AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
PDF (1.7 MB)
Submit Manuscript AI Chat Paper
Show Outline
Show full outline
Hide outline
Show full outline
Hide outline
Research Article | Open Access

Optimizing energy harvesting performance by tailoring ferroelectric/relaxor behavior in KNN-based piezoceramics

Yu HUANa( )Xinjian WANGaWenyu YANGaLimin HOUaMupeng ZHENGb( )Tao WEIaXiaohui WANGc( )
School of Materials Science and Engineering, University of Jinan, Jinan 250022, China
Key Laboratory of Advanced Functional Materials, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
Show Author Information


Piezoelectric energy harvesters (PEHs) fabricated using piezoceramics could convert directly the mechanical vibration energy in the environment into electrical energy. The high piezoelectric charge coefficient (d33) and large piezoelectric voltage coefficient (g33) are key factors for the high-performance PEHs. However, high d33 and large g33 are difficult to simultaneously achieve with respect to g33=d33/(ε0εr) and d33=2Qε0εrPr. Herein, the energy harvesting performance is optimized by tailoring the CaZrO3 content in (0.964-x)(K0.52Na0.48)(Nb0.96Sb0.04)O3 -0.036(Bi0.5Na0.5)ZrO3-xCaZrO3 ceramics. First, the doping CaZrO3 could enhance the dielectric relaxation due to the compositional fluctuation and structural disordering, and thus reduce the domain size to ~30 nm for x = 0.006 sample. The nanodomains switch easily to external electric field, resulting in large polarization. Second, the rhombohedral-orthorhombic-tetragonal phases coexist in x = 0.006 sample, which reduces the polarization anisotropy and thus improves the piezoelectric properties. The multiphase coexistence structures and miniaturized domains contribute to the excellent piezoelectric properties of d33 (354 pC/N). Furthermore, the dielectric relative permittivity (εr) reduces monotonously as the CaZrO3 content increases due to the relatively low ion polarizability of Ca2+ and Zr4+. As a result, the optimized energy conversion coefficient (d33 × g33, 5508 × 10-15 m2/N) is achieved for x = 0.006 sample. Most importantly, the assembled PEH with the optimal specimen shows the excellent output power (~48 μW) and lights up 45 red commercial light-emitting diodes (LEDs). This work demonstrates that tailoring ferroelectric/relaxor behavior in (K,Na)NbO3-based piezoelectric ceramics could effectively enhance the electrical output of PEHs.

Electronic Supplementary Material

Download File(s)
s40145-022-0587-1_ESM.pdf (1.5 MB)


