本文应用密度泛函理论指导人们深入理解氧化锆溶胶中分子的结构和光谱性能,探讨了溶胶中锆配合物的结构参数、光谱特性和原子的Mulliken 电荷布局. 理论结果表明掺杂引起粒径尺寸减少是由于掺杂引起氧桥聚合速度减慢和颗粒间吸引力的减弱.此外,振动光谱分析表明锆配位前驱体的有序化和第二相掺杂剂的引入明显减少了单斜氧化锆的特征光谱.理论分析结果很好地符合了实验结果.
This work constitutes a study guided to the design of the molecular geometry and the growth process of zirconia gels aided by computer-based calculations (density functional theory). The geometric parameters, spectroscopic properties and Mulliken charge population of zirconium complexes are explored. Theoretical calculations show that the reduced crystallite size of doped-zirconia powder is attributed to the slow oxolation reaction rate because of the reduced intergranular attraction force. Moreover, vibration spectra analysis shows that the order of precursor and the second-phase dopant will apparently reduce the characteristic spectrum of monoclinic-phase zirconia. Our theoretical results are relatively in good accordance with the experimental results.
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