Effect of manganese doping on ferroelectric and piezoelectric properties of KNbO3 and (K0.5Na0.5)NbO3 lead-free ceramics

Xu Ze; Lou Lu-Yao; Zhao Chun-Lin; Tang Hao-Cheng; Liu Yi-Xuan; Li Zhao; Qi Xiao-Mei; Zhang Bo-Ping; Li Jing-Feng; Gong Wen; Wang Ke

doi:10.7498/aps.69.20200277

Abstract

Potassium sodium niobate ((K_0.5Na_0.5)NbO₃)-based lead-free piezoelectric ceramics are excellent ferroelectric materials and have been demonstrated to have many practical applications. Recent studies have revealed that chemical doping plays a crucial role in optimizing the electromechanical coupling properties of (K_0.5Na_0.5)NbO₃-based piezoelectric ceramics. In this paper, MnO₂ is doped into potassium niobate (KNbO₃) and (K_0.5Na_0.5)NbO₃ piezoelectric ceramics prepared by the conventional solid-state reaction method. The influences of doped Mn cation on KNbO₃ and (K_0.5Na_0.5)NbO₃ piezoelectric ceramics including microstructure and macroscopic electrical properties are systematically investigated. The doping effects of Mn cation on the KNbO₃ and (K_0.5Na_0.5)NbO₃ piezoelectric ceramics are significantly different from each other. For the Mn-doped KNbO₃ piezoelectric ceramics, the sizes of ferroelectric domains are reduced. Meanwhile, the diffused orthorhombic-tetragonal phase transition is observed, which is accompanied by reducing dielectric loss and Curie temperature, and broadening vibration peaks in Raman spectrum. It is known that the oxygen vacancy can be formed to compensate for the charges created by the acceptor doping of Mn into the B site of perovskite, and thus forming a defect dipole with the acceptor center. From the ferroelectric measurement, a double hysteresis loop (P-E curve) and a recoverable electric-field-induced strain due to the formation of defect dipole are observed. On the contrary, for the Mn-doped (K_0.5Na_0.5)NbO₃ piezoelectric ceramics, the sizes of ferroelectric domains are not reduced. Meanwhile, the Curie temperature and vibration peaks in Raman spectrum are not changed. A rectangular hysteresis loop (P-E curve) and an unrecoverable electric-field-induced strain are observed in the ferroelectric measurement. The difference between these systems might originate from the greater ionic disorder and lattice distortion in (K_0.5Na_0.5)NbO₃ piezoelectric ceramics. The difference in ionic radius between Na⁺ and K⁺ can affect the migration and distribution of oxygen vacancies, which makes it difficult to form stable defect dipoles in the Mn-doped (K_0.5Na_0.5)NbO₃ piezoelectric ceramics. The results will serve as an important reference for preparing high-performance (K_0.5Na_0.5)NbO₃-based piezoelectric ceramics via chemical doping.

Keywords:

Authors and contacts

1.
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
2.
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China
3.
Advanced Ceramic Materials & Devices Research Center, Yangtze Delta Region Institute of Tsinghua University, Zhejiang, Jiaxing 314006, China

Corresponding author: Zhang Bo-Ping, bpzhang@ustb.edu.cn ; Gong Wen, gongwen@tsinghua-zj.edu.cn ; Wang Ke, wang-ke@tsinghua.edu.cn

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Cited By

图 1 KN, KN-Mn, KNN和KNN-Mn陶瓷XRD图谱

Figure 1. XRD patterns of KN, KN-Mn, KNN, and KNN-Mn ceramics.

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图 2 经热腐蚀的表面SEM形貌图　(a) KN陶瓷; (b) KN-Mn陶瓷; (c) KNN陶瓷; (d) KNN-Mn陶瓷

Figure 2. SEM images of the thermally etched surface: (a) KN, (b) KN-Mn, (c) KNN, (d) KNN-Mn ceramics.

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图 3 (a)−(d)纵向压电响应模式(VPFM)、(e)−(h)横向压电响应模式(LPFM)下测试的未极化KN, KN-Mn, KNN, KNN-Mn陶瓷的铁电畴形貌图

Figure 3. Domain images of unpoled KN, KN-Mn, KNN, KNN-Mn ceramics tested in (a)−(d) vertical piezoresponse force microscopy (VPFM) and (e)−(h) lateral piezoresponse force microscopy (LPFM).

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图 4 X波段ESR谱图　(a) KN-Mn陶瓷; (b) KNN-Mn陶瓷

Figure 4. X-band ESR spectra: (a) KN-Mn ceramics; (b) KNN-Mn ceramics.

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图 5 (a) KN, KN-Mn, KNN和KNN-Mn陶瓷的拉曼散射光谱图; (b) NbO₆八面体三种内部振动模的示意图, 其中V₁和V₂为拉伸振动模、V₅为弯曲振动模

Figure 5. (a) Raman spectra of KN, KN-Mn, KNN, KNN-Mn ceramics; (b) schematic illustration of three internal vibrational modes of NbO₆ octahedra. V₁ and V₂ are stretching modes, and V₅ is bending mode.

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图 6 陶瓷的相对介电常数和介电损耗随温度的变化　(a) KN, KN-Mn陶瓷; (b) KNN, KNN-Mn陶瓷

Figure 6. Temperature dependence of dielectric permittivity and dielectric loss of unpoled for ceramics: (a) KN, KN-Mn ceramics; (b) KNN, KNN-Mn ceramics.

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图 7 (a) KN, (b) KN-Mn, (e) KNN, (f) KNN-Mn陶瓷的电滞回线; (c) KN, (d) KN-Mn, (g) KNN, (h) KNN-Mn陶瓷的双极场致应变曲线

Figure 7. Polarization hysteresis loops of (a) KN, (b) KN-Mn, (e) KNN, (f) KNN-Mn ceramics; bipolar piezoelectric strain curves of (c) KN, (d) KN-Mn, (g) KNN, (h) KNN-Mn ceramics.

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表 1 KN, KN-Mn, KNN和KNN-Mn陶瓷的相对密度、压电性能和介电性能

Table 1. Relative density, piezoelectric and dielectric properties of KN, KN-Mn, KNN, and KNN-Mn ceramics.

d₃₃/pC·N^–1 Relative density/% k_p Q_m θ_max/(°) tanδ ε_r (1 kHz)

KN 90 92.0 0.26 177 66 0.042 576
KN-Mn 83 95.1 0.27 185 77 0.015 526
KNN 115 94.9 0.29 85 64 0.060 393
KNN-Mn 109 94.3 0.32 330 83 0.024 355

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map

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Vol. 69, Issue 12 - 2020-06-20

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Effect of manganese doping on ferroelectric and piezoelectric properties of KNbO₃ and (K_0.5Na_0.5)NbO₃ lead-free ceramics