Rödel J, Webber KG, Dittmer R, et al. Transferring lead- free piezoelectric ceramics into application. J Eur Ceram Soc 2015, 35: 1659-1681.
Huan Y, Chen SX, Zeng R, et al. Intrinsic effects of Ruddlesden-Popper-based bifunctional catalysts for high- temperature oxygen reduction and evolution. Adv Energy Mater 2019, 9: 1901573.
Zhang M, Yang HB, Yu YW, et al. Energy storage performance of K0.5Na0.5NbO3-based ceramics modified by Bi(Zn2/3(Nb0.85Ta0.15)1/3)O3. Chem Eng J 2021, 425: 131465.
Siang J, Lim MH, Salman Leong M. Review of vibration- based energy harvesting technology: Mechanism and architectural approach. Int J Energy Res 2018, 42: 1866-1893.
Wang ZL, Song JH. Piezoelectric nanogenerators based on zinc oxide nanowire arrays. Science 2006, 312: 242-246.
Yan XD, Zheng MP, Gao X, et al. High-performance lead- free ferroelectric BZT-BCT and its application in energy fields. J Mater Chem C 2020, 8: 13530-13556.
Lin Y, Li D, Zhang M, et al. Excellent energy-storage properties achieved in BaTiO3-based lead-free relaxor ferroelectric ceramics via domain engineering on the nanoscale. ACS Appl Mater Interfaces 2019, 11: 36824-36830.
Zhang M, Yang HB, Lin Y, et al. Significant increase in comprehensive energy storage performance of potassium sodium niobate-based ceramics via synergistic optimization strategy. Energy Storage Mater 2022, 45: 861-868.
Khan A, Abas Z, Soo Kim H, et al. Piezoelectric thin films: An integrated review of transducers and energy harvesting. Smart Mater Struct 2016, 25: 053002.
Swain AB, Dinesh Kumar S, Subramanian V, et al. Engineering resonance modes for enhanced magnetoelectric coupling in bilayer laminate composites for energy harvesting applications. Phys Rev Appl 2020, 13: 024026.
Manjón-Sanz AM, Dolgos MR. Applications of piezoelectrics: Old and new. Chem Mater 2018, 30: 8718-8726.
Xu J, Lu QL, Lin JF, et al. Enhanced ferro-/piezoelectric properties of tape-casting-derived Er3+-doped Ba0.85Ca0.15Ti0.9Zr0.1O3 optoelectronic thick films. J Adv Ceram 2020, 9: 693-702.
Saito Y, Takao H, Tani T, et al. Lead-free piezoceramics. Nature 2004, 432: 84-87.
Fan Y, Wang ZX, Huan Y, et al. Enhanced thermal and cycling reliabilities in (K,Na)(Nb,Sb)O3-CaZrO3-(Bi,Na)HfO3 ceramics. J Adv Ceram 2020, 9: 349-359.
Tao H, Wu HJ, Liu Y, et al. Ultrahigh performance in lead-free piezoceramics utilizing a relaxor slush polar state with multiphase coexistence. J Am Chem Soc 2019, 141: 13987-13994.
Islam RA, Priya S. Realization of high-energy density polycrystalline piezoelectric ceramics. Appl Phys Lett 2006, 88: 032903.
Zhang SJ, Alberta EF, Eitel RE, et al. Elastic, piezoelectric, and dielectric characterization of modified BiScO3-PbTiO3 ceramics. IEEE Trans Ultrason Ferroelectr Freq Control 2005, 52: 2131-2139.
Priya S. Criterion for material selection in design of bulk piezoelectric energy harvesters. IEEE Trans Ultrason Ferroelectr Freq Control 2010, 57: 2610-2612.
Wang K, Li JF. Domain engineering of lead-free Li-modified (K,Na)NbO3 polycrystals with highly enhanced piezoelectricity. Adv Funct Mater 2010, 20: 1924-1929.
Zhang N, Zheng T, Li N, et al. Symmetry of the underlying lattice in (K,Na)NbO3-based relaxor ferroelectrics with large electromechanical response. ACS Appl Mater Interfaces 2021, 13: 7461-7469.
Huan Y, Wang XH, Li LT. Displacement of Ta-O bonds near polymorphic phase transition in Li-, Ta-, and Sb- modified (K,Na)NbO3 ceramics. Appl Phys Lett 2014, 104: 242905.
Huan Y, Wang XH, Shen ZB, et al. Nanodomains in KNN-based lead-free piezoelectric ceramics: Origin of strong piezoelectric properties. J Am Ceram Soc 2014, 97: 700-703.
Huan Y, Wei T, Wang XZ, et al. Achieving ultrahigh energy storage efficiency in local-composition gradient-structured ferroelectric ceramics. Chem Eng J 2021, 425: 129506.
Yan XD, Zheng MP, Hou YD, et al. Composition-driven phase boundary and its energy harvesting performance of BCZT lead-free piezoelectric ceramic. J Eur Ceram Soc 2017, 37: 2583-2589.
Ma J, Wu J, Wu B, et al. Advances in the modification of the contradictory relationship between piezoelectricity and Curie temperature: Simultaneous realization of large piezoelectricity and high Curie temperature in potassium sodium niobate-based ferroelectrics. J Mater Chem C 2020, 8: 9506-9510.
Deng AP, Wu JG. Effects of rare-earth dopants on phase structure and electrical properties of lead-free bismuth sodium titanate-based ceramics. J Materiomics 2020, 6: 286-292.
Xing J, Tan Z, Jiang LM, et al. Phase transition and piezoelectric properties of Nd3+ doped nonstoichiometric (K,Na)NbO3-based lead free ceramics. Appl Phys Lett 2017, 110: 022905.
Wang DW, Hussain F, Khesro A, et al. Composition and temperature dependence of structure and piezoelectricity in (1-x)(K1-yNay)NbO3-x(Bi1/2Na1/2)ZrO3 lead-free ceramics. J Am Ceram Soc 2017, 100: 627-637.
