臺灣博碩士論文加值系統

碳化矽為現代陶瓷中研究關注的焦點之一，碳化矽陶瓷相較於其他陶瓷材料擁有更好的機械強度、耐熱性耐腐蝕性極優良的熱傳導性，其中多孔碳化矽材料有著更為優異之性能，本研究試著發展一種超高孔隙率的多孔碳化矽陶瓷材料，作為散熱材之應用。
本研究將180-250µm的碳化矽顆粒與不同比例之(SiO2-BaO-ZnO)玻璃分別以(3、6、9、12)wt%混合，再加入羧甲基纖維素水溶液之後以行星式球磨2小時製成漿料，再經由烘箱進行8小時的乾燥將是片中的水份完全烘乾，再經由石膏模以類鑄漿成型法製成生胚，在空氣中以(900、850、825)°C進行30分鐘的常壓燒結，製成超高孔隙率碳化矽陶瓷。
由SEM/BSE-EDS觀察橫截面得知以此方式及溫度燒結下，玻璃能包覆在碳化矽的顆粒表面，並做為顆粒與顆粒之間的接合材料，並在表面形成許多針狀析出物，藉以製成多孔陶瓷。以XRD分析後，此多孔碳化矽大致上含有4H、6H及少量的15R碳化矽，將SEM影像以ImageJ影像軟體進行分析得出多孔碳化矽陶瓷之平均孔隙率約為60%左右，最高值可以達到70%(825°C、12wt%玻璃)，以萬能試驗機進行抗壓強度測試，顯示出在超高孔隙率下抗壓強度最高可以達到10.5MPa(825°C、12wt%玻璃)，以熱像儀測試熱性值，與市售之鋁製散熱片做為對比顯示出，將熱帶走的能力較市售鋁製散熱片較好些，由實驗得知以(SiO2-BaO-ZnO)玻璃做為黏結劑製作超高孔隙率碳化矽陶瓷，燒結溫度在相較低溫的825°C下(SiO2-BaO-ZnO)玻璃添加量在9wt%-12wt%，以此參數製作之超高孔隙率碳化矽陶瓷有較佳化的孔隙率、抗壓強度及熱性質。

Silicon carbide is one of the main research fields in contemporary ceramics. Silicon carbide ceramics have superior mechanical strength, resistance to heat and corrosion, and thermal conductivity compared to other ceramic materials. Porous silicon carbide materials have the best properties among them. In this study, we attempted to develop an ultra-porous silicon carbide ceramic material for use as a heat dissipation material.
In this study, silicon carbide particles of 180-250µm were mixed with different proportions of (SiO2-BaO-ZnO) glass at (3, 6, 9, 12) wt%, then carboxymethyl cellulose aqueous solution was added, followed by planetary ball milling. Slurry was made in 2 hours, then dried in an oven for 8 hours to completely dry the moisture in the sheet, then passed through a plaster mold to make a green embryo by a slurry-like molding method, and in the air at (900, 850, 825) °C for 30 minutes under atmospheric pressure to produce ultra-high porosity silicon carbide ceramics.
From SEM/BSE-EDS cross-sectional observations, it is known that according to this method and sintering temperature, glass can coat the surface of silicon carbide particles and act as the bonding material between particles, and that numerous needle-like precipitates form on the surface of the material to create porous ceramics. According to an XRD analysis, the porous silicon carbide consists of approximately 4H, 6H, and a small quantity of 15R silicon carbide. ImageJ imaging software is used to analyze the SEM image, which reveals that the average porosity of the porous silicon carbide ceramic is approximately 60 %, with the highest value being as 80 %. Under ultra-high porosity, it reaches 70% (825°C, 12wt % glass) and the compressive strength test using a universal testing machine indicates that the compressive strength can reach up to 10.5MPa (825°C, 12wt% glass). The thermal imager evaluated the thermal value and, in comparison to the commercially available aluminum heat sink, determined that the ability to remove heat is superior to that of the commercially available aluminum heat sink. For the production of ultra-high porosity silicon carbide ceramics for the binder, the sintering temperature is at a relatively low 825°C (SiO2-BaO-ZnO) with a glass content of 9wt% -12wt%, and the ultra-high porosity carbide produced by this parameter. The porosity, compressive strength, and thermal properties of silicon ceramics are optimized.

