硅烷偶联剂对制备硅酸锆薄膜及其抗氧化性能的影响

doi:10.15541/jim20170033

摘要/Abstract

摘要：

采用乙酸锆和正硅酸乙酯为原料, 硅烷偶联剂3-氨丙基三乙氧基硅(APTES)为表面改性剂, 通过溶胶-凝胶法制备了致密硅酸锆薄膜。系统研究了APTES的添加对硅酸锆薄膜的晶体结构、显微形貌及其抗氧化性能的影响。实验结果表明, 添加硅酸锆摩尔浓度10mol%的APTES可以制备出纯相的致密硅酸锆薄膜, 超过这一浓度则会出现少量的SiO₂杂质, 同时造成硅酸锆溶胶的黏度迅速升高。AFM测试结果表明添加APTES制备的薄膜更致密平滑。1300℃抗氧化测试102 h后, 未镀膜的碳化硅基底增重0.16%, 相比之下, 添加APTES前后的样品的增重分别为0.08% 和0.03%, 说明添加APTES有利于提高ZrSiO₄薄膜的致密度, 进而提高其抗氧化性能。

关键词: 薄膜, 硅酸锆, 溶胶-凝胶法, 抗氧化

Abstract:

The dense zircon film was prepared via Sol-Gel method using zirconium acetate and tetraethoxysilane as raw materials, and silane coupling agent 3-aminopropyltriethoxysilane (APTES) as surface modifying agent, respectively. Influences of APTES on the phase composition, morphology and antioxidation property of the ZrSiO₄ film were investigated. The experiment results indicated that the pure and dense zircon film was achieved with addition of 10mol% APTES into ZrSiO₄ sol. Once the molar ratio of APTES was beyond 10mol%, the impurity SiO₂ was observed, and the viscosity of the ZrSiO₄ sol increased significantly at the same time. AFM results showed that the smooth and dense film was obtained with APTES addition. After 102 h oxidation cyclic test at 1300℃, uncoated SiC substrate gained weight of 0.16%, while samples coated with ZrSiO₄ thin films only gained weight of 0.08% and 0.03% before and after addition of APTES. In summary, APTES addition is beneficial for the density of ZrSiO₄ thin film, resulting in excellent anti-oxidation property.

Key words: thin film, zircon, Sol-Gel method, anti-oxidation

中图分类号:

TB383

陈婷, 查剑锐, 张筱君, 江伟辉, 江莞, 刘健敏, 吴倩. 硅烷偶联剂对制备硅酸锆薄膜及其抗氧化性能的影响[J]. 无机材料学报, 2017, 32(11): 1154-1158.

CHEN Ting, ZHA Jian-Rui, ZHANG Xiao-Jun, JIANG Wei-Hui, JIANG Wan, LIU Jian-Min, WU Qian. Silane Coupling Agent on Synthesis and Antioxidation Property of Zircon Film[J]. Journal of Inorganic Materials, 2017, 32(11): 1154-1158.

图/表 8

图1 APTES辅助溶胶-凝胶法制备ZrSiO4薄膜的流程图

Fig.1 Schematic of the ZrSiO4 film prepared by APTES-assisted Sol-Gel method

图2 APTES添加量对ZrSiO4薄膜合成的影响

Fig. 2 Influence of APTES content on the synthesis of ZrSiO4 thin film

图3 APTES添加量对ZrSiO4的DTA-TG分析结果的影响

Fig. 3 DTA-TG curves of ZrSiO4 samples with different APTES contents

图4 不同APTES添加量的溶胶黏度-时间曲线

Fig. 4 Time-viscosity curves of ZrSiO4 sol with various APTES contents

图5 ZrSiO4薄膜的AFM图像

Fig. 5 AFM images of ZrSiO4 thin film (a, b) Without APTES; (c, d) With 10mol% APTES

图6 添加APTES制备的 ZrSiO4薄膜断面的面扫描分析结果

Fig. 6 Area scan analysis of the cross section of ZrSiO4 thin film with addition of APTES (a) SEM; (b) Zr; (c) O; (d) Si; (e) Line scan analysis

图7 薄膜质量随氧化时间的变化曲线

Fig. 7 Change of thin film’s weight with oxidation time (a) SiC; (b) SiC coated by ZrSiO4 without APTES-assisted; (c) SiC coated by ZrSiO4 with APTES-assisted

图8 1300℃氧化后样品的SEM照片及其面扫描分析(O元素)结果

Fig. 8 SEM images and area scan analysis for O element of the cross section of the sample after oxidation at 1300℃ (a) (b) SiC; (c) (d) SiC coated by ZrSiO4 without addition of APTES; (e) (f) SiC coated by ZrSiO4 with addition of APTES

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