Lv X, Zhu JG, Xiao DQ, et al. Emerging new phase boundary in potassium sodium-niobate based ceramics. Chem Soc Rev 2020, 49: 671-707.
Bokov AA, Ye ZG. Recent progress in relaxor ferroelectrics with perovskite structure. J Mater Sci 2006, 41: 31-52.
Hong CS, Chu SY, Tsai CC, et al. Effects of lanthanum dopants on the Curie-Weiss and the local order behaviors for Pb1-xLax(Fe2/3W1/3)0.7Ti0.3O3 relaxor ferroelectrics. Mater Res Bull 2013, 48: 200-206.
Kutnjak Z, Petzelt J, Blinc R. The giant electromechanical response in ferroelectric relaxors as a critical phenomenon. Nature 2006, 441: 956-959.
Qin YL, Zhang JL, Yao WZ, et al. Domain configuration and thermal stability of (K0.48Na0.52)(Nb0.96Sb0.04)O3- Bi0.50(Na0.82K0.18)0.50ZrO3 piezoceramics with high d33 coefficient. ACS Appl Mater Interfaces 2016, 8: 7257-7265.
Chen PY, Chou CC, Cheng NC, et al. The effects of aliovalent cations doping on electric-field-induced strain and microstructures of (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free piezoceramics. Ceram Int 2013, 39: S129-S133.
Huan Y, Wang XH, Fang J, et al. Grain size effects on piezoelectric properties and domain structure of BaTiO3 ceramics prepared by two-step sintering. J Am Ceram Soc 2013, 96: 3369-3371.
Wang XZ, Huan Y, Zhao PY, et al. Optimizing the grain size and grain boundary morphology of (K,Na)NbO3-based ceramics: Paving the way for ultrahigh energy storage capacitors. J Materiomics 2021, 7: 780-789.
Lv X, Zhang XX, Wu JG. Nano-domains in lead-free piezoceramics: A review. J Mater Chem A 2020, 8: 10026-10073.
Huan Y, Wang XH, Fang J, et al. Grain size effect on piezoelectric and ferroelectric properties of BaTiO3 ceramics. J Eur Ceram Soc 2014, 34: 1445-1448.
Cen ZY, Yu Y, Zhao PY, et al. Grain configuration effect on the phase transition, piezoelectric strain and temperature stability of KNN-based ceramics. J Mater Chem C 2019, 7: 1379-1387.
Shankar U, Kumar N, Narayan B, et al. Large electromechanical response in ferroelectrics: Beyond the morphotropic phase boundary paradigm. Phys Rev B 2019, 100: 094101.
Peng J, Liu WB, Zeng JT, et al. Large electromechanical strain at high temperatures of novel textured BiFeGaO3- BaTiO3 based ceramics. J Mater Sci Technol 2020, 48: 92-99.
Zheng T, Wu HJ, Yuan Y, et al. The structural origin of enhanced piezoelectric performance and stability in lead free ceramics. Energy Environ Sci 2017, 10: 528-537.
You XZ. Ionic polarizability. Chin Sci Bull 1974, 19: 419-423. (in Chinese)
Kim SW, Lee TG, Kim DH, et al. Determination of the appropriate piezoelectric materials for various types of piezoelectric energy harvesters with high output power. Nano Energy 2019, 57: 581-591.
Yan XD, Zheng MP, Gao X, et al. Giant current performance in lead-free piezoelectrics stem from local structural heterogeneity. Acta Mater 2020, 187: 29-40.
Yan XD, Zheng MP, Gao X, et al. Ultrahigh energy harvesting performance in lead-free piezocomposites with intragranular structure. Acta Mater 2022, 222: 117450.
Wu JG, Shi HD, Zhao TL, et al. High-temperature BiScO3-PbTiO3 piezoelectric vibration energy harvester. Adv Funct Mater 2016, 26: 7186-7194.
Kanno I, Ichida T, Adachi K, et al. Power-generation performance of lead-free (K,Na)NbO3 piezoelectric thin-film energy harvesters. Sens Actuat A Phys 2012, 179: 132-136.
Kim J, Koh JH. (Na,K)NbO3-(Bi,Na)TiO3 piezoelectric ceramics for energy-harvesting applications. J Eur Ceram Soc 2015, 35: 3819-3825.
Oh Y, Noh J, Yoo J, et al. Dielectric and piezoelectric properties of CeO2-added nonstoichiometric (Na0.5K0.5)0.97(Nb0.96Sb0.04)O3 ceramics for piezoelectric energy harvesting device applications. IEEE Trans Ultrason Ferroelectr Freq Control 2011, 58: 1860-1866.
Kim BY, Seo IT, Lee YS, et al. High-performance (Na0.5K0.5)NbO3 thin film piezoelectric energy harvester. J Am Ceram Soc 2015, 98: 119-124.
Zheng MP, Hou YD, Yan XD, et al. A highly dense structure boosts energy harvesting and cycling reliabilities of a high-performance lead-free energy harvester. J Mater Chem C 2017, 5: 7862-7870.
Coondoo I, Panwar N, Maiwa H, et al. Improved piezoelectric and energy harvesting characteristics in lead-free Fe2O3 modified KNN ceramics. J Electroceramics 2015, 34: 255-261.
Journal of Advanced Ceramics
Pages 935-944
Cite this article:
HUAN Y, WANG X, YANG W, et al. Optimizing energy harvesting performance by tailoring ferroelectric/relaxor behavior in KNN-based piezoceramics. Journal of Advanced Ceramics, 2022, 11(6): 935-944.








Web of Science






Received: 29 December 2021
Revised: 11 March 2022
Accepted: 12 March 2022
Published: 04 May 2022
© The Author(s) 2022.

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit