低温共烧玻璃陶瓷材料的制备及性能、机理研究
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摘要
根据最近国内外低温共烧陶瓷材料的研究进展及存在的主要问题，采用差热分析仪、X-射线衍射仪、扫描电子显微镜、能谱分析仪、阻抗分析仪、热学性能和力学性能测试仪等系统研究了添加剂及氧化物取代对堇青石基玻璃的结构、烧结性能、相组成、介电性能、热膨胀性能和力学性能等的影响规律；新型系列玻璃／陶瓷复合材料中陶瓷引入量和烧结(热压)工艺与烧结、相组成、介电性能、热学特性、显微组织与力学性能的影响规律；提出了微晶玻璃的烧结、晶化机理、相变机理和烧结过程中石英和方石英的析出机理以及AlN／堇青石玻璃陶瓷复合材料的补强增韧机制。主要结果如下：
系统地探讨了氧化铋和烧结工艺与堇青石基微晶玻璃的相转变、烧结特性、物理性能和界面特性的关系：氧化铋的加入降低了堇青石的μ相向α相转变的温度，有效促进了烧结致密化。介电常数和抗折强度均随氧化铋的增加而增加，且与密度变化曲线相似；介电损耗随氧化铋的增加呈“V”字变化。热膨胀系数随氧化铋的变化基本呈线性增加。氧化铋的合理添加量为3～5wt％。900～950℃烧结致密样品的介电常数约为5.3，介电损耗为10~(-3)，抗折强度大于130MPa，热膨胀系数约为3.5×10~(-6)K~(-1)，极化普适关系指数n为0.5～0.9，具有良好的温度和频率稳定性。材料与银电极的界面结合良好，银元素的扩散深度约5μm，材料具有高的可靠性。
首次提出了氧化铈在玻璃中的作用机制。添加少量氧化铈起到网络修饰体的作用，有利于降低玻璃的粘度，促进堇青石的μ相向α相的转变和烧结致密化。添加过多氧化铈不利于烧结。样品的介电性能取决于氧化铈含量和烧结温度、晶体相的组成及致密程度。热膨胀系数随氧化铈的增加呈“倒Z字”变化。热膨胀系数随温度的增加基本上呈线性减小的趋势，这与析出堇青石晶体的数量有关。抗折强度随氧化铈的增加呈先增后减的趋势，且与气孔率的变化曲线相似。添加氧化铈为4wt％的样品能够低温烧结(≤950℃)。样品具有良好的温度和频率稳定性，其介电常数为5.3，介电损耗为2×10~(-3)，热膨胀系数为2.5～2.8×10~(-6)K~(-1)，抗折强度为115MPa，能够满足低温共烧陶瓷的要求。
首次系统地研究了添加氧化锌和氧化锌取代氧化铝对微晶玻璃结构、烧结、相转变、显微组织和物理性能的影响规律。添加1.5～3wt％氧化锌有利于降低玻璃的粘度，促进玻璃粉体的烧结。添加过多的氧化锌将使玻璃容易析晶而不利于烧结。随氧化锌的增加，有利于锌铝尖晶石和石英晶体相的析出。添加3wt％氧化锌样品的晶体析出顺序与红外光谱强吸收峰的位置变化相吻合。随氧化锌的增加，介电常数大体上呈增加趋势，介电损耗在氧化锌为1～3wt％时有最小值。膨胀系数随氧化锌的增加呈线性增加。随氧化锌的增加，抗折强度先升后降，在氧化锌为1.5wt％达到最大值。添加1.5～3.0wt％氧化锌样品低温(≤950℃)烧结后具有低的介电常数(5.0～5.3)，低的介电损耗(2×10~(-3))，低的热膨胀系数(3.0～4.8×10~(-6)K~(-1))，较高的抗折强度(≥120MPa)。样品的温度和频率稳定性良好。
随氧化锌替代量的增加，玻璃的熔化温度和晶化温度明显降低，玻璃转变温度呈先降后升的趋势。当氧化锌为5wt％和8wt％时，主晶相为α—堇青石；11wt％时，主晶相变为锌铝尖晶石和石英。氧化锌的合理取代量为8wt％。900～925℃烧结的样品具有97％的相对密度，低的介电常数(5.0～5.2)，低的介电损耗(＜10~(-3))，低的热膨胀系数(4.0-4.2×10~(-6)K~(-1))和高的抗折强度(≥125MPa)，是一种优质的低温共烧陶瓷材料。
提出了添加氧化铈微晶玻璃的烧结机制和晶化机理：玻璃粉体的烧结机制属于粘性流动占主导地位的液相烧结过程。推导出气孔率随时间的变化和烧结动力学常数K与烧结温度的关系分别为：—ln p=kt+B和ln k=C-E／R T。据此可算出添加0wt％，2wt％、4wt％和7wt％氧化铈样品的烧结活化能分别为221kJ／mol，203.1kJ／mol、196.0kJ／mol和232.0kJ／mol。该烧结数学模型适用于烧结初、中期。随氧化铈的增加，玻璃的析晶活化能逐渐增加，添加氧化铈不利于玻璃的析晶。所有玻璃样品均为表面晶化机理。
基于晶体结构和玻璃“分相”的理论，首次提出了硼玻璃／钙(锶)长石复合材料烧结过程中石英和方石英的析出机理。长石独特的晶体结构使得M~(2+)(M=Ca，Sr)填充在四面体组成的通道空隙中来平衡电价保持电中性。在适当的条件下，组成中的M~(2+)(M=Ca，Sr)和玻璃中的组分容易发生相互扩散，使得陶瓷颗粒周围的玻璃组成发生了改变。由玻璃“分相”理论可知，Ca~(2+)、Sr~(2+)和Zn~(2+)的共同作用导致了玻璃的分相。α-石英从富SiO_2中析出。温度增加加剧了“分相”，方石英越容易从富硅玻璃相中直接析出，同时石英也能转变为方石英。这与添加氧化铝抑制方石英的机理有所不同。
系统研究了玻璃／陶瓷复合材料的组成和物理性能的关系。介电常数、热膨胀系数和显微硬度随陶瓷含量的增加而增加，而介电损耗随之减小。烧结中α-石英和方石英的析出增加了材料的热膨胀系数，但对材料的介电性能影响不大。硼酸铝的生成对玻璃／尖晶石复合材料的介电和热膨胀性能有益。添加10wt％硼酸铝能完全抑制高硅玻璃／硼酸铝复合材料中石英和方石英的析出。750～1000℃制备的复合材料具有优良的综合性能，能够用于微电子封装领域。
首次提出了AlN／堇青石玻璃复合材料的强化机制主要是载荷传递，增韧机制主要是裂纹的绕道偏转、分叉和钉扎与增强颗粒相的拔出。
系统研究了AlN及热压工艺和复合材料烧结特性、介电性能、热学性能和力学性能的内在关系。随AlN的增加，致密度略有下降，介电常数和介电损耗逐渐增加。随热压温度提高，相对密度明显增加，介电常数和介电损耗都降低。增加保温时间可提高致密度。热膨胀系数和热导率随AlN的增加而增加。AlN引入量不同的样品表现出不同的导热特性。抗折强度和断裂韧性随AlN的增加逐渐增加。当AlN引入量为40％时，抗折强度和断裂韧性都达到最大值，分别从基体的117MPa和1.27MPa.m~(1／2)提高到212MPa和3.04MPa.m~(1／2)。AlN与堇青石玻璃不发生化学反应，化学相容性好。
采用真空热压法低温(≤1000℃)制备的样品具有低介电常数(5.6～6.6)、低介电损耗(＜0.18％)、与Si匹配的热膨胀系数、较高的热导率(6.5Wm~(-1)K~(-1))、高的力学性能、良好的温度和频率稳定性，能够满足高密度电子封装的要求。