摘要....................................................................i
Abstract................................................................iii
誌謝....................................................................v
目錄....................................................................vi
表目錄..................................................................ix
圖目錄..................................................................x
第一章 緒論..............................................................1
1.1前言..................................................................1
1.2研究動機..............................................................2
第二章 理論基礎及文獻回顧..................................................4
2.1 多孔陶瓷介紹..........................................................4
2.1.1多孔陶瓷概述.........................................................4
2.1.2多孔陶瓷原材介紹......................................................5
2.1.3多孔陶瓷製備..........................................................10
2.2 陶瓷燒結實務...........................................................11
2.2.1陶瓷燒結理論..........................................................11
2.2.2燒結的基本原理及機構...................................................13
2.2.3燒結種類及技術.........................................................17
2.2.4液相燒結...............................................................21
2.3陶瓷材料特性及其檢測......................................................23
2.3.1粉體特性及檢測..........................................................23
2.3.2陶瓷密度及孔隙率檢測.....................................................25
2.3.3阿基米德法..............................................................28
2.3.4陶瓷材料之機械性質檢測...................................................28
2.3.5物理及化學特性..........................................................32
2.4陶瓷材料的熱性質與其測試方式................................................35
2.4.1熱傳導..................................................................35
2.4.2熱膨脹..................................................................36
2.4.3比熱....................................................................37
第三章 研究方法及步驟..........................................................38
3.1實驗材料...................................................................38
3.1.1 實驗粉末基材............................................................38
3.1.2 實驗添加劑..............................................................38
3.2 實驗流程..................................................................40
3.2.1 實驗基材製備.............................................................40
3.2.2多孔碳化矽................................................................40
3.3 實驗設備..................................................................43
3.3.1 高溫燒結爐(High temperature furnace).....................................43
3.3.2 行星式球模機(Planetary Ball Mills).......................................43
3.4分析儀器及原理..............................................................45
3.4.1 掃描式電子顯微鏡 (Scanning Electron Microscope, SEM).....................45
3.4.2 能量散射X射線光譜儀 (Energy Dispersive Spectroscopy, EDS)................45
3.4.3 X光繞射分析儀 (X-ray Diffraction, XRD)...................................46
3.4.4 ImageJ圖像分析軟體.......................................................46
3.4.5 紅外線熱像儀(IR thermal imager)..........................................47
3.4.6 萬能試驗機(Universal testing machine)....................................48
3.5實驗參數及試片命名..........................................................52
第四章 實驗結果與討論..........................................................53
4.1碳化矽基材.................................................................53
4.2 900°C燒結多孔碳化矽陶瓷....................................................56
