本文主要探討氧化鋯材料相變韌化機制與離子導電性之應用，利用臨場同步輻射X光繞射-(循環)應力試驗、拉曼光譜與穿透式電子顯微鏡等手法分析存在於共摻雜適當含量氧化釔(Y2O3)、氧化鈮(Nb2O5)和氧化釔(Y2O3)、氧化鈰(CeO2)於氧化鋯(3Y)之兩種氧化鋯基材料之韌化機制。結果顯示，兩種共摻雜型氧化鋯基材料在適當量添加時皆具有相當優異的機械性質，屬於立方相與正方相混合之部分安定氧化鋯結構(PSZ)，其韌性值遠優於3 mol%釔安定正方相氧化鋯多晶體(3Y-TZP)1-3倍。在臨場同步輻射X光繞射-應力試驗中，共摻雜型氧化鋯試片之繞射圖譜並未發現繞射峰有出現正方晶轉單斜晶(t-to-m)相變化與其他類似正方晶轉菱方晶(t-to-r)與正方晶轉斜方晶(t-to-o)等相變化韌化機制，也尚未觀察到正方相鐵彈域轉換(Ferroelastic domain switching)的韌化機制。有趣的是，我們觀察到一個與立方相(c)和亞安定型正方相(t’)具有相依性的新相變韌化機制，且運用穿透式電子顯微鏡觀察彼此之間結晶學方位關聯性與定義晶格常數。同時搭配應力應變試驗觀察此新相變化對於氧化鋯材料於應力動態循環情況下所扮演的角色。此外，利用不同的熱處理機制觀察氧化鋯材料韌性值變化的情形。
本文之另一個重點即是對於上述共摻雜型氧化鋯基材料進行離子導電特性量測；結果顯示，添加於氧化鋯中之氧化物若其本身晶格束縛能過大，則會導致材料內部平均晶格束縛能提升，使氧離子於晶格中擴散不易，因而降低整體材料離子導電性。離子半徑也是影響離子導電性的因素之一，若添加離子半徑與母相之離子差異過大，則易使材料內部產生較大的晶格應變，使離子導電性降低。藉由對前述兩種共摻雜型氧化鋯基材料離子導電性研究所歸納出的離子導電性影響因子，依循(1)離子半徑接近母材鋯離子、(2)平均晶格束縛能越小越好、(3)最大的陽離子添加量，設計出共摻雜二價與三價陽離子於氧化鋯材料，結果顯示可有效的原始材料之離子導電性46%以上。
對於添加過多陽離子之氧化鋯成分進行拉曼光譜與穿透式電子顯微鏡觀察內部結構的變化，發現影響電性下降的來源是因為晶界出現了對稱性較低的結構，並非一般文獻所提及的氧空缺序化或是缺陷叢聚所致；亦利用同步輻射X光螢光吸收試驗：X光吸收光譜(XAS)、近邊緣X光微細結構(NEXAF)與傅立葉轉換(FT)分析共摻雜系統之近邊緣微細結構與電性之關聯性。
最後，將前章節所開發的電解質材料用以設計出新型電極材料並應用於固態氧化物燃料電池進行催化活性(塔弗曲線)、極化阻抗(交流阻抗分析)與發電效率測試，結果顯示在交流阻抗圖譜與塔弗曲線皆可觀察到本次所開發之新型電極比傳統Ni-YSZ具有較低的極化電阻並具有較高的交換電流(催化性)，且其於循環伏安測試中包圍極大的面積，由此可預期新型電極將有助於提升固態氧化物燃料電池的發電能力；於半電池發電效率的測試，利用0.6mm的8YSZ電解質作支撐，以Pt-ZrO2作為參考陰極，並於5%H2無加濕的環境下具有34.54 mW/cm2之功率密度為常用的Ni-YSZ (28.02 mW/cm2)之1.23倍。

Toughening mechanism and ionic conductivity enhancement in zirconia based ceramics containing Y2O3 and Nb2O5 as co-dopants to ZrO2 as well as Y2O3 and CeO2 as co-dopants to ZrO2 were investigated by using In-situ compression-X-ray diffraction technique with synchrotron radiation, Raman spectrum and Transmission electron microscopy (TEM). The results demonstrated that the co-doping zirconia system containing cubic and tetragonal mixed phases (Partially-stabilized zirconia: PSZ) exhibit outstanding mechanical properties by adding appropriate amount of dopants. The toughness values of PSZ specimens are 1-3 times higher than that of 3mol% yttria stabilized tetragonal zirconia polycrystal (3Y-TZP). Neither tetragonal-to-monoclinic phase transformation nor tetragonal-to-rhombohedral (t-to-r) nor tetragonal-to-orthorhombic (t-to-o) toughening mechanisms nor existence of ferroelastic domain switching of tetragonal phase were observed. Interestingly, a peculiar phase transformation which correlates cubic (c) and metastable tetragonal phases (pseudo-cubic phase: t’) was observed. The crystallographic relationship between c, t’ and new phase was identified as well as lattice parameters of each phase were calculated using TEM in the present study. Besides, the results of dynamic stress-stain curve and in-situ cyclic compression - X-ray diffraction technique with synchrotron radiation were analyzed to understand the contribution of peculiar phase transformation in toughening mechanism. The effect of thermal annealing on the performance of zirconia based ceramics was also discussed.