According to the latest development and shortcoming of lowtemperature co-fired ceramic: substrate materials (LTCCs), the effects ofthe additives and oxide replacement on glass structure, sintering, phasecompositions, dielectric properties, thermal expansion characterizationand mechanical properties of cordierite-based glass-ceramics wereinvestigated by using the differential thermal analysis (DTA), X-raydiffraction (XRD), scanning electron microscope (SEM), energyspectrum analysis, a Hewlett-Packard (HP) AC impedance, a thermalproperty test apparatus and a mechanical property test apparatus. Theinfluences of the ceramic content and sintering or hot-pressingtemperature on firing, phase composition, thermal expansioncharacterization, dielectric property, heat exchange behavior, microstructure and mechanical properties of new glass/ ceramicsystems were studied. The mechanisms of sintering densificationkinetics, crystallization kinetics and phase transition of glass-ceramicsand those of the precipitation of cristobalite and quartz in sinteringprocess for the borosilicate/feldspar composites as well as ofstrengthening and toughening in the AlN/cordierite glass compositeswere put forward respectively in this paper and the results showed as thefollowing:
The relationships betwe, en the content of bismuth oxide, sinteringtechnologic parameters and the phase transition, sinteringcharacterization, physical properties and interfacial characteristics ofcordierite-based glass-ceramics were investigated. The addition ofbismuth oxide can lower the phase transformation temperature fromμ-toα- cordierite and enhance the sintering densification. The dielectricconstant and the flexural strength of samples increase with the additionof bismuth oxide in a similar way as that of the density. The dielectricloss manifests "V" curve with bismuth oxide. The thermal expansion coefficients with increasing bismuth oxide exhibit the characteristic oflinear increase. The reasonable addition of bismuth oxide is 3～5wt%.The material fired at 900～950℃in air has a low dielectric constant(～5.3), low dielectric loss (～0.001), low thermal expansion coefficient(～3.5×10~(-6)K~(-1))and high flexural strength (≥130MPa). The polarizationuniversal relation index is in the range of 0.5～0.9. The dielectricproperties of the sample with temperature dependence and frequencydependence possess the excellent stability. The interfacial coalescentbetween the glass-ceramic substrate and Ag electrode is good and thethickness of Ag diffusion layer is about 5μm. The glass-ceramicsubstrate can meet the demand for a long-term reliability in LTCCs.
The role of ceria in the cordierite-based glasses was put forward forthe first time. The results show that a small amount of ceria added act asthe network modifier, lower the viscosity of the glass, accelerate phasetransformation of cordierite fromμtoαand enhance sinteringdensification of cordierite-based glass powders. Over ceria added willinhibit the sintering densification. The dielectric properties ofglass-ceramics depend on not only the content of ceria and sinteringtemperature but also the crystalline