碳化硅（SiC）纤维增强陶瓷基复合材料具有强度高，热稳定性好，耐腐蚀，抗氧化等优良性能，可作为结构及功能一体化吸波隐身材料，在航空航天、能源等高科技领域有广阔的发展前景。本研究以SiC纤维作为复合材料的增强体和吸波剂，以氮化硅（Si3N4）作为复合材料的基体，在基体中引入硼粉（B）原位氮化生成BN调节纤维与基体的结合力，最终通过反应烧结法制备SiC纤维增强陶瓷基复合材料。研究了B原位氮化对基体氮化率、相组成、微观结构、力学性能、介电性能以及可加工性能等的影响，同时探究了B原位氮化对复合材料性能的影响。研究结果表明： ZrO2作为催化剂，提高了基体的氮化率。成型压力为8MPa的条件下，B含量为...Silicon carbide (SiC) fiber reinforced ceramic matrix composites are advanced absorbing composite materials with high strength, good thermal stability, corrosion resistance, oxidation resistance and other excellent performance. Its have potential applications in the field of aerospace and energy. In this study, SiC fibers are used as the reinforcement and microwave absorbing agent and silicon nitr...学位：工程硕士院系专业：材料学院_工程硕士(材料工程)学号：2072014115010

李永伟

English

Xiamen University Institutional Repository

  学校编码：10384                                  分类号    密级     学    号：20720141150109                              UDC        硕  士  学  位  论  文   硼原位氮化制备含硼氮化硅陶瓷基复合材料 Preparation of boron-containing silicon nitride ceramic matrix composites by boron in situ nitridation  李永伟  指导教师姓名：张  颖  教授               唐学原 助理教授 专 业 名 称：材 料 工 程 论文提交日期：2017年     月 论文答辩日期：2017年     月 学位授予日期：2017年     月  答辩委员会主席： 评    阅    人： 2017 年 5 月 厦门大学博硕士论文摘要库 2   厦门大学博硕士论文摘要库  厦门大学学位论文原创性声明  本人呈交的学位论文是本人在导师指导下,独立完成的研究成果。本人在论文写作中参考其他个人或集体已经发表的研究成果，均在文中以适当方式明确标明，并符合法律规范和《厦门大学研究生学术活动规范（试行）》。 另外，该学位论文为（                            ）课题（组）的研究成果，获得（               ）课题（组）经费或实验室的资助，在（               ）实验室完成。（请在以上括号内填写课题或课题组负责人或实验室名称，未有此项声明内容的，可以不作特别声明。） 厦门大学博硕士论文摘要库厦门大学博硕士论文摘要库   厦门大学学位论文著作权使用声明  本人同意厦门大学根据《中华人民共和国学位条例暂行实施办法》等规定保留和使用此学位论文，并向主管部门或其指定机构送交学位论文（包括纸质版和电子版），允许学位论文进入厦门大学图书馆及其数据库被查阅、借阅。本人同意厦门大学将学位论文加入全国博士、硕士学位论文共建单位数据库进行检索，将学位论文的标题和摘要汇编出版，采用影印、缩印或者其它方式合理复制学位论文。 本学位论文属于： （     ）1.经厦门大学保密委员会审查核定的保密学位论文，于  年   月   日解密，解密后适用上述授权。 （       ）2.不保密，适用上述授权。 （请在以上相应括号内打“√”或填上相应内容。保密学位论文应是已经厦门大学保密委员会审定过的学位论文，未经厦门大学保密委员会审定的学位论文均为公开学位论文。此声明栏不填写的，默认为公开学位论文，均适用上述授权。）                                声明人（签名）： 年   月   日   厦门大学博硕士论文要库厦门大学博硕士论文摘要库摘要   I  摘要 碳化硅（SiC）纤维增强陶瓷基复合材料具有强度高，热稳定性好，耐腐蚀，抗氧化等优良性能，可作为结构及功能一体化吸波隐身材料，在航空航天、能源等高科技领域有广阔的发展前景。本研究以 SiC 纤维作为复合材料的增强体和吸波剂，以氮化硅（Si3N4）作为复合材料的基体，在基体中引入硼粉（B）原位氮化生成 BN 调节纤维与基体的结合力，最终通过反应烧结法制备 SiC 纤维增强陶瓷基复合材料。研究了 B 原位氮化对基体氮化率、相组成、微观结构、力学性能、介电性能以及可加工性能等的影响，同时探究了 B 原位氮化对复合材料性能的影响。研究结果表明： ZrO2作为催化剂，提高了基体的氮化率。成型压力为 8MPa 的条件下，B 含量为0wt%、5 wt%、10wt%的样品经 1390°C 氮化处理后，氮化率分别为 89.91%，89.15%，87.22%。而未添加 ZrO2的含 B 量为 0wt%、5wt%、10wt%的基体经 1390°C 氮化处理后，氮化率仅为 59.11%，62.43%，64.60%，经 1470°C氮化处理后，氮化率达到 87.91%，85.02%，83.08%。 原位生成的 BN 呈弯曲的片层状，在 Si3N4晶粒周围形成类似于核-壳结构。随着B 原位氮化生成 BN 含量的增加，β-Si3N4相的量增加，基体的孔隙率逐渐增加，弯曲强度逐渐降低。B原位氮化生成的BN有效地改善了基体的机械加工性能及介电性能，在 2-18GHz 的频率下，基体的介电常数和介电损耗正切值随着 B 原位氮化生成 BN量的增加而降低。对于添加 ZrO2的基体，当 B 含量为 10wt%时，基体的介电常数为3.36-3.81，介电损耗正切值为 3.62×10-3-1.38×10-2。而未添加 ZrO2的基体经 1470°C 氮化处理后才充分氮化，B 含量为 10wt%的基体介电常数为 3.26-3.57，介电损耗正切值为 1.01×10-3-1.07×10-2。 原位生成的 BN 改善了纤维与基体的结合状态。未添加 B 的复合材料断面为脆性断裂，无 SiC 纤维拔出，纤维与基体结合较强。添加 B 粉原位生成 BN 后，复合材料断面有明显的 SiC 纤维拔出和解离脱粘，为假塑性断裂行为。在 2-18GHz 的频率下，陶瓷基复合材料介电常数和介电损耗正切值随着 B 原位氮化生成 BN 量的增加而下降。此外，提高 SiC 纤维体积分数后，介电常数和介电损耗正切值也随之增加。 关键词：复合材料；反应烧结；原位氮化；介电性能  厦门大学博硕士论文摘要库厦门大学硕士学位论文 II  Abstract Silicon carbide (SiC) fiber reinforced ceramic matrix composites are advanced absorbing composite materials with high strength, good thermal stability, corrosion resistance, oxidation resistance and other excellent performance. Its have potential applications in the field of aerospace and energy. In this study, SiC fibers are used as the reinforcement and microwave absorbing agent and silicon nitride (Si3N4) is used as the matching matrix. The SiC/Si3N4 composite is fabricated by reactive sintering, BN synthesized by boron in situ nitriding in the matrix to adjust the interfacial properties between the fiber and the matrix. The effects of boron content on the nitriding rate, phase composition, microstructure, mechanical properties, machinability and dielectric properties of the matrix were studied. At the same time, the effect of boron in situ nitriding on the properties of the composite was researched.  