粉末烧结法制备α-堇青石基玻璃陶瓷的析晶动力学和性能

doi:10.15541/jim20220179

无机材料学报 ›› 2022, Vol. 37 ›› Issue (12): 1351-1357.DOI: 10.15541/jim20220179

粉末烧结法制备α-堇青石基玻璃陶瓷的析晶动力学和性能

孙扬善¹^,³(), 杨治华², 蔡德龙², 张正义¹^,³, 柳琪¹^,³, 房树清¹^,³, 冯良¹^,³, 石丽芬¹^,³, 王友乐¹^,³, 贾德昌²

1.中建材玻璃新材料研究院集团有限公司, 浮法玻璃新技术国家重点实验室,, 蚌埠 233000
2.哈尔滨工业大学, 结构功能一体化材料及其绿色制造技术工信部重点实验室, 哈尔滨 150001
3.安徽省硅基材料实验室, 蚌埠 233000

收稿日期:2022-03-30 修回日期:2022-05-25 出版日期:2022-12-20 网络出版日期:2022-06-03
作者简介:孙扬善(1989-), 男, 高级工程师. E-mail: ashan19890608@163.com

Crystallization Kinetics, Properties of α-cordierite Based Glass-ceramics Prepared by Glass Powder Sintering

SUN Yangshan¹^,³(), YANG Zhihua², CAI Delong², ZHANG Zhengyi¹^,³, LIU Qi¹^,³, FANG Shuqing¹^,³, FENG Liang¹^,³, SHI Lifen¹^,³, WANG Youle¹^,³, JIA Dechang²

1. State Key Laboratory of Advanced Technology for Float Glass, CNBM Research Institute for Advanced Glass Materials Group Co., Ltd, Bengbu 233000, China
2. Key Laboratory of Advanced Structrual-Functional Integration Materials & Green Manufacturing Technology, Harbin Institute of Technology, Harbin 150001, China
3. Silica-based Materials Laboratory of Anhui Province, Bengbu 233000, China

Received:2022-03-30 Revised:2022-05-25 Published:2022-12-20 Online:2022-06-03
About author:SUN Yangshan (1989-), male, senior engineer. E-mail: ashan19890608@163.com
Supported by:
Anhui Provincial Natural Science Foundation (Youth Project)(2008085QE248);Key Research and Development Projects of Anhui Province(202004a05020061);Key Research and Development Projects of Anhui Province(202004a05020036);The 6th China Association for Science and Technology “Young Talent Support Project”

摘要/Abstract

摘要：

在堇青石化学计量组分和非堇青石化学计量组分中分别添加B₂O₃, 通过玻璃粉末烧结法制备玻璃陶瓷,并研究了玻璃陶瓷的性能, 包括非等温析晶动力学、热学、力学和介电性能。本研究使用非堇青石化学计量组分制备了α-堇青石基玻璃陶瓷, 并加入B₂O₃促进α-堇青石析出, 提高MgO-Al₂O₃-SiO₂玻璃的结晶能力。玻璃成分中过量的MgO和SiO₂不会影响玻璃的析晶能力, 但会影响析晶的类型; 增加B₂O₃含量可以制备低热膨胀系数的α-堇青石基玻璃陶瓷, 但会降低玻璃陶瓷的软化点。此外, 增加B₂O₃含量还可以提高玻璃陶瓷的致密性和强度。α-堇青石基玻璃陶瓷的最大抗弯强度、弹性模量、断裂韧性和体积密度分别为(42.4±3.0) MPa、(34.0±2.9) GPa、(0.7±0.15) MPa·m^1/2和1.53 g/cm³。制备的α-堇青石基玻璃陶瓷表现出良好的介电性能(介电常数低至3.5), 热膨胀系数低至4.22×10^-6 K^-1。

关键词: α-堇青石, 玻璃陶瓷, 粉末烧结, 析晶动力学, 力学性能, 介电性能

Abstract:

The resulting glass-ceramics were prepared by glass powder sintering using stoichiometric and non-stoichiometric cordierite components with addition of B₂O₃. Properties of the glass-ceramics, including the non- isothermal crystallization kinetics, thermal, mechanical and dielectric properties were investigated. The α-cordierite based glass-ceramics can be easily prepared by using non-stoichiometric cordierite components, and B₂O₃ addition can promote the precipitation of α-cordierite and improve the crystallization ability of the MgO-Al₂O₃-SiO₂ glass. Moreover, rich MgO and SiO₂ in the glass composition did not affect the crystallization ability of the glass, but affect the type of precipitated crystal phase. The increase of B₂O₃ addition can prepare α-cordierite based glass-ceramics with a low coefficient of thermal expansion (CTE), but it also lower its softening point. In addition, the increase of B₂O₃ addition can also improve the compactness and mechanical strength of the glass-ceramics. The maximum flexural strength, elastic moduli, fracture toughness and bulk density of α-cordierite based glass-ceramics are (42.4±3.0) MPa, (34.0±2.9) GPa, (0.7±0.15) MPa·m^1/2, and 1.53 g/cm³, respectively. And the as-prepared α- cordierite based glass-ceramics show good dielectric properties (ɛ as low as 3.5) with a low CTE of 4.22 × 10^-6 K^-1.

Key words: α-cordierite, glass-ceramics, powder sintering, crystallization kinetics, mechanical property, dielectric property

中图分类号:

TQ174

孙扬善, 杨治华, 蔡德龙, 张正义, 柳琪, 房树清, 冯良, 石丽芬, 王友乐, 贾德昌. 粉末烧结法制备α-堇青石基玻璃陶瓷的析晶动力学和性能[J]. 无机材料学报, 2022, 37(12): 1351-1357.

SUN Yangshan, YANG Zhihua, CAI Delong, ZHANG Zhengyi, LIU Qi, FANG Shuqing, FENG Liang, SHI Lifen, WANG Youle, JIA Dechang. Crystallization Kinetics, Properties of α-cordierite Based Glass-ceramics Prepared by Glass Powder Sintering[J]. Journal of Inorganic Materials, 2022, 37(12): 1351-1357.

图/表 11

Table 1 Proportion of MAS based glass raw materials (molar percent)

Powder	MgO	Al₂O₃	SiO₂	B₂O₃	Molar ratio of MgO : Al₂O₃ : SiO₂
S	13.80 g (21.38%)	34.90 g (21.19%)	51.30 g (52.8%)	5.00 g (4.45%)	2 : 2 : 5
NS1	24.00 g (33.56%)	22.00 g (12.08%)	54.00 g (50.34%)	5.00 g (4.02%)	6 : 2 : 9
NS2	24.00 g (32.26%)	22.00 g (11.61%)	54.00 g (48.39%)	10.00 g (7.74%)	6 : 2 : 9
NS3	24.00 g (31.06%)	22.00 g (11.18%)	54.00 g (46.58%)	15.00 g (11.18%)	6 : 2 : 9

Fig. 1 DTA curves of MAS glass powders at heating rate of 5 ℃/min

Fig. 2 XRD patterns of the glass-ceramics samples

Fig. 3 DTA curves of the glass powders at different heating rates (a) S; (b) NS1; (c) NS2; (d) NS3

Fig. 4 Plots of ln(β/Tp2) versus 1/Tp according to Kissinger equation

Table 2 Non-isothermal crystallization kinetic parameters of the glass powders

Powder	E/ (kJ·mol^-1)	A	k (T_p)
Powder	E/ (kJ·mol^-1)	A	5 ℃/ min	10 ℃/ min	15 ℃/ min	20 ℃/ min	Mean
S	330.56	4.39×10¹²	0.117	0.265	0.348	0.417	0.285
NS1	332.06	3.54×10¹²	0.118	0.245	0.345	0.430	0.285
NS2	412.12	4.68×10¹⁵	0.141	0.287	0.424	0.528	0.345
NS3	417.86	8.05×10¹⁵	0.156	0.271	0.412	0.580	0.355

Fig. 5 Thermal expansion curves (a) and CTE (b) of the as-prepared glass-ceramics

Fig. 6 Bulk density and apparent porosity of the as-prepared glass-ceramics

Fig. 7 Mechanical properties of the as-prepared glass-ceramics

Fig. 8 Morphologies of the as-prepared glass-ceramics (a) S; (b) NS1; (c) NS2; (d) NS3

Fig. 9 Dielectric constant (a) and loss tangent (b) of the as- prepared glass-ceramics

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粉末烧结法制备α-堇青石基玻璃陶瓷的析晶动力学和性能

Crystallization Kinetics, Properties of α-cordierite Based Glass-ceramics Prepared by Glass Powder Sintering

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