phases and relative density. Thethermal expansion coefficient of glass-ceramics present the reciprocal "Z" curve with ceria content and it basically decrease according to thelinearity with increasing temperature, which depend upon the amount ofcordierite. The flexural strength of samples firstly increases and thendecreases with the content of ceria, which is similar to the curve of theporosity. The glass-ceramics with 4wt% ceria sintered at 900～950℃has a low dielectric constant(5.3), low dissipation factor (≤0.002), lowthermal expansion coefficient (2.5～2.8×10~(-6)K~(-1)) and high flexuralstrength (115MPa), suggesting that it would be a promising material inLTCCs.
The effects of ZnO added and the replacement of Al_2O_3 by ZnO onglass structure, crystallization behavior, phase transition, microstructure, sintering dynamics and physical properties were discussed for the firsttime. With increasing ZnO content, the melting temperature, glasstransition temperature and crystallization temperature all decreased.Addition of ZnO can greatly improve the sinterability of samples andalter the type of the crystalline phase. Too much ZnO addition (morethan 3wt%) seems to be needless for deteriorating the physicalproperties of the sample. The reasonable ZnO content is 3wt%. Thecrystallization sequence of crystalline phases in the sample with 3%ZnO corresponds to the position of IR absorption spectra. The dielectricconstants increase with ZnO content and the dielectric loss has thelowest value at 1.5wt%～3wt% ZnO. The thermal expansioncoefficients increase with ZnO content. The flexural strength firstlyincreases and then decreases with ZnO and get to the highest value at1.5wt% ZnO. The glass-ceramics with 1.5～3wt% ZnO sintered at900～950℃has a low dielectric constant(5.0～5.3), low dielectric loss(≤0.002), low thermal expansion coefficient (3.0～4.8×10~(-6)K~(-1)) andhigh flexural strength (≥120MPa). The dielectric properties of thesample with temperature dependence and frequency dependence possessthe excellent stability.
With increasing replacement amount of Al_2O_3 by ZnO, the meltingtemperature and crystallization temperature of the glass-ceramics lower, and the glass transition temperature firstly decrease and then increase.With the replacement of 5wt% and 8wt%, the predominant crystallinephases in the glass-ceramics were found to beα-cordierite and thesecondary crystalline phase to be gahnite and quartz. When thereplacement was increased to 11wt%, the predominant crystalline phaseswere found to be gahnite and quartz and the secondary phase to beα-cordierite. Only the sample with 8wt% ZnO can be fully sinteredbefore 1000℃. Therefore, the sample fired at 900～925℃has 97.0%theoretical density, a fairly low dielectric constant (5.0～5.2), a lowdielectric loss (≤0.001) at 1MHz, a lower thermal expansion coefficient(4.0～4.2×10~(-6)K~(-1)) and a higher flexural strength (≥125MPa), suggesting that it would be a promising material in the electronicpackaging field.