4.2.1 橫截面形貌觀察(SEM/BSE/EDS)..............................................56
4.2.2 X光繞射分析(XRD).........................................................61
4.2.3抗壓測試(Compression)....................................................62
4.2.4 熱性值測試..............................................................64
4.2.5 ImageJ圖像軟體孔隙率分析.................................................67
4.3 850°C燒結多孔碳化矽陶瓷....................................................70
4.3.1橫截面形貌觀察(SEM/BSE/EDS)...............................................70
4.3.2 X光繞射分析(XRD).........................................................75
4.3.3抗壓測試(Compression)....................................................76
4.3.4 熱性值測試...............................................................78
4.2.5 ImageJ圖像軟體孔隙率分析.................................................81
4.4 825°C燒結多孔碳化矽陶瓷....................................................84
4.4.1橫截面形貌觀察(SEM/BSE/EDS)...............................................84
4.4.2 X光繞射分析(XRD).........................................................89
4.4.3抗壓測試(Compression)....................................................90
4.4.4熱性值測試................................................................92
4.4.5 ImageJ圖像軟體孔隙率分析.................................................95
4.5 孔隙率對250秒後恆溫溫度及抗壓強度之探討......................................98
4.5.1孔隙率對抗壓強度探討......................................................98
4.5.2孔隙率對250秒後恆溫溫度探討................................................99
第五章 結論...................................................................103
參考文獻.....................................................................104
Extended Abstract............................................................109

[1]Reza Taheri-Ledair,1- Classification of micro and nanoscale composites, Heterogeneous Micro and Nanoscale Composites for the Catalysis of Organic Reactions,Mirco and Nano Technologies,Pages1-21,(2022)
[2]Yu Chen,NannanWang,Oluwafunmilola Ola,Yongde Xia,Yanqiu Zhu, Porous ceramics: Light in weight but heavy in energy and environment technologies, Materials Science and Engineering: R: Reports,Volume 143 100589,(2021)
[3]Atanu Dey,Nijhuma Kayal,Omprakash Chakrabarti, Preparation of porous SiC ceramics by an infiltration technique, Ceramics International, Volume 37, Issue 1,Pages 223-230,(2021)
[4]Che-Yuan Liu, Wei-Hsing Tuana,Shih-Chieh Chenb, Preparation of porous SiC ceramics for thermal dissipation purposes, Ceramics International, Volume 41, Issue 3, Part B, Pages 4564-4568,(2015)
[5]Jung-Hye Eom, Young-Wook Kim, Santosh Raju, Processing and properties of macroporous silicon carbide ceramics: A review, Journal of Asian Ceramic Societies 1-220-242(2013)
[6]Dulal Das,Nijhuma Kayal,Review On Oxide Bonded Porous SiC Ceramics:Processing,Properties and Applications, Journal of Materials Science Research and Reviews,2(2):1-25.(2019)
[7]汪建民，陶瓷技術手冊(下)，第二十二章碳化矽，p745-p760(1998)
[8]Philip J.Guichelaar, Carbide,Nitride and Boride Materials Synthesis and Processing(Acheson Process),pp115-129(1997)
[9]Henry N. Baumann,JR, The Relationship of Alpha and Beta Silicon Carbide,Jornal of The Electrochemical Society,Volume99,N0.3(1952)
[10]D.C.Phillips,Concise Encyclopedia of Advanced Ceramic Materials,Fiber-Reinforced Ceramics,pp155-160(1991)
[11]Xinbin Lao,Xiaoyang Xu,Weihui Jiang,Jian Liang,Lifeng Miao,Guanghui Leng,Effect of various sintering additives on the properties of β-SiAlON-SiC ceramics obtained by liquid phase sintering,Ceramics International,47-13078-13092(2021)
[12]Anne Aimable,Thierry Chartier,Organic Additives in Ceramic Processing,Encyclopedia of Materials:Techical Ceramics and Glasses,Volume1pp103-111(2021)
