脱脂工艺对光固化3D打印堇青石陶瓷性能的影响

doi:10.15541/jim20210624

无机材料学报 ›› 2022, Vol. 37 ›› Issue (3): 317-324.DOI: 10.15541/jim20210624 CSTR: 32189.14.10.15541/jim20210624

所属专题：增材制造专题(2022)

脱脂工艺对光固化3D打印堇青石陶瓷性能的影响

朱俊逸(), 张成, 罗忠强, 曹继伟, 刘志远, 王沛, 刘长勇, 陈张伟()

深圳大学增材制造研究所, 深圳 518060

收稿日期:2021-10-08 修回日期:2021-10-21 出版日期:2022-03-20 网络出版日期:2021-11-01
通讯作者: 陈张伟, 教授. E-mail: chen@szu.edu.cn
作者简介:朱俊逸(1996-), 男, 硕士研究生. E-mail: 386398374@qq.com
基金资助:
国家自然科学基金(51975384);广东省自然科学基金(2020A1515011547);深圳市基础研究(JCYJ20190808144009478);深圳市高校稳定支持项目(20200731211324001);深大-台北科大合作项目(2021007)

Influence of Debinding Process on the Properties of Photopolymerization 3D Printed Cordierite Ceramics

ZHU Junyi(), ZHANG Cheng, LUO Zhongqiang, CAO Jiwei, LIU Zhiyuan, WANG Pei, LIU Changyong, CHEN Zhangwei()

Additive Manufacturing Institute, Shenzhen University, Shenzhen 518060, China

Received:2021-10-08 Revised:2021-10-21 Published:2022-03-20 Online:2021-11-01
Contact: CHEN Zhangwei, professor. E-mail: chen@szu.edu.cn
About author:ZHU Junyi (1996-), male, Master candidate. E-mail: 386398374@qq.com
Supported by:
National Natural Science Foundation of China(51975384);Natural Science Foundation of Guangdong Province(2020A1515011547);Basic Research Foundation of Shenzhen(JCYJ20190808144009478);University Support Fund of Shenzhen City(20200731211324001);NTUT-SZU Joint Research Program(2021007)

摘要/Abstract

摘要：

光固化3D打印是制造高度复杂结构陶瓷的一种有效方法。打印的样件需要经历脱脂和烧结等热处理才能成为可用的陶瓷件, 脱脂工艺对打印件性能影响巨大。本工作通过研究脱脂工艺对DLP光固化3D打印制备的堇青石陶瓷性能的影响规律, 建立缺陷抑制策略。比较并分析了脱脂气氛和升温速率对陶瓷样件的表面裂纹和元素分布状态的影响, 还对比进一步烧结后样件显微组织、尺寸收缩率、相对密度和弯曲强度等性能。研究发现脱脂气氛对样件各性能影响最大, 使用氩气脱脂可显著降低表面裂纹, 提高相对密度与弯曲强度; 并确定最佳升温速率为1 ℃/min。最终获得表面完整无裂纹且相对密度为(94.6±0.3)%, 弯曲强度为(94.3±3.2) MPa的堇青石陶瓷样件。本研究为光固化3D打印堇青石陶瓷的无缺陷制造与应用提供了科学依据与技术参考。

关键词: 堇青石陶瓷, 光固化3D打印, 脱脂, 烧结, 性能

Abstract:

Photopolymerization 3D printing method is an effective means for the manufacturing of ceramics with highly complex-shaped structures and exceptional performance. The printed samples need to undergo heat treatment such as debinding and sintering before becoming usable final ceramic parts in various industrial applications, and the debinding process has a great impact on the properties of the printed ceramic parts. In this study, effect of the debinding process on physical properties and mechanical performance of the cordierite ceramics prepared by DLP photopolymerization 3D printing was studied, and defect suppression strategy was established accordingly. The effects of debinding atmosphere and heating rate on surface cracks and material elemental distribution of ceramic samples were compared and analyzed. The microstructure, size shrinkage, relative density, and mechanical performance such as bending strength of the sintered samples were also studied. It is found that the debinding atmosphere has the most significant influence on the properties of the sintered samples, in which the surface cracks can be significantly reduced, and the relative density, and bending strength can be increased when the debinding process is conducted in argon atmosphere at the optimized heating rate of 1 ℃/min. After debinding and sintering, the cordierite ceramic samples with a relative density of (94.6±0.3)% and a bending strength of (94.3±3.2) MPa was obtained. In conclusion, this study provides a scientific basis and technical reference for fabrication and application of cordierite ceramics based on photopolymerization 3D printing method.

Key words: cordierite ceramic, photopolymerization 3D printing, debinding, sintering, properties

中图分类号:

TQ174

朱俊逸, 张成, 罗忠强, 曹继伟, 刘志远, 王沛, 刘长勇, 陈张伟. 脱脂工艺对光固化3D打印堇青石陶瓷性能的影响[J]. 无机材料学报, 2022, 37(3): 317-324.