The results show that ZrO2 can improve the nitridation rate of the matrix, The nitriding rates were 89.91%, 89.15%, 87.22% after 1390°C nitriding with boron boron 0, 5 and 10 mass fraction mass fraction.However, The nitriding rate was only 59.11%, 62.43% and 64.60% after nitriding without ZrO2 addition by boron 0, 5 and 10 mass fraction, it reached 87.91%, 85.02%, 83.08% after nitriding at 1470°C. The curved BN coats the Si3N4 grains to form a shell-core structure.The in-situ nitridation of boron to form BN affects the β-Si3N4 and effectively improves the machinability and dielectric properties of the matrix. With the increase of boron mass fraction, the porosity of matrix gradually increases while the bending strength decreases. Boron can improve the dielectric properties and machinability processing performance. For the matrix with ZrO2 and 10% mass fraction boron, the dielectric constant is 3.36-3.81 and loss tangent is 3.62×10-3-1.38×10-2 at a frequency range of 2-18 GHz. While the matrix without ZrO2 achieves full nitriding until 1470°C. The dielectric constant and loss tangent are 3.26-3.57 and 1.01×10-3-1.07×10-2, respectively. The BN improves the binding force of the fiber to the substrate. The fracture surface of composite without boron show a brittle fracture behavior without fibers being pulled out. Oppositely, the composite with boron addition has obvious SiC fiber extraction, dissociation 厦门大学博硕士论文摘要库Abstract III  and debonding, which shows obviously pseudoplastic fracture behavior. In addition. In addition, the dielectric constant and loss tangent of composite increase with the increasing the volume fraction of SiC fibers. Key words: composites; reactive sintering; in situ nitriding; dielectric properties   厦门大学博硕士论文摘要库厦门大学博硕士论文摘要库目录 I  目录 摘要 ....................................................................................................................I 英文摘要 .......................................................................................................... II 第一章 引言 ..................................................................................................... 1 1.1 氮化硼/氮化硅陶瓷简介 ....................................................................................... 3 1.1.1 氮化硅 ......................................................................................................... 3 1.1.2 氮化硼 ......................................................................................................... 5 1.1.3 原位制备氮化硼/氮化硅陶瓷 .................................................................... 6 1.2 碳化硅纤维增强陶瓷基复合材料研究进展 ...................................................... 11 1.2.1 碳化硅纤维增强陶瓷基复合材料的制备方法 ....................................... 13 1.2.2 氮化硼界面层 ........................................................................................... 15 1.3 存在的问题 .......................................................................................................... 17 1.4 本课题的研究目标及内容 .................................................................................. 18 第二章 实验 ................................................................................................................... 19 2.1 实验原料及设备 .................................................................................................. 19 2.2 样品制备 .............................................................................................................. 23 2.2.1 硼原位氮化制备氮化硼/氮化硅陶瓷基体 .............................................. 