[13]Giorgio Pia,Ludovica Casnedi,Ulrico Sanna,Porous ceramic materials by pore-forming agent method:An intermingled fractal units analysis and procedure to predict thermal conductivity,Ceramics International,Volume41Pages6350-6357(2015)
[14]Dehua Liang,Jiguang Huang,Heng Zhang,Hongming Fu,Yuntao Zhang,Haiping Cheng,Influencing factors on the performance of tubular ceramic membrane supports prepared by extrusion,Ceramics International 47-10464-10477(2021)
[15]Lei Yuan,Endong Jin,Chaoyue Li,Zhenli Liu,Chen Tian,Beiyue Ma,Jingkun Yu,Preparation of calcium hexaluminate porous ceramics by novel pectin based gelcasting freeze-drying method, Ceramics International,47-9017-9023(2021)
[16]Mengyong Sun,Shuangyan Yang,Xiaoju Gao,Peng Man,Junfeng Qu,Wu Zhang,Shaoqing Yin,Laifei Cheng,Structure and performance control of porous Si3N4 ceramics fabricated by freeze-drying process, Ceramics International, Volume47,Issue6,pages8159-8174(2021)
[17]Mamoru Omori,Humihiko Takei,Pressureless Sintering of SiC,Journal of the American Ceramic Society,Volume 65 Issue6 Pages c92-c92(1982)
[18]Thomas B.Troczynski,Patrick S.Nicholson, Effect of Additives on the Pressureless Sintering of Aluminum Nitride between 1500°C and 1800°C, Journal of the American Ceramic Society, Volume72 Issue8,Pages1488-1491(1989)
[19]Da Li,Shaou Chen,Weiquan Shao,Xiaohui Ge,Yongcheng Zhang,Shasha Zhang,Densification evolution of TiO2 ceramics during sintering based on the master sintering curve theory,Materials Letters Volume 62 Issue 6-7 Pages 849-851(2008)
[20]J Liebertz,Uniaxial hot-pressing of fine-particle,pure barium titanate without die,International Journal of High Technology Ceramics,Volume 3,Issue2,Pages153-163(1987)
[21]Biao Hu,Gaoshen Cai,Jubo Fu,Yanxi Xin,Dongxing Zhang,Yongfeng Yuan,Shaoyi Guo,Densification behavior of tungsten alloy powders during hot isostatic pressing,Materials Today Communications31 103576(2022)
[22]C.Hu,F.Li,D.Qu,Q.Wang,R.Xie,H.Zhang,S.Peng,Y.Bao,Y.Zhou,8-Developments in hot pressing(HP)and hot isostatic pressing(HIP)of ceramic matrix composites,Advances in Ceramic Matrix Composites,Pages164-189(2014)
[23]Carmen Baudin,Reaction Sintering,Encyclopedia of Materials:Technical Ceramics and Glasses,Volume1,Pages278-285(2021)
[24]Tristan Garnault,Dider Bouvard,Jean-Marc Chaix,Sylvain Marinel,Christelle Harnois,Is direct microwave heating well suited for sintering ceramics? Ceramic International Volume47,Issue12,Pages 16716-16729(2021)
[25]Hanqin Liang,Xiumin Yao,Xuejian Liu,Zhengren Huang,The effect of powder bed on the liquid phase sintering of a-SiC,Materials and Design56,1009-1013(2014)
[26]A.C.Santos,S.Ribeiro,Liquid phase sintering and characterization of SiC ceramics,Ceramics International 44, 11048-11059(2018)
[27]S.Ribeiro,L.A.Genova,G.C.Ribeiro,M.R.Oliveira,A.H.A.Bressiani,Effect of heating rate on the sharinkage and microstructure of liquid phase sintered SiC ceramic,Ceramic International Volume 42,Issue 15,Pagse 17398-17404(2016)
[28]R.M.German,S.Farooq,C.M.kipphut,Kinetics of liquid sintering,Materials Science and Engineering:A,Volumes 105-106,Pages 215-224(1988)
[29]汪建民，粉末冶金技術手冊，第三章粉末之特性和測試，Pages29-34(1998)
[30]Pamella Jureves Esteves,Vanesa Seriacopi,Marcelo Camargo,Severo de Macedo,Roberto Martins Souza,Cherlio Scandian,Combined effect of abrasive particle size distribution and ball material on the wear coefficient in micro-scale abrasive wear tests,Wear,Wear 476,(2021)
[31]Davit Hakobyan,Maher Hamdi,Olivier Redon,Anthony Ballestero,Alexis Mayaudon,Laurence Boyer,Olivvier Durand,Emmanuel Abraham,Non-destructive evaluation of ceramic porosity using teraherz time-domain spectroscopy,Journal of the European Ceramic Society, 42 525-533 (2022)