ZHU Junyi, ZHANG Cheng, LUO Zhongqiang, CAO Jiwei, LIU Zhiyuan, WANG Pei, LIU Changyong, CHEN Zhangwei. Influence of Debinding Process on the Properties of Photopolymerization 3D Printed Cordierite Ceramics[J]. Journal of Inorganic Materials, 2022, 37(3): 317-324.

图/表 8

图1 DLP光固化增材制造原理

Fig. 1 Working principle of DLP 3D printing technology

图2 堇青石陶瓷生坯的热重分析结果与脱脂和烧结曲线

Fig. 2 TG/DSC curves, debinding and sintering curves of printed cordierite green body (a) TG/DSC curves; (b) Debinding curve; (c) Sintering curve

图3 不同升温速率脱脂后的样件表面宏观形貌

Fig. 3 Surface macro-graphs of sample after debinding at different heating rates In air: (a) 0.1 ℃/min; (b) 0.5 ℃/min; (c) 1 ℃/min; (d) 3 ℃/min; (e) 5 ℃/min; In argon: (f) 0.1 ℃/min; (g) 0.5 ℃/min; (h) 1 ℃/min; (i) 3 ℃/min; (j) 5 ℃/min

图4 空气气氛下脱脂后样件的EDS元素分析

Fig. 4 Element analysis of sample after debinding in air (a) SEM image; EDS mappings of (b) Al, (c) Mg, (d) O and (e) Si; (f) EDS spectrum

图5 氩气气氛下脱脂后样件EDS元素分析

Fig. 5 Element analysis after debinding in argon (a) SEM image; EDS mappings of (b) Al, (c) Mg, (d) C and (e) O; (f) Si; (g) EDS spectrum

图6 在氩气气氛下脱脂后的样件表面微观形貌

Fig. 6 Micrographs of sample surfaces after debinding in argon(a) 0.1 ℃/min; (b) 0.5 ℃/min; (c) 1 ℃/min; (d) 3 ℃/min; (e) 5 ℃/min

图7 在不同气氛、不同脱脂升温速率下脱脂并经烧结后样件的性能

Fig. 7 Properties of samples after debinding in different atmospheres followed by sintering (a) Shrinkage rate-debinding in air; (b) Shrinkage rate-debinding in argon; (c) Relative density; (d) Bending strength

图8 优化脱脂策略后烧结的样件

Fig. 8 Final cordierite ceramics prepared with optimized debinding scheme followed by sintering (a, b) Dense rectangular sample; (c) Honeycomb structures with complex inter-crossing channels

