硅酸盐学报

含锌钇铝硅酸盐玻璃的晶化特征和力学性能

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郑庆双 ¹ , 陈胜林 ¹ , 乔昂 ¹ , 王觅堂 ² , 陶海征 ¹

硅酸盐学报 | 微晶玻璃专题—研究论文 2024,52(8): 2495-2501

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硅酸盐学报 |微晶玻璃专题—研究论文 2024 , 52 (8) : 2495 -2501

含锌钇铝硅酸盐玻璃的晶化特征和力学性能

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郑庆双¹, 陈胜林¹, 乔昂¹, 王觅堂², 陶海征¹

作者信息

^1．武汉理工大学，硅酸盐建筑材料国家重点实验室，武汉 430070

^2．上海理工大学材料与化学学院，上海 200093

通讯作者:

陶海征（1973—），男，博士，教授。

作者简介:

郑庆双（1994—），男，博士研究生。

Crystallization Behavior and Mechanical Properties of Zinc-Containing Yttrium Aluminosilicate Glasses

Qingshuang ZHENG¹, Shenglin CHEN¹, Ang QIAO¹, Mitang WANG², Haizheng TAO¹

Affiliations

^1.State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China

^2.School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China

Corresponding Author:

TAO Haizheng (1973-), male, Ph.D., Professor. E-mail: thz@whut.edu.cn

ZHENG Qingshuang (1994-), male, Doctoral candidate. E-mail: qingshuangzheng@163.com

出版时间: 2024-08-20 doi: 10.14062/j.issn.0454-5648.20230897

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摘要

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因具有与碳化硅陶瓷相匹配的膨胀系数和良好的物化性能，钇铝硅酸盐（YAS）玻璃和玻璃陶瓷广受关注。为进一步提升YAS玻璃陶瓷的力学性能，以22Y₂O₃·19Al₂O₃·59SiO₂玻璃为基础，基于n（ZnO）∶n（Al₂O₃）=2∶1摩尔比，利用ZnO逐步替换Al₂O₃，探索了系列含锌YAS玻璃的晶化特征和力学性能。通过选择合适的热处理工艺，制备了系列玻璃陶瓷。结果发现：ZnO的引入具有晶粒细化作用，随着ZnO含量的增加，析出晶粒的尺寸逐渐减小；通过合适的热处理，获得了最大断裂韧性为1.92 MPa·m^0.5的含锌YAS玻璃陶瓷；与原始无锌YAS玻璃陶瓷（1.16 MPa·m^0.5）相比，提升了65%。上述工作为高性能玻璃陶瓷的研制提供了一种新的思路。

关键词

钇铝硅酸盐 / 玻璃陶瓷 / 断裂韧性 / 硬度

Abstract

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Introduction

Yttrium aluminum silicate (YAS) glass ceramics, known for their high-temperature resistance, excellent hardness, and mechanical strength, attract wide attention as coating materials for bonding or protecting silicon carbide ceramics. The precipitation of the y-Y₂Si₂O₇ crystalline phase in YAS glass, particularly in comparison with SiC, is advantageous due to the matched coefficients of thermal expansion between y-Y₂Si₂O₇ and SiC. This often leads to its use as a sintering aid or in anti-oxidation coatings for SiC. A glass composition with reported proportions of 22Y₂O₃-19Al₂O₃-59SiO₂ (in mole) has been designed to selectively precipitate only the y-Y₂Si₂O₇ crystalline phase through process engineering, achieving a softening temperature exceeding 1 400 ℃. However, this glass composition initially undergoes a droplet-type phase separation, resulting in the precipitation of y-Y₂Si₂O₇ crystals in regions enriched with Y₂O₃ and SiO₂. The large gap between these two phase-separated regions leads to non-uniform distribution of y-Y₂Si₂O₇ grain sizes. The cross-sectional morphology exhibits a fibrous structure, which may affect the mechanical properties of the glass ceramics. Compared to fibrous structures, spherical grains have a higher stress distribution, providing the glass ceramics with greater strength. Previous studies have shown that TiO₂ and CaF₂ are unsuitable as nucleating agents for achieving uniform and fine grains in YAS glass. In this study, a base glass has a composition of 22Y₂O₃·19Al₂O₃·59SiO_2., The addition of ZnO into the base glass was found to inhibit large-sized phase separation in YAS glass, resulting in a significant refinement of precipitated grain sizes. This led to a substantial improvement in the fracture toughness of the glass ceramics. By observing the crack propagation patterns in the glass ceramics, the toughening mechanism has been elucidated. Methods On the basis of the glass composition 22Y₂O₃·19Al₂O₃·59SiO₂, a series of glasses with varying compositions, 2xZnO·22Y₂O₃·(19-x)Al₂O₃·59SiO₂ (2x=0, 3, 6, 12, 18, in mole), were obtained by gradually replacing Al₂O₃ with ZnO at a ZnO∶Al₂O₃ ratio of 2∶1. The glasses were subjected to a nucleation temperature (T_g+30 ℃) heat treatment for 3 h, followed by ramping to the crystallization peak temperature (T_c) and holding for 2 h to obtain glass ceramics for testing. Characteristic temperatures of the glasses were determined using DSC at a heating rate of 10 K/min. The glass ceramics, after fine polishing, were etched for 60 s in a 4% HF solution (volume fraction) and then subjected to SEM testing. Vickers hardness of the samples was measured under a 2.94 N load. Fracture toughness (K_Ic) of the samples was determined under the ASTM C-1421-01b standard.

