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The Configuration and electronic state of SO$$_{3}$$ adsorbed on Au surface

Au表面に吸着したSO$$_{3}$$の配置と電子状態

鈴木 知史; 中桐 俊男

Suzuki, Chikashi; Nakagiri, Toshio

日本原子力研究開発機構では、高速増殖炉で(FBR)発生する熱と電気を利用した水素製造プロセスとして、ハイブリッド熱化学法を開発している。このプロセスには、三酸化イオウ(SO$$_{3}$$)分解が含まれている。しかしながら、SO$$_{3}$$の電気分解の反応機構は明らかでなく、さらなる高性能化には、反応機構を明らかにする必要がある。これまでに、第一原理計算を実施してSO$$_{3}$$のPt電極表面への吸着・解離反応を明らかにしてきた。さらに電極の高性能化のため、実験より比較的優れた特性を示したAuについての検討を行うため、第一原理計算を実施した。計算結果より、Au表面上でSO$$_{3}$$は6種類の安定構造を取ることが明らかとなった。

We evaluated the adsorption of SO$$_{3}$$ molecule on the Au (111) surface using the first-principles calculations by a slab model with a periodic boundary condition. We find that there are six stable adsorption configurations on the Au surface, where SO$$_{3}$$ molecules are adsorbed above the three-fold fcc and hcp hallow sites and atop site. In two of these configurations, S and two O atoms are bound to the Pt atoms, and in two other of them, all the three O atoms are bound to Pt surface atoms, and then, S atom is bound to Au surface atom on the atop site and O atoms are situated on the hallow sites. In addition, it is found that molecular orbitals of SO$$_{3}$$ and those of Au surface are hybridized in the active metal d-bands region, that the localized molecular orbitals in SO$$_{3}$$ are stabilized, and that the charge is transferred from Au to S 3p by SO$$_{3}$$ adsorption on Au surface though the other interaction of S and O (bound to Au) component with Au is little. In addition, the bond between S and O bound to Au become weak by SO$$_{3}$$ adsorption on Au surface because the charge polarization to O-Au bond weakens the bond between S and O bound to Au. This interaction is assumed to encourage the breakage of S-O bond.

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パーセンタイル:80.91

分野:Chemistry, Multidisciplinary

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