参考文献 30

[1]	CAMERUCCI M A, URRETAVIZCAYA G, CASTRO M S, et al. Electrical properties and thermal expansion of cordierite and cordierite- mullite materials. Journal of the European Ceramic Society, 2001, 21(16): 2917-2923. DOI URL
[2]	LAMARA S, REDAOUI D, SAHNOUNE F, et al. Microstructure, thermal expansion, hardness and thermodynamic parameters of cordierite materials synthesized from Algerian natural clay minerals and magnesia. Boletín de la Sociedad Española de Cerámica y Vidrio, 2020, 60(5): 291-306. DOI URL
[3]	SITTIAKKARANON S. Thermal shock resistance of mullite- cordierite ceramics from kaolin, talc and alumina raw materials. Materials Today: Proceedings, 2019, 17(4): 1864-1871.
[4]	CHEN Z, LIU C, LI J, et al. Mechanical properties and microstructures of 3D printed bulk cordierite parts. Ceramics International, 2019, 45(15): 19257-19267. DOI URL
[5]	GÖKÇE H, AĞAOĞULLARI D, ÖVEÇOĞLU M L, et al. Characterization of microstructural and thermal properties of steatite/ cordierite ceramics prepared by using natural raw materials. Journal of the European Ceramic Society, 2011, 31(14): 2741-2747. DOI URL
[6]	AVILA P, MONTES M, MIRÓ E E. Monolithic reactors for environmental applications: a review on preparation technologies. Chemical Engineering Journal, 2005, 109(1/2/3): 11-36. DOI URL
[7]	DAS R N, MADHUSOODANA C D, OKADA K, Rheological studies on cordierite honeycomb extrusion. Journal of the European Ceramic Society, 2002, 22(16): 2893-2900. DOI URL
[8]	LIANG Q, LI D, YANG G. Rapid fabrication of diamond-structured ceramic photonic crystals with graded dielectric constant and its controllable stop band properties. Ceramics International, 2013, 39(1): 153-157. DOI URL
[9]	MELCHELS F P W, FEIJEN J, GRIJPMA D W. A review on stereolithography and its applications in biomedical engineering. Biomaterials, 2010, 31(24): 6121-6130. DOI URL
[10]	ZHOU W, LI D, CHEN Z. Direct fabrication of an integral ceramic mould by stereolithography. Proceedings of the Institution of Mechanical Engineers, Part B: Journal of Engineering Manufacture, 2010, 224(2): 237-243. DOI URL
[11]	ZOCCA A, COLOMBO P, GOMES C M, et al. Additive manufacturing of ceramics: issues, potentialities, and opportunities. Journal of the American Ceramic Society, 2015, 98(7): 1983-2001. DOI URL
[12]	CHEN Z, LI Z, LI J, et al. 3D printing of ceramics: a review. Journal of the European Ceramics Society, 2019, 39(4): 661-687. DOI URL
[13]	CHEN Z, LI D, ZHOU W. Process parameters appraisal of fabricating ceramic parts based on stereolithography using the Taguchi method. Proceedings of the Institution of Mechanical Engineers, Part B: Journal of Engineering Manufacture, 2012, 226(7): 1249-1258. DOI URL
[14]	LIU Y, CHEN Z, LI J, et al. 3D printing of ceramic cellular structures for potential nuclear fusion application. Additive Manufacturing, 2020, 35: 101348. DOI URL
[15]	RASAKI S A, XIONG D, XIONG S, et al. Photopolymerization- based additive manufacturing of ceramics: a systematic review. Journal of Advanced Ceramics, 2021, 10(3): 442-471. DOI URL
[16]	LIU C, XU F, LIU Y, et al. High mass loading ultrathick porous Li₄Ti₅O₁₂ electrodes with improved areal capacity fabricated via low temperature direct writing. Electrochimica Acta, 2019, 314: 81-88. DOI URL
[17]	WU Z, HUAN Z, ZHU Y, et al. 3D printing and characterization of microsphere hydroxyapatite scaffolds. Journal of Inorganic Materials, 2021, 36(6): 601-607. DOI URL
[18]	CHEN Z, BRANDON N. Inkjet printing and nanoindentation of porous alumina multilayers. Ceramics International, 2016, 42(7): 8316-8324. DOI URL
[19]	CHEN Z, OUYANG J, LIANG W, et al. Development and characterizations of novel aqueous-based LSCF suspensions for inkjet printing. Ceramics International, 2018, 44(11): 13381-13388. DOI URL
[20]	ZHANG L, YANG X, XU X, et al. 3D printed zirconia ceramics via fused deposit modeling and its mechanical properties. Journal of Inorganic Materials, 2021, 36(4): 436-442. DOI
[21]	LIU S, LI M, WU J, et al. Preparation of high-porosity Al₂O₃ ceramic foams via selective laser sintering of Al₂O₃ poly-hollow microspheres. Ceramics International, 2020, 46(4): 4240-4247. DOI URL
[22]	FERRAGE L, BERTRAND G, LENORMAND P. Dense yttria- stabilized zirconia obtained by direct selective laser sintering. Additive Manufacturing, 2018, 21: 472-478. DOI URL
[23]	MINASYAN T, LIU L, AGHAYAN M, et al. A novel approach to fabricate Si₃N₄ by selective laser melting. Ceramics International, 2018, 44(12): 13689-13694. DOI URL
[24]	CHEN Z, LI J, LIU C, et al. Preparation of high solid loading and low viscosity ceramic slurries for photopolymerization-based 3D printing. Ceramics International, 2019, 45(9): 11549-11557. DOI URL
[25]	SHUAI X, ZENG Y, LI P, et al. Fabrication of fine and complex lattice structure Al₂O₃ ceramic by digital light processing 3D printing technology. Journal of Materials Science, 2020, 55: 6771-6782. DOI URL
[26]	LI H, SONG L, SUN J, et al. Stereolithography-fabricated zirconia dental prostheses: concerns based on clinical requirements. Journal of Advances in Applied Ceramics, 2020, 119(5/6): 236-243.
[27]	FENG C, ZHANG C, HE R, et al. Additive manufacturing of hydroxyapatite bioceramic scaffolds: dispersion, digital light processing, sintering, mechanical properties, and biocompatibility. Journal of Advanced Ceramics, 2020, 9: 360-373. DOI URL
[28]	HE R, DING G, ZHANG K, et al. Fabrication of SiC ceramic architectures using stereolithography combined with precursor infiltration and pyrolysis. Ceramics International, 2019, 45(11): 14006-14014. DOI URL
[29]	ZHANG C, LUO Z, LIU C, et al. Dimensional retention of photocured ceramic units during 3D printing and sintering processes. Ceramics International, 2021, 47(8): 11097-11108. DOI URL
[30]	CHEN Z, LIU C, LI J, et al. Mechanical properties and microstructures of 3D printed bulk cordierite parts. Ceramics International, 2019, 45(15): 19257-19267. DOI URL

脱脂工艺对光固化3D打印堇青石陶瓷性能的影响

Influence of Debinding Process on the Properties of Photopolymerization 3D Printed Cordierite Ceramics

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