The sintering and crystallization mechanisms of the glass-ceramicscontaining ceria were put forward. The sintering mechanism is the liquidsintering process in which Newtonian viscosity flow predominates. Theporosity is determined by time and is given by—lnp=kt+B. Themethod of the sintering kinetic parameter used gives an equation of theform In k=C-E/RT. According to two equations, the sinteringactivation energy calculated of samples with 0wt%, 2wt%, 4wt%and7wt%ceria is 221 kJ/mol, 203.1kJ/mol, 196.0 kJ/mol and 232.0 kJ/molrespectively. However, the mathematic models mentioned above are thesame with the initial and medium-term phases. The results obtained byusing differential thermal analysis and JMA equation illuminate that thecrystallization activation energy of glass-ceramics increases with ceriacontent and adding ceria will inhibit the crystallization of glasses. Thecrystallization mechanism of all the glass is believed to crystallize fromthe surface.
Based on the crystal structure and phase separation of glass, thedevitrification mechanisms of cristobalite and quartz in the borosilicateglass/feldspar (anorthite or Sr-celsian) composites in the sinteringprocess were put forward for the first time, which is different from thatof alumina. The unique crystal structure of feldspar makes M~(2+) ion(M=Ca, Sr) exist in the large channels. According to the above analysis, the Al~(3+)ion from feldspar is very difficult to diffuse into glass. Incontrast, the M~(2+) ion from feldspar and other ions (Ca~(2+), Zn~(2+))from theglass phase can easily reciprocally diffuse into that increasing thetendency of phase separation in borosilicate glass, which leads to theformation of rich SiO_2 glass phase and rich-R~(2+)(R=Ca, Sr, Zn) glassphase. The precipitation ofα-quartz crystal occurs in the compositesduring the firing and some amount ofα-quartz may synchronously transformed into cristobalite. Certainly, elevating temperature andincreasing ceramic content can accelerate the formation ofα-quartz andcristobalite directly from the composite, which leads to having badeffect on the thermal expansion coefficient of the composites.
The relationships between the composition and physical propertywere investigated. The results show that the dielectric constant andthermal expansion coefficient as well as hardness increases butdielectric loss of samples decreases with ceramic content. The formationofα-quartz and cristobalite leads to having bad effect on the thermalexpansion coefficient but has little effect on the values of the dielectricconstant of the composites. The formation of aluminum borate ispropitious to the dielectric property and thermal expansion property inthe glass/spinel composites. Adding 10wt% aluminum borate (Al_(18)B_4O_(33))drastically inhibits the precipitation of quartz and cristobalite in the highSiO_2 glass/aluminum borate composites. The material sintered at lowtemperature between 750℃and 1000℃has good physical propertiesand would be applied to the electronic packaging field.
The strengthening and toughening mechanisms of AlN/cordieriteglass composites were put forward. The strengthening mechanism isload transfer and the toughening mechanisms are deflexion, divaricationand transfixion as well as AlN particle pulling out.
The relationships between AlN content, hot-pressing technology, sintering characterization and thermo-physical properties of theAlN/cordierite glass composites were systemically investigated. Therelative density of the composites slightly decreases with AlN contentand obviously increases with increasing hot-pressing temperature andholding time. The thermal expansion coefficient and the thermalconductivity increases with increasing AlN. The variety of the thermalconductivity for the samples containing different AlN content hasdifferent characteristic. The dielectric constant and dielectric lossincrease with AlN content and reduce with hot-pressing temperature.
The flexural strength and fracture toughness gradually improve withincreasing AlN. The flexural strength and fracture toughness reach amaximum, i.e. from 117MPa and 1.27MPa.m~(1/2) of the glass matrix to212MPa and 3.04MPa.m~(1/2) of the composites at 40vol% AlN. XRDanalysis indicates that no chemical reaction occurs between cordieriteglass matrix and AlN particles suggesting that the glass matrix haveexcellent chemical compatibility with AlN particles.
