|
|
|
| Gel casting preparation and electrical properties study of Pb(Zr,Ti)O3 ceramics |
| WANG Siyuan1, LIU Shengwen1, ZHANG Dou1, YUAN Xi2 |
1. Powder Metallurgy Research Institute, Central South University, Changsha 410083, China; 2. College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China |
|
|
|
|
Abstract To meet the manufacturing requirements of piezoelectric ceramics with special-shaped structures, this study employed the gel casting process to fabricate Pb(Zr,Ti)O3 (PZT) ceramics. The effects of dispersant dosage, solid content, and resin concentration on slurry rheological property, green body strength, and ceramic electrical properties were systematically investigated using rotational rheometer, universal mechanical testing machine, ferroelectric analyzer, impedance analyzer, quasi-static piezoelectric tester, and scanning electron microscope. The results show that when using ammonium polyacrylate as the dispersant, the slurry achieves the lowest viscosity at a dispersant content of 0.7% (mass fraction), with a viscosity of 201.05 mPa·s at 100 s-1, indicating optimal fluidity. When the solid content does not exceed 55% (volume fraction), the slurry exhibits favorable shear-thinning behavior, making it suitable for filling complex structures. The bending strength of the green body increases with the increase of resin concentration, reaching (41.79±5.49) MPa at a resin mass fraction of 25% and a solid volume fraction of 55%, meeting the demolding requirements for special-shaped green bodies. Using this formulation, with the ceramic sintered at 1 275 ℃ exhibits a dense structure with uniform grains, achieving a piezoelectric constant d33 of (618.36±5.65) pC/N, a relative dielectric constant εr of 2 455.41±33.16, and an electromechanical coupling coefficient kp of 0.62. The comprehensive performance is comparable to or even better than that of samples prepared by conventional dry pressing, and significantly surpasses that of 3D-printed samples. This study demonstrates that high-quality near net shaping of complex-shaped PZT ceramics can be achieved by optimizing the gel casting process parameters, providing an effective approach for the fabrication of special-shaped piezoelectric components.
|
|
Received: 06 February 2026
Published: 03 July 2026
|
|
|
|
|
|
[1] MANBACHI A, COBBOLD R S C. Development and application of piezoelectric materials for ultrasound generation and detection[J]. Ultrasound, 2011, 19(4): 187-196. [2] LI Z X, HE J R, FEI C L, et al.Piezoelectric metasurface for high-frequency ultrasonic transducer application around 50 MHz[J]. Ceramics International, 2024, 50(23): 51919-51927. [3] ZHOU X, YUE Q W, ZHANG Q Z, et al.Preparation and simulation of lead free NBBT/epoxy 1-3 piezoelectric composites for high frequency medical ultrasound[J]. Composites Communications, 2022, 36: 101399. [4] AJENIFUJA G R.Comparative study of non-destructive testing methods for failure detection in high-pressure industrial equipment[J]. International Journal of Research in Engineering and Science, 2025, 13(8): 125-134. [5] LIM Y Y, KWONG K Z, LIEW W Y H, et al. Non-destructive concrete strength evaluation using smart piezoelectric transducer: a comparative study[J]. Smart Materials and Structures, 2016, 25(8): 085021. [6] HU H J, HUANG H, LI M H, et al.A wearable cardiac ultrasound imager[J]. Nature, 2023, 613(7945): 667-675. [7] ZASZCZYŃSKA A, GRADYS A, SAJKIEWICZ P. Progress in the applications of smart piezoelectric materials for medical