本文中我們利用理論計算來研究CO, O2在IrO2 (110)表面上進行吸附作用，以及在IrO2 (110)表面上進行O2裂解反應與CO氧化反應。本研究中模擬計算最佳化後的IrO2單元晶胞之powder x-ray diffraction pattern以及目前廣用的Rietceld refinement method來驗證實驗與模擬的精確性，並且得到一與實驗值誤差極小的單元晶胞。計算結果顯示，IrO2 (110)表面的表面重構不明顯。可見金紅石IrO2 (110)的表面相當穩定。本研究中，我們計算了CO分子與不同型態的氧原子進行氧化反應，結果顯示CO在多氧環境下的氧化反應有較低的能障。此外，在本文中我們模擬不同覆蓋率的貴金屬於IrO2 (110)表面上的吸附作用。在 ML覆蓋率下，貴金屬最穩定的吸附位置為沿著[001]方向，吸附於Obr原子與Ircus原子之間。Ir原子與Pt原子的平均吸附能分別為5.13 eV以及3.81 eV。隨著覆蓋率增加到 ML，貴金屬平均的吸附能也跟著下降，在Ir/IrO2與Pt/IrO2表面中，最穩定的吸附位置為沿著[001]方向，吸附於Obr原子與Ircus原子之間。在Pt2Ir/IrO2中最穩定的吸附位置為沿著[ ]方向，吸附於Obr原子與Ircus原子之間。本研究在IrO2, Pt/IrO2, Ir/IrO2, PtIr/IrO2表面進行水裂解反應。由計算結果顯示，較高覆蓋率之貴金屬吸附在IrO2 (110)表面上對於水裂解反應有良好的催化效果。我們也在IrO2, Pt/IrO2, Ir/IrO2, Pt2IrO2進行CO氧化反應以及CO2脫附的模擬。計算結果顯示Pt/IrO2表面對CO氧化反應以及CO2脫附有良好的催化效果。

A DFT study of the adsorption and reaction of CO, O2 and H2O on the IrO2 rutile-type (110) 2 × 1 surface was performed. The structural identification was determined via a simulation of X-ray powder diffraction (XRD). Structure parameters of IrO2 were refined by the Rietveld method from simulated XRD data. The calculated XRD is in good agreement with previous experimental works by Natl. et al. The calculated results show that the surface reconstruction of IrO2 (110) surface is not obvious due to its rutile structure. In addition, the potential energy surfaces of CO oxidation with different oxygen species on the surfaces were examined. The barrier of CO oxidation on the oxygen-rich surface is lower. Furthermore, the Ir and Pt adsorptions on the IrO2 (110) 2 × 1 surface at coverage of 1/2 and 3/4 ML were simulated. It has been found that the most stable site of the 1/2 ML is with the metal atom bridging between Obr atom and Ircus atom along the [001] direction. The adsorption energy of Ir and Pt are 5.13 eV and 3.81 eV, respectively. The simulation model of Pt2Ir/IrO2 (110) surface at a metal coverage of 3/4 ML is sequential addition of Pt to the 1/2 ML PtIr/IrO2 (110) surface, and the most stable site of Pt2Ir/IrO2 surface is Pt metal bridging between Obr atom and Ircus atom along the[ ]direction. At the coverage of 3/4 ML, the average adsorption energy per atom is lower than that at the coverage of 1/2 ML. Final, the CO oxidation with H2O on the Pt-Ir/IrO2 (110) surface is also examined. The reaction energies and barriers for the water dissociation and CO oxidation have been predicted in solid—gas interface. On the basis of energetics, the Pt/IrO2 (110) surface has good catalytic ability for water dissociation and CO oxidation reaction

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