The composites sintered in vacuum by hot-pressing at lowtemperature (≤1000℃) have a fairly low dielectric constant (5.6～6.6), a low dielectric loss (0.001), a low thermal expansioncoefficient(≤3.8×10~(-6)K~(-1)), a high thermal conductivity (6.5Wm~(-1)K~(-1)), ahigh mechanical properties and is suitable for high density electronicpackaging.
系统地探讨了氧化铋和烧结工艺与堇青石基微晶玻璃的相转变、烧结特性、物理性能和界面特性的关系：氧化铋的加入降低了堇青石的μ相向α相转变的温度，有效促进了烧结致密化。介电常数和抗折强度均随氧化铋的增加而增加，且与密度变化曲线相似；介电损耗随氧化铋的增加呈“V”字变化。热膨胀系数随氧化铋的变化基本呈线性增加。氧化铋的合理添加量为3～5wt％。900～950℃烧结致密样品的介电常数约为5.3，介电损耗为10~(-3)，抗折强度大于130MPa，热膨胀系数约为3.5×10~(-6)K~(-1)，极化普适关系指数n为0.5～0.9，具有良好的温度和频率稳定性。材料与银电极的界面结合良好，银元素的扩散深度约5μm，材料具有高的可靠性。
首次提出了氧化铈在玻璃中的作用机制。添加少量氧化铈起到网络修饰体的作用，有利于降低玻璃的粘度，促进堇青石的μ相向α相的转变和烧结致密化。添加过多氧化铈不利于烧结。样品的介电性能取决于氧化铈含量和烧结温度、晶体相的组成及致密程度。热膨胀系数随氧化铈的增加呈“倒Z字”变化。热膨胀系数随温度的增加基本上呈线性减小的趋势，这与析出堇青石晶体的数量有关。抗折强度随氧化铈的增加呈先增后减的趋势，且与气孔率的变化曲线相似。添加氧化铈为4wt％的样品能够低温烧结(≤950℃)。样品具有良好的温度和频率稳定性，其介电常数为5.3，介电损耗为2×10~(-3)，热膨胀系数为2.5～2.8×10~(-6)K~(-1)，抗折强度为115MPa，能够满足低温共烧陶瓷的要求。
首次系统地研究了添加氧化锌和氧化锌取代氧化铝对微晶玻璃结构、烧结、相转变、显微组织和物理性能的影响规律。添加1.5～3wt％氧化锌有利于降低玻璃的粘度，促进玻璃粉体的烧结。添加过多的氧化锌将使玻璃容易析晶而不利于烧结。随氧化锌的增加，有利于锌铝尖晶石和石英晶体相的析出。添加3wt％氧化锌样品的晶体析出顺序与红外光谱强吸收峰的位置变化相吻合。随氧化锌的增加，介电常数大体上呈增加趋势，介电损耗在氧化锌为1～3wt％时有最小值。膨胀系数随氧化锌的增加呈线性增加。随氧化锌的增加，抗折强度先升后降，在氧化锌为1.5wt％达到最大值。添加1.5～3.0wt％氧化锌样品低温(≤950℃)烧结后具有低的介电常数(5.0～5.3)，低的介电损耗(2×10~(-3))，低的热膨胀系数(3.0～4.8×10~(-6)K~(-1))，较高的抗折强度(≥120MPa)。样品的温度和频率稳定性良好。
随氧化锌替代量的增加，玻璃的熔化温度和晶化温度明显降低，玻璃转变温度呈先降后升的趋势。当氧化锌为5wt％和8wt％时，主晶相为α—堇青石；11wt％时，主晶相变为锌铝尖晶石和石英。氧化锌的合理取代量为8wt％。900～925℃烧结的样品具有97％的相对密度，低的介电常数(5.0～5.2)，低的介电损耗(＜10~(-3))，低的热膨胀系数(4.0-4.2×10~(-6)K~(-1))和高的抗折强度(≥125MPa)，是一种优质的低温共烧陶瓷材料。
提出了添加氧化铈微晶玻璃的烧结机制和晶化机理：玻璃粉体的烧结机制属于粘性流动占主导地位的液相烧结过程。推导出气孔率随时间的变化和烧结动力学常数K与烧结温度的关系分别为：—ln p=kt+B和ln k=C-E／R T。据此可算出添加0wt％，2wt％、4wt％和7wt％氧化铈样品的烧结活化能分别为221kJ／mol，203.1kJ／mol、196.0kJ／mol和232.0kJ／mol。该烧结数学模型适用于烧结初、中期。随氧化铈的增加，玻璃的析晶活化能逐渐增加，添加氧化铈不利于玻璃的析晶。所有玻璃样品均为表面晶化机理。
基于晶体结构和玻璃“分相”的理论，首次提出了硼玻璃／钙(锶)长石复合材料烧结过程中石英和方石英的析出机理。长石独特的晶体结构使得M~(2+)(M=Ca，Sr)填充在四面体组成的通道空隙中来平衡电价保持电中性。在适当的条件下，组成中的M~(2+)(M=Ca，Sr)和玻璃中的组分容易发生相互扩散，使得陶瓷颗粒周围的玻璃组成发生了改变。由玻璃“分相”理论可知，Ca~(2+)、Sr~(2+)和Zn~(2+)的共同作用导致了玻璃的分相。α-石英从富SiO_2中析出。温度增加加剧了“分相”，方石英越容易从富硅玻璃相中直接析出，同时石英也能转变为方石英。这与添加氧化铝抑制方石英的机理有所不同。
系统研究了玻璃／陶瓷复合材料的组成和物理性能的关系。介电常数、热膨胀系数和显微硬度随陶瓷含量的增加而增加，而介电损耗随之减小。烧结中α-石英和方石英的析出增加了材料的热膨胀系数，但对材料的介电性能影响不大。硼酸铝的生成对玻璃／尖晶石复合材料的介电和热膨胀性能有益。添加10wt％硼酸铝能完全抑制高硅玻璃／硼酸铝复合材料中石英和方石英的析出。750～1000℃制备的复合材料具有优良的综合性能，能够用于微电子封装领域。
首次提出了AlN／堇青石玻璃复合材料的强化机制主要是载荷传递，增韧机制主要是裂纹的绕道偏转、分叉和钉扎与增强颗粒相的拔出。
系统研究了AlN及热压工艺和复合材料烧结特性、介电性能、热学性能和力学性能的内在关系。随AlN的增加，致密度略有下降，介电常数和介电损耗逐渐增加。随热压温度提高，相对密度明显增加，介电常数和介电损耗都降低。增加保温时间可提高致密度。热膨胀系数和热导率随AlN的增加而增加。AlN引入量不同的样品表现出不同的导热特性。抗折强度和断裂韧性随AlN的增加逐渐增加。当AlN引入量为40％时，抗折强度和断裂韧性都达到最大值，分别从基体的117MPa和1.27MPa.m~(1／2)提高到212MPa和3.04MPa.m~(1／2)。AlN与堇青石玻璃不发生化学反应，化学相容性好。