devices[J]. Polymers, 2020, 12(11): 2754. [8] HAERTLING G H.Ferroelectric ceramics: history and technology[J]. Journal of the American Ceramic Society, 1999, 82(4): 797-818. [9] WANG H, ZHAI X, XU J W, et al.Effect of sintering time on structure and properties in CuO-doping KNN-LS-BF piezoelectric ceramics[J]. Journal of Wuhan University of Technology-Materials Science Edition, 2019, 34(2): 308-311. [10] GONZÁLEZ-GUTIÉRREZ J, STRINGARI G B, EMRI I. Powder injection molding of metal and ceramic parts[M]//WANG J. Some Critical Issues for Injection Molding. London: IntechOpen, 2012: 65-88. [11] STANIMIROVIĆ Z, STANIMIROVIĆ I.Ceramic injection molding[M]//WANG J. Some Critical Issues for Injection Molding. London: IntechOpen, 2012: 131-148. [12] DOERFFEL C, DECKER R, HEINRICH M, et al.Polypropylene based piezo ceramic compounds for micro injection molded sensors[J]. Key Engineering Materials, 2017, 742: 807-814. [13] LI Z Y, LI J, LUO H, et al.Direct ink writing of 3D piezoelectric ceramics with complex unsupported structures[J]. Journal of the European Ceramic Society, 2022, 42(9): 3841-3847. [14] 王小锋, 刘子瑞, 周红莉, 等. SiC浆料的流变性能及多孔陶瓷的直写成型[J]. 粉末冶金材料科学与工程, 2023, 28(6): 580-586. WANG Xiaofeng, LIU Zirui, ZHOU Hongli, et al.Rheological properties of SiC slurry and direct-ink writing of porous ceramic[J]. Materials Science and Engineering of Powder Metallurgy, 2023, 28(6): 580-586. [15] PUMA J, YANG Z, JOHNSTON E, et al. 3D necroprinting: leveraging biotic material as the nozzle for 3D printing[J]. Science Advances, 2025, 11(47): eadw9953. [16] SRIPHUTKIAT Y.Development of acoustic nozzle for 3D printing[D]. Singapore: Nanyang Technological University, 2019. [17] 谭彦妮, 刘咏, 向其军. 牙科光固化复合树脂材料的性能与展望[J]. 粉末冶金材料科学与工程, 2007, 12(3): 139-145. TAN Yanni, LIU Yong, XIANG Qijun.Properties and prospect of light-cured dental composite resins[J]. Materials Science and Engineering of Powder Metallurgy, 2007, 12(3): 139-145. [18] 李青, 刘耀, 蔡伟金, 等. 粉体表面改性对氧化锆光固化成形的影响[J]. 粉末冶金材料科学与工程, 2020, 25(2): 140-147. LI Qing, LIU Yao, CAI Weijin, et al.Effect of powder surface modification on stereolithography of zirconia[J]. Materials Science and Engineering of Powder Metallurgy, 2020, 25(2): 140-147. [19] MA W G, WANG C M, WANG X R, et al.Multifarious strategies for resolving the deep-curing challenges of PZT piezoceramics slurry in vat photopolymerization[J]. Journal of the American Ceramic Society, 2025, 108(10): e70067. [20] MITKUS R, PIEROU A, FEDER J, et al.Investigation and attempt to 3D print piezoelectric 0-3 composites made of photopolymer resins and PZT[C]//Proceedings of the ASME 2020 Conference on Smart Materials, Adaptive Structures and Intelligent Systems. New York: ASME, 2020: V001T04A017. [21] CHEN Y, BAO X L, WONG C M, et al.PZT ceramics fabricated based on stereolithography for an ultrasound transducer array application[J]. Ceramics International, 2018, 44(18): 22725-22730. [22] OMATETE O O, JANNEY M A, NUNN S D.Gelcasting: from laboratory development toward industrial production[J]. Journal of the European Ceramic Society, 1997, 17(2/3): 407-413. [23] KASTYL J, CHLUP Z, STASTNY P, et al.Machinability and properties of zirconia ceramics prepared by gelcasting method[J]. Advances in Applied Ceramics, 2020, 119(5/6): 252-260. [24] 胡汇明, 杜文艺. 