23 2.2.2 硼原位氮化制备碳化硅纤维增强氮化硼/氮化硅陶瓷基复合材料 ...... 25 2.3 表征方法 .............................................................................................................. 28 2.3.1 元素组成表征 ........................................................................................... 28 2.3.2 结构表征 ................................................................................................... 29 2.3.3 性能表征 ................................................................................................... 29 第三章 结果与讨论 ..................................................................................................... 32 3.1 硼原位氮化制备氮化硼/氮化硅陶瓷基体 .......................................................... 32 3.1.1 成型压力的影响 ....................................................................................... 33 3.1.2 添加 ZrO2制备氮化硼/氮化硅陶瓷基体 ................................................ 34 3.1.3 未添加 ZrO2制备氮化硼/氮化硅陶瓷基体 ............................................ 52  3.1.4 本节小结 ................................................................................................... 60 厦门大学博硕士论文摘要库厦门大学硕士学位论文 II  3.2 硼原位氮化制备碳化硅纤维增强氮化硼/氮化硅陶瓷基复合材料 .................. 61 3.2.1 添加 ZrO2制备氮化硼/氮化硅陶瓷基复合材料 .................................... 62 3.2.2 未添加 ZrO2氮化硼/氮化硅陶瓷基复合材料 ........................................ 65 3.2.3 本节小结 ................................................................................................... 70 第四章 结论 ................................................................................................... 71 第五章 对未来工作的建议 ........................................................................... 73 参考文献 ......................................................................................................... 74 硕士期间发表论文 ......................................................................................... 82 致谢 ................................................................................................................. 83     厦门大学博硕士论文摘要库厦门大学硕士学位论文 III  Table of contents Abstract in Chinese ..........................................................................................I Abstract in Englissh ....................................................................................... II Chapter 1 Introduction ................................................................................... 1 1.1 Introduction of Boron Nitride / Silicon Nitride Ceramics ................................. 3 1.1.1 Silicon nitride ............................................................................................... 3 1.1.2 Boron nitride ................................................................................................. 5 1.1.3 In-situ preparation of boron nitride/silicon nitride ceramics ........................ 6 1.2 Research On Silicon Carbide Fiber Reinforced Ceramic Matrix Composites ..................................................................................................................................... 11 1.2.1 Preparation of Silicon Carbide Fiber Reinforced Ceramic Matrix Composites ............................................................................................................................. 13 1.2.2 Interface layer of boron nitride ................................................................... 15 1.3 Existing problems ................................................................................................ 17 1.4 Research purposes and contents ........................................................................ 18 Chapter 2 Experimental ............................................................................................. 19 2.1 Experimental materials and equipment ............................................................ 