Electrical properties of zirconia based ceramics demonstrated that the ionic conductivity of zirconia decreases by doping with high lattice binding energy dopants. Oxygen ion migration is found difficult in co-doped zirconia ceramics due to increase in the average binding energy. Moreover, ionic radius of the dopant is identified as another factor that influences the ionic conductivity. When the difference in radius between the dopant and host ions is too large, then a decrease in conductivity was observed due to serious lattice strain in zirconia crystal. The results of the previous investigation concludes that the influencing factors for the enhancement of ionic conductivity in zirconia system were (1) ionic radius of the dopant should be closer to zirconium cation (2) low average binding energy of doped zirconia (3) dopant concentration should not exceed the maximum interfering oxygen vacancies. In the present study, these principles are applied to achieve better ionic conductivity in divalent and trivalent cations co-doped zirconia system. When the amount of dopants exceeds the maximum interfering oxygen vacancies, the low symmetry phase is found. Due to this reason, ionic conductivity of doped zirconia was explained using Raman spectrum and TEM, instead of using general principles like oxygen vacancy clustering and/or occurring of defect association in zirconia specimens. The correlation between outstanding ionic conductivity and local structure of co-doping zirconia system was analyzed by using X-ray absorption spectrum (XAS), near edge X-ray absorption fine structure (NEXAFS) and Fourier transform (FT) method.
Finally, novel anodes were developed with the mixture of 40wt% co-doped zirconia material of high ionic conductivity and 60wt% catalytic Ni. The characteristics like Tafel curve, current-overpotential, cyclic voltammetry curves and power density of half cell were studied to understand the mechanisms involved in the present system of specimens. Experimental results shows that the polarization resistance of Ni-8YSZ decreases significantly from 2.32 Ω-cm2 to 1.57 Ω-cm2 (at 800oC) by substituting Zr0.92Y0.155Mg0.005O2.0775 (MgYSZ) instead of 8YSZ, due to enhancement of triple phase boundary (TPB) area. Moreover, a decrease in activation energy for oxygen ion migration in 8YSZ was observed by modifying appropriate elements to 8YSZ, which is good for enhancing the velocity for oxygen ion migration in 8YSZ crystal and electrochemical reaction, containing oxygen ion oxidation and combination of oxygen and hydrogen to become water in modified anode. The catalytic activity of modified anode was correlated with the value of exchange current density (logi0) measured from Tafel plots under 5% H2 condition. The exchange current densities of modified anodes are found to be much higher than that of Ni-8YSZ. The order of catalytic activity in modified anodes follow Ni-MgYSZ> Ni-CaYSZ> Ni-SrYSZ> Ni-YSZ and hence the catalytic activity of anode is observed to depend on the ionic conductivity of co-doping zirconia in modified anode. Besides, the correlation is also found between logi0 and Rp. Increase in exchange current density and decrease in polarization loss were observed due to mass transfer of oxygen ions and easy charge transfer in modified anodes. The electrochemical reactions of anodes were explained using cyclic voltammetry method. Hysteresis loop like curves whose area increases with an increase of catalytic activity of anode is attributed to the easy formation of oxygen ion oxidation (O2-à1/2O2+2e-). The power density of the half cell Ni-MgYSZ/8YSZ with Pt-8YSZ as reference cathode (34.54 mW/cm2) is 23% higher than that of Ni-8YSZ/8YSZ with Pt-8YSZ as reference cathode (28.02 mW/cm2) at 800oC and the tendency of power density in modified anode is similar to that of catalytic activity variation in anode, indicating that the performance of the fuel cell could be enhanced by employing modified anodes with high ionic conductivity zirconia ceramics.

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