Results and discussion

As the amount of ZnO gradually increases, the glass transition temperature (T_g) and T_c of the glass decrease progressively. The addition of ZnO reduces both T_g and T_c of the YAS glasses, which is advantageous for lowering the sealing temperature when used in conjunction with SiC ceramics. XRD patterns, SEM images, and EDS patterns confirm that the mechanism for the precipitation of y-Y₂Si₂O₇ in 22Y₂O₃·19Al₂O₃·59SiO₂ glass belongs to crystallization through phase separation. After the addition of ZnO to YAS glass, nearly spherical grains are precipitated, and the distribution of grains becomes more uniform. With increasing ZnO content, the grain size gradually decreases. The addition of ZnO has a minor impact on the hardness and density of both YAS glass and glass-ceramics. However, a significant improvement is observed in the fracture toughness of the glass ceramics, showing a 65% increase for the glass ceramic containing 18% ZnO compared to the YAS glass ceramic. In glass ceramics formed through phase separation and grain growth, both the size and distribution of grains are uneven. Cracks propagate in a straight-line manner, resulting in longer crack lengths under the same load. In contrast, when cracks propagate in glass ceramics with similar and evenly distributed grain sizes, numerous circumferential cracks around grains occur, leading to increased energy consumption during the crack propagation process and resulting in relatively shorter crack propagation distances.

Conclusions

As ZnO gradually replaces Al₂O₃, both the T_g and T_c of YAS glasses decrease. This leads to reduce the sealing temperature when used as sealing materials. With the addition of ZnO, the crystal phases deposited from the YAS glasses transitions from only the y-Y₂Si₂O₇ grains to two phases, i.e., ZnAl₂O₄ and y-Y₂Si₂O₇. The content of precipitated ZnAl₂O₄ phase increases with the gradual introduction of ZnO. Although no significant increase in hardness was observed following the compositional change from 0 to 18% of ZnO (in mole), a distinct enhancement of about 1 GPa in hardness after crystallization occurs for the glass with ZnO. Despite a decrease in K_Ic of YAS glass from 0.82 MPa·m^0.5 to 0.71 MPa·m^0.5 with the addition of ZnO, the prepared glass ceramics with 18% ZnO (in mole) shows a significant enhancement of K_Ic, reaching a maximum value of 1.92 MPa·m^0.5. The microscopic mechanisms of this enhancement was then revealed by further investigation using SEM.

Key words

yttrium aluminosilicate / glass-ceramic / fracture toughness / hardness

引用本文

郑庆双, 陈胜林, 乔昂, 王觅堂, 陶海征. 含锌钇铝硅酸盐玻璃的晶化特征和力学性能. 硅酸盐学报, 2024 , 52 (8) : 2495 -2501 . DOI: 10.14062/j.issn.0454-5648.20230897

Qingshuang ZHENG, Shenglin CHEN, Ang QIAO, Mitang WANG, Haizheng TAO. Crystallization Behavior and Mechanical Properties of Zinc-Containing Yttrium Aluminosilicate Glasses[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (8) : 2495 -2501 . DOI: 10.14062/j.issn.0454-5648.20230897

基金

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国家自然科学基金(52172007; 51974168; 51662033)
江苏省碳达峰碳中和科技创新专项(BE2022035)

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2024年第52卷第8期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230897

接收时间：2023-11-22
首发时间：2026-10-22
出版时间：2024-08-20

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收稿日期：2023-11-22
修回日期：2023-12-24

基金

国家自然科学基金(52172007; 51974168; 51662033)

江苏省碳达峰碳中和科技创新专项(BE2022035)

作者信息

^1．武汉理工大学，硅酸盐建筑材料国家重点实验室，武汉 430070

^2．上海理工大学材料与化学学院，上海 200093

通讯作者:

陶海征（1973—），男，博士，教授。

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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