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Mn掺杂对KNbO3和(K0.5Na0.5)NbO3无铅钙钛矿陶瓷铁电压电性能的影响

徐泽 娄路遥 赵纯林 汤浩正 刘亦轩 李昭 齐晓梅 张波萍 李敬锋 龚文 王轲

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Mn掺杂对KNbO3和(K0.5Na0.5)NbO3无铅钙钛矿陶瓷铁电压电性能的影响

徐泽, 娄路遥, 赵纯林, 汤浩正, 刘亦轩, 李昭, 齐晓梅, 张波萍, 李敬锋, 龚文, 王轲

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
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  • (K0.5Na0.5)NbO3基无铅压电陶瓷具有出色的综合铁电压电性能, 已经初步满足了部分实际应用场景的需求. 近期的研究发现, 某些元素的掺杂对优化(K0.5Na0.5)NbO3基陶瓷的机电耦合性能起着至关重要的作用. 本文将MnO2添加到KNbO3和(K0.5Na0.5)NbO3两种压电陶瓷中, 对比研究了Mn掺杂对两种陶瓷微观结构和宏观电学性能的不同影响, 分析了造成这些差异的微观物理机理. 实验结果表明, 掺杂后的两种陶瓷中均存在Mn2+. Mn掺杂会使KNbO3陶瓷的铁电畴尺寸减小、居里温度降低、拉曼光谱中的振动峰宽化、相变过程变得弥散, 并呈现出束腰电滞回线和可回复的双极场致应变曲线; 在(K0.5Na0.5)NbO3陶瓷中掺杂Mn后, 其性能变化却显著不同, 陶瓷的铁电畴尺寸无明显变化、居里温度未发生变化、拉曼光谱中的振动峰未发生宽化, 呈现出饱和的矩形电滞回线和不可回复的双极场致应变曲线. 这可能是因为, (K0.5Na0.5)NbO3陶瓷相比KNbO3陶瓷具有更大的离子无序度和晶格畸变, 从而使得Mn掺杂所产生的影响相对减小.
    Potassium sodium niobate ((K0.5Na0.5)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 (K0.5Na0.5)NbO3-based piezoelectric ceramics. In this paper, MnO2 is doped into potassium niobate (KNbO3) and (K0.5Na0.5)NbO3 piezoelectric ceramics prepared by the conventional solid-state reaction method. The influences of doped Mn cation on KNbO3 and (K0.5Na0.5)NbO3 piezoelectric ceramics including microstructure and macroscopic electrical properties are systematically investigated. The doping effects of Mn cation on the KNbO3 and (K0.5Na0.5)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 (K0.5Na0.5)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 (K0.5Na0.5)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 (K0.5Na0.5)NbO3 piezoelectric ceramics. The results will serve as an important reference for preparing high-performance (K0.5Na0.5)NbO3-based piezoelectric ceramics via chemical doping.
      通信作者: 张波萍, bpzhang@ustb.edu.cn ; 龚文, gongwen@tsinghua-zj.edu.cn ; 王轲, wang-ke@tsinghua.edu.cn
    • 基金项目: 国家级-国家自然科学基金优秀青年科学基金项目(51822206)
      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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  • 图 1  KN, KN-Mn, KNN和KNN-Mn陶瓷XRD图谱

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

    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

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

    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

    Fig. 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).

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

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

    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

    Fig. 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.

    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

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

    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

    Fig. 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.

    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–1Relative density/%kpQmθmax/(°)tanδεr (1 kHz)
    KN9092.00.26177660.042576
    KN-Mn8395.10.27185770.015526
    KNN11594.90.2985640.060393
    KNN-Mn10994.30.32330830.024355
    下载: 导出CSV
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    吴金根, 高翔宇, 陈建国, 王春明, 张树君, 董蜀湘 2018 物理学报 67 207701Google Scholar

    Wu J G, Gao X Y, Chen J G, Wang C M, Zhang S J, Dong S X 2018 Acta Phys. Sin. 67 207701Google Scholar

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    刘涛, 丁爱丽, 何夕云, 郑鑫森, 仇萍荪, 程文秀 2007 无机材料学报 22 469Google Scholar

    Liu T, Ding A L, He X Y, Zheng X S, Qiu P S, Cheng W X 2007 J. Inorg. Mater. 22 469Google Scholar

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    Saito Y, Takao H, Tani T, Nonoyama T, Takatori K, Homma T, Nagaya T, Nakamura M 2004 Nature 432 84Google Scholar

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    Koruza J, Bell A J, Frömling T, Webber K G, Wang K, Rödel J 2018 J. Materiomics 4 13Google Scholar

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出版历程
  • 收稿日期:  2020-02-24
  • 修回日期:  2020-03-09
  • 刊出日期:  2020-06-20

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