稀土及鹼土氧化物添加劑對燒結氮化鋁陶瓷性質研究

朱智鴻

doi:10.6844/NCKU.2010.00431

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稀土及鹼土氧化物添加劑對燒結氮化鋁陶瓷性質研究

Effects of rare-earth and alkaline earth oxides additives on the sintering properties of aluminum nitride ceramics

朱智鴻 , Ph.D　　Advisor：申永輝　　Co-advisor ：溫紹炳;林志朋

英文 DOI： 10.6844/NCKU.2010.00431

氮化鋁；稀土氧化物；氧化鋁坩堝；二矽化鉬加熱元件；熱傳導值；介電；維氏硬度；破裂韌性； Aluminum nitride ； Rare-earth oxides ； Al2O3 crucible ； MoSi2 heating element ； Thermal conductivity ； Dielectric ； Fracture toughness

Abstract │ Reference (107) │ Altmetrics

Abstract 〈TOP〉

本研究起始氮化鋁粉末分別添加不同稀土氧化物(Y、Sm、Gd和Yb)與氧化鈣共添加作為粉末燒結助劑，並採氧化鋁坩堝置入一般箱型二矽化鉬高溫爐中通入普通純度氮氣進行溫度1570oC~1700oC的氮化鋁燒結試驗。這個製程的優勢在於不需要有高精密控制氣氛的燒結爐，如石墨爐、微波燒結爐和電漿爐等，因而燒結爐設備不僅裝置簡單且體積也相對較小，最重要的是製程及設備的成本可大幅地降低，更增添後續業界量產氮化鋁基板的可行性。由密度量測結果顯示三種不同原子量的稀土元素在燒結期間的原子擴散動力學差異會影響氮化鋁的燒結緻密化，其中燒結條件在1700oC持溫3小時的緻密燒結體可獲得熱傳導值介於106-147 Wm-1K-1之間，當中試片添加1 wt.%氧化釔和1 wt.%氧化鈣的試片可得相對密度達99%以上且最高熱傳導值147 Wm-1K-1。
再者，由氮化鋁分別添加氧化釔-氧化鈣和氧化鐿-氧化鈣兩組試片分別進行有無通入氮氣氛進行燒結溫度1615oC持溫4小時的試驗，其結果顯示通入氮氣氛進行燒結的試片密度相較無通入氮氣氛的試片密度高，明顯由80%提升至87%。此外，由燒結體殘碳量分析結果顯示，試片中的殘碳量皆低於0.4%，甚至與原樣中的碳雜質含量0.11%相當，說明本製程中的隔絕劑-碳黑在製備氮化鋁的熱處理期間無明顯擴散至晶粒中的現象產生。除此之外，實驗中採田口實驗計劃法進行氮化鋁燒結試驗，其相對密度結果經訊號雜訊比(SN ratio)及變異數分析(ANOVA)顯示眾多製程控制因子中，以燒結溫度和持溫時間對氮化鋁的緻密度提升影響較大，其貢獻度分別達50.4%和29.3%。另外，試片添加0.215和0.43 mole%的氧化釔試片相對密度隨著氧化鈣含量增加而增加，然而添加0.86 mole%的氧化釔試片則在氧化鈣添加量為1.29 mole%時，緻密度達最高96%以上。XRD結果顯示二次相由單一Al5Y3O12相轉變至Al5Y3O12, CaYAl3O7 and CaAl4O7等複合相，主要是受到不同添加劑含量影響，而且試片熱傳導值可達130 Wm-1K-1以上，最主要原因應是受到單一二次相，AlN晶格的純化以及晶界相的獨立分佈有關。
此外，經無壓液相燒結氮化鋁的試驗中，氮氧分析結果與c軸晶格常數的計算結果顯示，氮氧比(N/O ratio)與c軸晶格常數呈現較大值時，表示燒結體中的氧原子取代氮原子位置的機率較小，則產生不利於熱傳導的鋁空缺相對較少。除此之外，由SEM及BSI顯微結構觀察分布於氮化鋁晶界處的二次相種類及型態對試片的熱傳導值有一定程度的影響，當二次相種類多及二次相的分布呈現圍繞氮化鋁晶粒時，其晶格振盪所產生的聲子傳遞熱能的阻礙便增加；反之，若試片中僅存在單一晶界相或存在氮化鋁晶粒間的二次相呈現孤立分布時，則聲子傳遞的阻礙少，試片的熱傳導值便會有所提高。在熱性質方面，試片經1650oC和1700oC持溫3小時的條件下，可獲得其熱傳導值介於65-110 Wm-1K-1之間；在電性方面，試片在測試條件1 MHz下，介電常數量測介於8.96到10.6之間而介電損失則為0.02 to14.6 x10-3；在機械性質方面，其試片最高維氏硬度值可達1124 kgmm-2而破裂韌性值3.5 MPa•m1/2。最後，由以上最高密度結果顯示，產生緻密氮化鋁的臨界燒結溫度大約為1650oC。