一种异形压电风扇、热源结构: CN202211624957.4[P].2023-03-07. HU Huiming, DU Wenyi. A special-shaped piezoelectric fan and heat source structure: CN202211624957.4[P].2023-03-07. [25] TIAN J T, LI X B, LIANG Z, et al.Fabrication of 1-3 piezoelectric composites via modified soft mold process for 40 MHz ultrasonic medical transducers[J]. Ceramics International, 2022, 48(3): 3841-3848. [26] GÜNTHER P A, NEUMEISTER P, NEUBERT H, et al. Development of 40-MHz ultrasonic transducers via soft mold process[J]. IEEE Transactions on Ultrasonics, Ferroelectrics, and Frequency Control, 2019, 66(9): 1497-1503. [27] BUŠOVÁ M, BENCKO V, LAKTIČOVÁ K V, et al. Risk of exposure to acrylamide[J]. Central European Journal of Public Health, 2020, 28: S43-S46. [28] KIM J, CHOI Y J, GAL C W, et al.Effect of dispersants on structural integrity of 3D printed ceramics[J]. International Journal of Applied Ceramic Technology, 2022, 19(2): 968-978. [29] DAVIES J, BINNER J G P. The role of ammonium polyacrylate in dispersing concentrated alumina suspensions[J]. Journal of the European Ceramic Society, 2000, 20(10): 1539-1553. [30] 荆慧, 李奕宁, 姜博, 等. 空心涡轮叶片氧化铝基陶瓷铸型的凝胶注模成型行为[J]. 硅酸盐通报, 2014, 33(8): 2073-2077. JING Hui, LI Yining, JIANG Bo, et al.Gelcasting filling behavior of alumina ceramic mold of hollow turbine blade[J]. Bulletin of the Chinese Ceramic Society, 2014, 33(8): 2073-2077. [31] SHEN Z G, CHEN J F, ZOU H K, et al.Rheology of colloidal nanosized BaTiO3 suspension with ammonium salt of polyacrylic acid as a dispersant[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2004, 244(1/2/3): 61-66. [32] BOISVERT J P, MALGAT A, POCHARD I, et al.Influence of the counter-ion on the effective charge of polyacrylic acid in dilute condition[J]. Polymer, 2002, 43(1): 141-148. [33] XIONG H W, ZHAO L Z, CHEN H H, et al.3D SiC containing uniformly dispersed, aligned SiC whiskers: printability, microstructure and mechanical properties[J]. Journal of Alloys and Compounds, 2019, 809: 151824. [34] 赵阳, 谢睿, 张妍, 等. 水溶性环氧树脂的锆钛酸铅压电陶瓷凝胶注模成型[J]. 中国有色金属学报, 2014, 24(3): 773-778. ZHAO Yang, XIE Rui, ZHANG Yan, et al.Gelcasting of lead zirconate titanate prepared by water-soluble epoxy resin[J]. The Chinese Journal of Nonferrous Metals, 2014, 24(3): 773-778. [35] MUELLER S, LLEWELLIN E W, MADER H M.The rheology of suspensions of solid particles[J]. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, 2010, 466(2116): 1201-1228. [36] 谢睿. 精细结构PZT陶瓷阵列的新型凝胶注模成型研究[D]. 长沙: 中南大学, 2014. XIE Rui.Fabrication of fine scale piezoelectric arrays by novel aqueous gelcasting[D]. Changsha: Central South University, 2014. [37] EDIRISINGHE M J, SHAW H M, TOMKINS K L.Flow behaviour of ceramic injection moulding suspensions[J]. Ceramics International, 1992, 18(3): 193-200. [38] 李旭晖, 单肖文, 段文洋. 格子玻尔兹曼正则化碰撞模型的理论进展[J]. 空气动力学学报, 2022, 40(3): 46-64. LI Xuhui, SHAN Xiaowen, DUAN Wenyang.Theoretical progress on regularized lattice Boltzmann collision models[J]. Acta Aerodynamica Sinica, 2022, 40(3): 46-64. [39] MORRIS J F.A review of microstructure in concentrated suspensions and its implications for rheology and bulk flow[J]. Rheologica Acta, 2009, 48(8): 909-923. [40] STICKEL J J, POWELL R L.Fluid mechanics and rheology of dense suspensions[J]. Annual Review of Fluid Mechanics, 2005, 37: 129-149. [41] DUŠEK K. Network formation in curing of epoxy resins[M]//DUŠEK K. Epoxy Resins and Composites III. Berlin: Springer. 