[32]Ying chang,Huihu Wang,Qinbiao Zhu,Ping Luo,Shijie Dong,Theoretical calculation and analysis of ZrO2 spherical nanometer powders,Journal of Advanced Ceramics 2,21-25 (2013)
[33]Xuexiang Ge,Mingkai Zhou,Huaide Wang,Lishun Chen,Xian Li,Xiao Chen,Effects of flux components on the properties and pore strucrure of ceramic foams produced from coal bottom ash,Ceramics International 45,12528-12534,(2019)
[34]Faisal A.AlMarzooqi,M.R.Bilad,Bilad Mansoor,Hassan A.Arafat,A comparative of image analysis and porometry techniques for characterization of porous membranes,Journal of Materials Science 51,(2016)
[35]Wessel W.Wits,Simone Carmignato,Filippo Zanini,Tom H.J.Vaneker,Porosity testing methods for the quality assessment of selective laser melthed parts,CIRP Annals,Voulme 65,Issue 1,Pages201-204,(2016)
[36]Thibaut de Terris,Olivier Andreau,Patrice Peyre,Frederic Adamski,Imade Koutiri,Cyril Gorny,Corinne Dupuy,Optimization and comparison of porosity rate measurement methods of Selective Laser Melthed metallic parts,Additive Manufacturing,Voiume 28,Pages802-813,(2019)
[37]Martin Dannemann,Klaudiusz Holeczek,Jana Leimert,Stefan Friebe,Niels Modler,Adapted measuring sequence for the determination of directional-dependent dynamic material properties using a bending resonance method,Polymer Testing 79,106044,(2019)
[38]Xianxi Li,Liwen Yan,Yibo Zhang,Xukun Yang,Anran Guo,Haiyan Du,Feng Hou,Jiachen Liu,Lightweight porous silica ceramics with ultra-low thermal conductivitiy and enhanced compressive strength,Ceramics Interantional 48 9788-9796,(2022)
[39]Tapatee Kundu Roy,Estimation of fracture toughness in ZnO ceramics from indentation crack opening displacement measurements,Measurement,Volume 137 Pages 588-594,(2019)
[40]D.Chicot,D.Mercier,F.Roudet,K.Sliva,J.Lesage,Comparison of instrumented Knoop and Vickers hardness measurements on various soft materials and hard ceramics,Journal of the European Ceramic Dociety,Volume 27,Issue 4,Pages 1905-1911,(2007)
[41]Guixiang Liu,Bo Dai,Yong Ren,Kuibao Zhang,Dengjian Ye,Chunfeng Hu,Weitong Zhang,Shuai Fu,Microstructure and magnetic of nickel-zinc ferrite ceramics fabricated by spark plasms sintering,Ceramics International 48,10412-10419(2022)
[42]Soˇna Hˇríbalov ́a, Willi Pabst, Modeling light scattering by spherical pores for calculating the transmittance of transparent ceramics – All you need to know, Journal of the European Ceramic Society 41 2169-2192,(2021)
[43]E.Z.Meilikhov, Critical currents and current-voltage characteristics of high temperature superconducting ceramics, Applied Superconductivity,Volume 4 Issues 1-2,Pages61-78
[44]ZhongpingYao, Yongjun Xu,Yunfu Liu,Dali Wang,Zhaohua Jiang,Fuping Wang, Structure and corrosion resistance of ZrO2 ceramic coatings on AZ91D Mg alloys
by plasma electrolytic oxidation, Journal of Alloys and Compounds 500,8469-8474(2011)
[45]Donald R.Askeland,Wendelin J.Wright,蘇春熺，劉偉隆，曾春風，王玉瑞，于劍平，材料科學與工程第7版第20章材料的熱性質,(2016)
[46]Anqing Wei ,Zhifu Liu,Faqiang Zhang,Mingsheng Ma,Guanyu Chen,Yongxiang Li, Thermal expansion coefficient tailoring of LAS glass-ceramic for anodic
bondable low temperature co-fired ceramic application,Ceramics International 46,4771-4777,(2020)
[47]Czestaw Sulkowski,Andrzej Chuchmala,Andrzej J.Zaleski,Marcin Matusiak,Jan Mucha,Pawel Gluchowski,Wieslaw Strek, Transport properties specific heat and thermal conductivity of GaN nanocrystalline ceramic,Journal of Solid State Chemistry 183,2501-2505,(2010)
[48]Jung-HyeEom,Young-WookKim, SantoshRaju, Processing and properties of macroporous silicon carbide ceramics: A review, Journal of Asian Ceramic Societies, Volume 1, Issue 3,Pages220-242,(2013)