采用真空热压法低温(≤1000℃)制备的样品具有低介电常数(5.6～6.6)、低介电损耗(＜0.18％)、与Si匹配的热膨胀系数、较高的热导率(6.5Wm~(-1)K~(-1))、高的力学性能、良好的温度和频率稳定性，能够满足高密度电子封装的要求。
According to the latest development and shortcoming of lowtemperature co-fired ceramic: substrate materials (LTCCs), the effects ofthe additives and oxide replacement on glass structure, sintering, phasecompositions, dielectric properties, thermal expansion characterizationand mechanical properties of cordierite-based glass-ceramics wereinvestigated by using the differential thermal analysis (DTA), X-raydiffraction (XRD), scanning electron microscope (SEM), energyspectrum analysis, a Hewlett-Packard (HP) AC impedance, a thermalproperty test apparatus and a mechanical property test apparatus. Theinfluences of the ceramic content and sintering or hot-pressingtemperature on firing, phase composition, thermal expansioncharacterization, dielectric property, heat exchange behavior, microstructure and mechanical properties of new glass/ ceramicsystems were studied. The mechanisms of sintering densificationkinetics, crystallization kinetics and phase transition of glass-ceramicsand those of the precipitation of cristobalite and quartz in sinteringprocess for the borosilicate/feldspar composites as well as ofstrengthening and toughening in the AlN/cordierite glass compositeswere put forward respectively in this paper and the results showed as thefollowing:
The relationships betwe, en the content of bismuth oxide, sinteringtechnologic parameters and the phase transition, sinteringcharacterization, physical properties and interfacial characteristics ofcordierite-based glass-ceramics were investigated. The addition ofbismuth oxide can lower the phase transformation temperature fromμ-toα- cordierite and enhance the sintering densification. The dielectricconstant and the flexural strength of samples increase with the additionof bismuth oxide in a similar way as that of the density. The dielectricloss manifests "V" curve with bismuth oxide. The thermal expansion coefficients with increasing bismuth oxide exhibit the characteristic oflinear increase. The reasonable addition of bismuth oxide is 3～5wt%.The material fired at 900～950℃in air has a low dielectric constant(～5.3), low dielectric loss (～0.001), low thermal expansion coefficient(～3.5×10~(-6)K~(-1))and high flexural strength (≥130MPa). The polarizationuniversal relation index is in the range of 0.5～0.9. The dielectricproperties of the sample with temperature dependence and frequencydependence possess the excellent stability. The interfacial coalescentbetween the glass-ceramic substrate and Ag electrode is good and thethickness of Ag diffusion layer is about 5μm. The glass-ceramicsubstrate can meet the demand for a long-term reliability in LTCCs.
