″</mml:mo> <mml:mo>'</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:mrow> <mml:mo>)</mml:mo></mml:mrow> </mml:mrow> <mml:mrow><mml:mo>'</mml:mo></mml:mrow> </mml:msup> </mml:math> and trimeric <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow> <mml:mfenced> <mml:mrow> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>C</mml:mi> <mml:mi>u</mml:mi></mml:mrow> <mml:mrow><mml:mi>N</mml:mi> <mml:mi>b</mml:mi></mml:mrow> <mml:mrow><mml:mo>″</mml:mo> <mml:mo>'</mml:mo></mml:mrow> </mml:msubsup> <mml:mo>-</mml:mo> <mml:msubsup><mml:mrow><mml:mi>V</mml:mi></mml:mrow> <mml:mrow><mml:mi>O</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo> <mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:mrow> </mml:mfenced> </mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> defects. The dimeric defects form defect dipole polarization that pins domain wall motion, while the trimeric ones introduce the local structural heterogeneity that leads to nano-scale multi-phase coexistence and abundant nano-domains. Encouragingly, for the Cu-doped sample with x = 1, Q<sub>m</sub> increases by a factor of 4, but d<sub>33</sub> only decreases by 1/5 (i.e., achieving a d<sub>33</sub> of 340 pC/N and a Q<sub>m</sub> of 256). Our research provides a new paradigm for balancing d<sub>33</sub> and Q<sub>m</sub> in lead-free piezoceramics, which holds promise for high-power applications.

Nature CommunicationsVol. 16(1)
Xidian University (CN), Chinese Academy of Sciences (CN), Sichuan University (CN), Guangdong Technion-Israel Institute of Technology (CN), Shanghai Institute of Ceramics (CN), King Abdullah University of Science and Technology (SA), Lanzhou University (CN)
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