Parallel Abstract 〈TOP〉

Aluminum nitride (AlN) ceramics, prepared with additives of CaO plus three different rare-earth oxides (Y, Sm, and Gd, separately), have been densified in an Al2O3 crucible at temperatures of up to 1650°C and 1700°C using a conventional MoSi2 heating element furnace. The advantage of using the particular experimental system and sintering condition is considered to be amenable to lower production cost and enhance the feasibility of mass production. The results of density measurements show that the atomic weight of the rare-earth element may substantially affect the apparent density of the sintered AlN specimen due to the kinetics of atomic diffusion during sintering. Dense AlN ceramics with higher thermal conductivity of 106-147 Wm-1K-1 were successfully obtained by using sintering additives of CaO plus separate rare-earth oxides of Gd, Sm, and Y at 1700°C with 3 h soaking time. The results of this study show that relative densities in excess of 99% of theoretical and a relatively highest thermal conductivity of 147 W/m-1K-1 have been achieved for feedstock materials prepared with combined addition of 1 wt.% Y2O3 and 1 wt.% CaO.
Moreover, it is noted that fabrication of AlN samples having separately additives in the coupling of (1) Y2O3-CaO and (2) Yb2O3-CaO with the flow of nitrogen atmosphere is significantly related to the densification of AlN, namely the enhancement of densities from 80% to 87%. Results of residual carbon content analysis show that the protective agent as carbon black does not diffuse into sintered bodies in this processing method, seemingly, it seems to be ignored that the trace amount of residual carbon is thus shown to be harmful to properties for AlN ceramics. In addition, it is noted from Taguchi method that the control factors as sintering temperature and soaking time, are main notable factors for the densification of sintered AlN, and the contribution ratios are 50.4% and 29.3%, respectively. Noted that the relative densities of samples having 0.215 and 0.43 mole% Y2O3 increase with increasing CaO addition; whereas, the relative densities of samples with 0.86 mole% Y2O3 steeply increase first and then, starting at 1.29 mole%, to decrease with increasing CaO addition. Results of XRD profiles show that the formation of secondary phases was given to transform form single Al5Y3O12 phase to the presence of Al5Y3O12, CaYAl3O7 and CaAl4O7 multiple phases due to the mixture of various amount of Y2O3 and CaO addition. Moreover, results shown that the relative density in excess of 96% of theoretical was obtained for AlN sample fired at 1600oC for 8 h, indicating that the employment of micro hot-pressed sintering has been shown to be helpful for augmenting the densification of AlN ceramics. The thermal conductivities up to 130 Wm-1K-1 has greatly related to the merely Al5Y3O12 as secondary phases, the purification of the AlN lattice, and the grain boundary phases isolated distribution.
The thermal conductivities of 65-110 Wm-1K-1 were obtained for test samples sintered at 1650 and 1700oC for 3 h, giving that the influence of the secondary phase distribution enriched at the grain boundaries for each sintered AlN. For the compacts sintered at 1650oC and 1700oC for 3 h, the dielectric constant and loss factors range form 8.98 to 10.6 and 0.02 to14.6 x10-3 at 1 MHz, respectively. Additionally, higher Vicker's hardness of 1124 kgmm-2 and fracture toughness of approaching 3.5 MPa•m1/2 were obtained for the series of test runs. Critical temperature for AlN densification to obtain the highest density is around1650°C.

Reference ( 107 ) 〈TOP〉

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連結：

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