2005: 1-59. [42] JIN J Y, TAKAHASHI H, IWASAKI N.Effect of test method on flexural strength of recent dental ceramics[J]. Dental Materials Journal, 2004, 23(4): 490-496. [43] WACHTMAN J B, CANNON W R, MATTHEWSON M J.Mechanical Properties of Ceramics[M]. Newyork: John Wiley & Sons, Inc., 2009. [44] GUO X.Gel casting of high strength ceramics[D]. Göteborg: Chalmers University of Technology, 2011. [45] MALEKSAEEDI S, PAYDAR M H, MA J.Centrifugal deairing of concentrated ceramic slurries[J]. Journal of the American Ceramic Society, 2009, 92(12): 2861-2869. [46] LAURO N, OUMMADI S, ALZINA A, et al.Computer model of drying behaviour of ceramic green bodies with particular reference to moisture content dependent properties[J]. Journal of the European Ceramic Society, 2021, 41(14): 7321-7329. [47] BROSNAN D A, ROBINSON G C.Introduction to Drying of Ceramics: With Laboratory Exercises[M]. Hoboken: Wiley, 2003. [48] SOARES M R, SENOS A M R, MANTAS P Q. Phase coexistence region and dielectric properties of PZT ceramics[J]. Journal of the European Ceramic Society, 2000, 20(3): 321-334. [49] HELKE G, LUBITZ K.Piezoelectric PZT ceramics[M]//HEYWANG W, LUBITZ K, WERSING W. Piezoelectricity: Evolution and Future of a Technology. Berlin: Springer, 2008: 89-130. [50] KANG S J L. Sintering: Densification, Grain Growth and Microstructure[M]. Oxford: Elsevier Butterworth-Heinemann, 2004. [51] 刘亦轩, 李昭, 汤浩正, 等. 晶粒尺寸对钙钛矿型压电陶瓷压电性能的影响[J]. 物理学报, 2020, 69(21): 86-104. LIU Yixuan, LI Zhao, TANG Haozheng, et al.Grain size effect on piezoelectric performance in perovskite-based piezoceramics[J]. Acta Physica Sinica, 2020, 69(21): 86-104. [52] SCHULTHEIß J, CHECCHIA S, URŠIČ H, et al. Domain wall-grain boundary interactions in polycrystalline Pb(Zr0.7Ti0.3)O3 piezoceramics[J]. Journal of the European Ceramic Society, 2020, 40(12): 3965-3973. [53] MARTIRENA H T, BURFOOT J C.Grain-size effects on properties of some ferroelectric ceramics[J]. Journal of Physics C: Solid State Physics, 1974, 7(17): 3182-3192. [54] WANG J C, ZHENG P, YIN R Q, et al.Different piezoelectric grain size effects in BaTiO3 ceramics[J]. Ceramics International, 2015, 41(10): 14165-14171. [55] CHENG Z H, CHEN L L, LIAO Y H, et al.The effect of solid content on the anisotropy for 3D printed barium titanate piezoelectric ceramics[J]. Ceramics International, 2024, 50(23): 50697-50703. [56] ZHANG Y, ROSCOW J, LEWIS R, et al.Understanding the effect of porosity on the polarisation-field response of ferroelectric materials[J]. Acta Materialia, 2018, 154: 100-112. [57] PADURARIU L, CURECHERIU L, GALASSI C, et al.Tailoring non-linear dielectric properties by local field engineering in anisotropic porous ferroelectric structures[J]. Applied Physics Letters, 2012, 100(25): 252905. [58] 曾芳芳. BiFeO3-BaTiO3基高温压电陶瓷的电致应变机理及性能研究[D]. 武汉: 华中科技大学, 2022. ZENG Fangfang.Electrostrain performance and its mechanism of high temperature BiFeO3-BaTiO3-based piezoelectric ceramics[D]. Wuhan: Huazhong University of Science and Technology, 2022. [59] BUTT Z, ANJUM Z, SULTAN A, et al.Investigation of electrical properties & mechanical quality factor of piezoelectric material (PZT-4A)[J]. Journal of Electrical Engineering and Technology, 2017, 12(2): 846-851. [60] SADEGHPOUR S, MEYERS S, KRUTH J P, et al.Resonating shell: a spherical-omnidirectional ultrasound transducer for underwater sensor networks[J]. Sensors, 2019, 19(4): 757. [61] 刘春磊. PZT基压电陶瓷数字光处理成形的固化增强方法及其性能调控研究[D]. 武汉: 华中科技大学, 2024. LIU Chunlei.Research on the curing enhancement method and performance regulation of PZT-based piezoceramics fabricated by digital light processing[D]. Wuhan: Huazhong University of Science and Technology, 2024. [62] WANG X, LÜ S, HU X, et al.Effect of solid loading on the electrical properties of PZT-based porous piezoelectric ceramics produced by DIW 3D printing[J]. Ceramics International, 2026, 52(10): 14660-14669. |
|
|
|