The role of ceria in the cordierite-based glasses was put forward forthe first time. The results show that a small amount of ceria added act asthe network modifier, lower the viscosity of the glass, accelerate phasetransformation of cordierite fromμtoαand enhance sinteringdensification of cordierite-based glass powders. Over ceria added willinhibit the sintering densification. The dielectric properties ofglass-ceramics depend on not only the content of ceria and sinteringtemperature but also the crystalline phases and relative density. Thethermal expansion coefficient of glass-ceramics present the reciprocal "Z" curve with ceria content and it basically decrease according to thelinearity with increasing temperature, which depend upon the amount ofcordierite. The flexural strength of samples firstly increases and thendecreases with the content of ceria, which is similar to the curve of theporosity. The glass-ceramics with 4wt% ceria sintered at 900～950℃has a low dielectric constant(5.3), low dissipation factor (≤0.002), lowthermal expansion coefficient (2.5～2.8×10~(-6)K~(-1)) and high flexuralstrength (115MPa), suggesting that it would be a promising material inLTCCs.
The effects of ZnO added and the replacement of Al_2O_3 by ZnO onglass structure, crystallization behavior, phase transition, microstructure, sintering dynamics and physical properties were discussed for the firsttime. With increasing ZnO content, the melting temperature, glasstransition temperature and crystallization temperature all decreased.Addition of ZnO can greatly improve the sinterability of samples andalter the type of the crystalline phase. Too much ZnO addition (morethan 3wt%) seems to be needless for deteriorating the physicalproperties of the sample. The reasonable ZnO content is 3wt%. Thecrystallization sequence of crystalline phases in the sample with 3%ZnO corresponds to the position of IR absorption spectra. The dielectricconstants increase with ZnO content and the dielectric loss has thelowest value at 1.5wt%～3wt% ZnO. The thermal expansioncoefficients increase with ZnO content. The flexural strength firstlyincreases and then decreases with ZnO and get to the highest value at1.5wt% ZnO. The glass-ceramics with 1.5～3wt% ZnO sintered at900～950℃has a low dielectric constant(5.0～5.3), low dielectric loss(≤0.002), low thermal expansion coefficient (3.0～4.8×10~(-6)K~(-1)) andhigh flexural strength (≥120MPa). The dielectric properties of thesample with temperature dependence and frequency dependence possessthe excellent stability.
With increasing replacement amount of Al_2O_3 by ZnO, the meltingtemperature and crystallization temperature of the glass-ceramics lower, and the glass transition temperature firstly decrease and then increase.With the replacement of 5wt% and 8wt%, the predominant crystallinephases in the glass-ceramics were found to beα-cordierite and thesecondary crystalline phase to be gahnite and quartz. When thereplacement was increased to 11wt%, the predominant crystalline phaseswere found to be gahnite and quartz and the secondary phase to beα-cordierite. Only the sample with 8wt% ZnO can be fully sinteredbefore 1000℃. Therefore, the sample fired at 900～925℃has 97.0%theoretical density, a fairly low dielectric constant (5.0～5.2), a lowdielectric loss (≤0.001) at 1MHz, a lower thermal expansion coefficient(4.0～4.2×10~(-6)K~(-1)) and a higher flexural strength (≥125MPa), suggesting that it would be a promising material in the electronicpackaging field.
