引用本文:吴玉厚,杨淯淼,闫广宇,王贺,刘鲁生,白旭,张慧森.Si3N4工程陶瓷基底金刚石涂层生长规律及性能[J].中国表面工程,2024,37(1):179~191
WU Yuhou,YANG Miao,YAN Guangyu,WANG He,LIU Lusheng,BAI Xu,ZHANG Huisen.Growth and Properties of Diamond Films on Si3N4 Ceramic Substrates[J].China Surface Engineering,2024,37(1):179~191
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Si3N4工程陶瓷基底金刚石涂层生长规律及性能
吴玉厚1,2, 杨淯淼1,2,3, 闫广宇1,2,3, 王贺1,2, 刘鲁生4, 白旭3, 张慧森1,2,3
1.沈阳建筑大学高档石材数控加工装备与技术国家地方联合工程实验室 沈阳 110168;2.沈阳建筑大学现代建筑工程装备与技术国际合作联合实验室 沈阳 110168;3.沈阳建筑大学机械工程学院 沈阳 110168;4.中国科学院金属研究所沈阳材料科学国家研究中心 沈阳 110016
摘要:
为了避免氮化硅材料因产生裂纹或延伸破裂等造成的失效,利用热丝化学气相沉积法(Hot filament chemical vapor deposition,HFCVD)在氮化硅基底上沉积具有高硬度的金刚石涂层,采用单因素影响试验,分别探究碳源浓度、腔室压力、 基底温度对金刚石成膜过程的影响机制,探究微米和纳米金刚石涂层的最优生长工艺参数。利用拉曼光谱仪(Raman)、X 射线衍射仪(XRD)、扫描电子显微镜(SEM)和原子力显微镜(AFM)对不同参数制备出的金刚石的形核、表面形貌、薄膜质量、表面粗糙度等进行表征,利用洛氏硬度计分析膜基结合力。结果表明,腔室压力越大,活性物质到达基底的动能越小, 不利于金刚石的成核和生长。生长速率和表面粗糙度主要受甲烷浓度的影响:甲烷浓度从 1%到 7%,生长速率从 0.84 μm / h 上升到 1.32 μm / h;表面粗糙度 Ra 从 53.4 nm 降低到 23.5 nm;甲烷浓度过高导致涂层脱落严重,膜基结合力变差;晶面形貌和金刚石含量受到基底温度的影响较为明显,随着温度升高,金刚石质量提高。综合基底温度、腔室压力对金刚石涂层的影响,确定最佳生长温度为 900 ℃,气压为 1 kPa。调节甲烷浓度 1%为微米金刚石;甲烷浓度 5%为纳米金刚石。研究方法可以优化在陶瓷基底上制备具有优异性能的金刚石薄膜的制备参数。
关键词:  金刚石涂层  氮化硅  热丝化学气相沉积法(HFCVD)
DOI:10.11933/j.issn.1007-9289.20220518001
分类号:TQ174
基金项目:国防科技创新特区计划(20-163-00-TS-006-002-11);国家自然科学基金(51975388);辽宁省科技计划(2018106007);沈阳市科技计划(18-400-6-05)
Growth and Properties of Diamond Films on Si3N4 Ceramic Substrates
WU Yuhou1,2, YANG Miao1,2,3, YAN Guangyu1,2,3, WANG He1,2, LIU Lusheng4, BAI Xu3, ZHANG Huisen1,2,3
1.National-Local Joint Engineering Laboratory of NC Machining Equipment and Technology ofHigh-Grade Stone, Shenyang Jianzhu University, Shenyang 110168 , China;2.Joint International Research Laboratory of Modern Construction Engineering Equipment and Technology,Shenyang Jianzhu University, Shenyang 110168 , China;3.School of Mechanical Engineering, Shenyang Jianzhu University, Shenyang 110168 , China;4.Shenyang National Laboratory for Materials Science, Institute of Metal Research,Chinese Academy of Sciences, Shenyang 110016 , China
Abstract:
To avoid failures such as cracking or elongation of silicon nitride (Si3N4), it is possible to use erosion-resistant diamond films. Diamond has very high hardness, high thermal conductivity, and a low friction factor, and its coefficient of thermal expansion is very close to that of Si3N4, which provides good adhesion, low residual stresses, and significantly increases the service life when deposited on Si3N4 substrates. Single-layer diamond films were deposited on Si3N4 substrates using hot filament chemical vapor deposition (HFCVD). A single variable control method was used to investigate the effect of the carbon source concentration, chamber pressure, and substrate temperature on the nucleation and growth of diamond on Si3N4 and to investigate the optimal parameters for the growth of micro- and nanodiamond films. Each of the three factors is defined as three series, where methane was selected as the carbon source. Series A represents the variation in the methane concentration, series B represents the variation in the chamber pressure, and series C represents the variation in the substrate temperature. The diamond surface and cross-sectional morphology, coating quality, and surface roughness of the diamonds in the as-deposited diamond films prepared with different parameters were characterized using Laser Raman Spectrometry (Raman), X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), and Atomic Force Microscopy (AFM). Indentation experiments were carried out using a Rockwell hardness tester to observe the cracks in the films and the area of delamination, in order to analyze the adhesion force between the diamond films deposited with different parameters and the substrates The results are summarized as follows: (1) The growth rate and surface roughness are mainly affected by the methane concentration: the growth rate increased from 0.84 μm / h to 1.32 μm / h when the methane concentration was increased from 1% to 7%, whereas the surface roughness (Ra) decreased from 53.4 nm to 23.5 nm. As the methane concentration increased, more carbon radicals were deposited in the films; however, secondary nucleation tended to occur and the non-diamond phase increased, resulting in a reduction in the surface roughness and film quality. Excessive methane concentration reduces the mechanical strength and hardness of the films themselves, decreasing the adhesion force with the substrate and increasing the delamination of the films when stressed by forces. (2) The chamber pressure affects the kinetic energy of the active material within the reaction chamber that reaches the substrate. As the pressure increased, the kinetic energy decreased, which is unfavorable for diamond nucleation and growth. Although the diamond content was highest in the films grown at 2 kPa, analysis of the other factors collectively showed that the adhesive force for the substrate and surface morphology of the films grown at 2 kPa were not as good as those of the diamond films deposited at 1 kPa. (3) The surface morphology and diamond phase composition of the films were significantly influenced by the substrate temperature. At 800 ℃, the surface of the coating could not form complete and continuous diamond crystals, many cavities appeared and no obvious diamond characteristic peaks appeared in the Raman spectra. Therefore, a temperature below 800 ℃ is not suitable for the growth of diamond. When the temperature was increased from 850 ℃ to 900 ℃, the nucleation density of the diamond surface and the quality increased. In addition, the content of the non-diamond phase was reduced, and the surface had a more stable (111) crystalline structure, which enables the growth of high-quality films and provides a stronger adhesion force to the substrate. (4) The optimum growth temperature and air pressure were 900 ℃ and 1 kPa, respectively. The methane concentration in the reaction chamber was adjusted to control the diamond grain size and sp2 carbon content, giving films with 1% microdiamond and 5% nanodiamond. The preparation parameters for diamond films with excellent properties on ceramic substrates were optimized using three-factor-coupled experiments.
Key words:  diamond films  silicon nitride  hot filament chemical vapor deposition (HFCVD)
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