19 2.2 Composite Preparation ....................................................................................... 23 2.2.1 Preparation of boron nitride / silicon nitride ceramic matrix by in situ nitridation of boron .............................................................................................. 23 2.2.2 Preparation of silicon carbide fiber reinforced boron nitride / silicon nitride ceramic matrix composites by in situ nitridation of boron .................................. 25 2.3 Characterization method .................................................................................... 28 2.3.1 Composition characterization ..................................................................... 28 2.3.2 Structure characterization ........................................................................... 29 2.3.3 Performance characterization ..................................................................... 29 Chapter 3 Results and Discussion ........................................................................... 32 3.1 Preparation of boron nitride / silicon nitride ceramic matrix by boron in situ 厦门大学博硕士论文摘要库Table of Contents IV  nitridation ................................................................................................................... 32 3.1.1 The effect of pressure for sample preparation ............................................ 33 3.1.2 Preparation of boron nitride/silicon nitride ceramic matrix with ZrO2 ...... 34 3.1.3 Preparation of boron nitride/silicon nitride ceramic matrix without ZrO2 . 52 3.1.4 Summary ..................................................................................................... 60 3.2 Preparation of Silicon Carbide Fiber Reinforced Boron Nitride/Silicon Nitride Ceramic Matrix Composites by In situ Nitridation of Boron ............................... 61 3.2.1 Preparation of boron nitride / silicon nitride ceramic matrix composites with ZrO2 ..................................................................................................................... 62 3.2.2 Preparation of boron nitride / silicon nitride ceramic matrix composites without ZrO2 ........................................................................................................ 65 3.2.3 Summary ..................................................................................................... 70 Chapter 4 Conclusions .................................................................................. 71 Chapter 5 Suggestions for future work ....................................................... 73 Reference ........................................................................................................ 74 Published paper ............................................................................................. 82 Acknowledgements ........................................................................................ 83厦门大学博硕士论文摘要库Abstract V    厦门大学博硕士论文摘要库厦门大学博硕士论文摘要库Degree papers are in the “Xiamen University Electronic Theses and Dissertations Database”. Fulltexts are available in the following ways: 1. If your library is a CALIS member libraries, please log on http://etd.calis.edu.cn/ and submitrequests online, or consult the interlibrary loan department in your library. 2. For users of non-CALIS member libraries, please mail to etd@xmu.edu.cn for delivery details.厦门大学博硕士论文摘要库

Preparation of boron-containing silicon nitride ceramic matrix composites by boron in situ nitridation

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Preparation of boron-containing silicon nitride ceramic matrix composites by boron in situ nitridation

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