The sintering and crystallization mechanisms of the glass-ceramicscontaining ceria were put forward. The sintering mechanism is the liquidsintering process in which Newtonian viscosity flow predominates. Theporosity is determined by time and is given by—lnp=kt+B. Themethod of the sintering kinetic parameter used gives an equation of theform In k=C-E/RT. According to two equations, the sinteringactivation energy calculated of samples with 0wt%, 2wt%, 4wt%and7wt%ceria is 221 kJ/mol, 203.1kJ/mol, 196.0 kJ/mol and 232.0 kJ/molrespectively. However, the mathematic models mentioned above are thesame with the initial and medium-term phases. The results obtained byusing differential thermal analysis and JMA equation illuminate that thecrystallization activation energy of glass-ceramics increases with ceriacontent and adding ceria will inhibit the crystallization of glasses. Thecrystallization mechanism of all the glass is believed to crystallize fromthe surface.
Based on the crystal structure and phase separation of glass, thedevitrification mechanisms of cristobalite and quartz in the borosilicateglass/feldspar (anorthite or Sr-celsian) composites in the sinteringprocess were put forward for the first time, which is different from thatof alumina. The unique crystal structure of feldspar makes M~(2+) ion(M=Ca, Sr) exist in the large channels. According to the above analysis, the Al~(3+)ion from feldspar is very difficult to diffuse into glass. Incontrast, the M~(2+) ion from feldspar and other ions (Ca~(2+), Zn~(2+))from theglass phase can easily reciprocally diffuse into that increasing thetendency of phase separation in borosilicate glass, which leads to theformation of rich SiO_2 glass phase and rich-R~(2+)(R=Ca, Sr, Zn) glassphase. The precipitation ofα-quartz crystal occurs in the compositesduring the firing and some amount ofα-quartz may synchronously transformed into cristobalite. Certainly, elevating temperature andincreasing ceramic content can accelerate the formation ofα-quartz andcristobalite directly from the composite, which leads to having badeffect on the thermal expansion coefficient of the composites.
The relationships between the composition and physical propertywere investigated. The results show that the dielectric constant andthermal expansion coefficient as well as hardness increases butdielectric loss of samples decreases with ceramic content. The formationofα-quartz and cristobalite leads to having bad effect on the thermalexpansion coefficient but has little effect on the values of the dielectricconstant of the composites. The formation of aluminum borate ispropitious to the dielectric property and thermal expansion property inthe glass/spinel composites. Adding 10wt% aluminum borate (Al_(18)B_4O_(33))drastically inhibits the precipitation of quartz and cristobalite in the highSiO_2 glass/aluminum borate composites. The material sintered at lowtemperature between 750℃and 1000℃has good physical propertiesand would be applied to the electronic packaging field.
The strengthening and toughening mechanisms of AlN/cordieriteglass composites were put forward. The strengthening mechanism isload transfer and the toughening mechanisms are deflexion, divaricationand transfixion as well as AlN particle pulling out.
The relationships between AlN content, hot-pressing technology, sintering characterization and thermo-physical properties of theAlN/cordierite glass composites were systemically investigated. Therelative density of the composites slightly decreases with AlN contentand obviously increases with increasing hot-pressing temperature andholding time. The thermal expansion coefficient and the thermalconductivity increases with increasing AlN. The variety of the thermalconductivity for the samples containing different AlN content hasdifferent characteristic. The dielectric constant and dielectric lossincrease with AlN content and reduce with hot-pressing temperature.
The flexural strength and fracture toughness gradually improve withincreasing AlN. The flexural strength and fracture toughness reach amaximum, i.e. from 117MPa and 1.27MPa.m~(1/2) of the glass matrix to212MPa and 3.04MPa.m~(1/2) of the composites at 40vol% AlN. XRDanalysis indicates that no chemical reaction occurs between cordieriteglass matrix and AlN particles suggesting that the glass matrix haveexcellent chemical compatibility with AlN particles.
The composites sintered in vacuum by hot-pressing at lowtemperature (≤1000℃) have a fairly low dielectric constant (5.6～6.6), a low dielectric loss (0.001), a low thermal expansioncoefficient(≤3.8×10~(-6)K~(-1)), a high thermal conductivity (6.5Wm~(-1)K~(-1)), ahigh mechanical properties and is suitable for high density electronicpackaging.
引文
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