Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

DOI HANDLE Web Site 被引用文献1件 参考文献101件 オープンアクセス

この論文をさがす

説明

Oxidative addition of CH_4 to the catalyst surface produces CH_3 and H. If the CH_3 species generated on the surface couple with each other, reductive elimination of C_2H_6 may be achieved. Similarly, H’s could couple to form H_2. This is the outline of nonoxidative coupling ofmethane (NOCM). It is difficult to achieve this reaction on a typical Pt catalyst surface. This is because methane is overoxidized and coking occurs. In this study, the authors approach this problem from a molecular aspect, relying on organometallic or complex chemistry concepts. Diagrams obtained by extending the concepts of the Walsh diagram to surface reactions are used extensively. C–H bond activation, i.e., oxidative addition, and C–C and H–H bond formation, i.e., reductive elimination, on metal catalyst surfaces are thoroughly discussed from the point of view of orbital theory. The density functional theory method for structural optimization and accurate energy calculations and the extended Hückel method for detailed analysis of crystal orbital changes and interactions play complementary roles. Limitations of monometallic catalysts are noted. Therefore, a rational design of single atom alloy (SAA) catalysts is attempted. As a result, the effectiveness of the Pt_1/Au(111) SAA catalyst for NOCM is theoretically proposed. On such an SAA surface, one would expect to find a single Pt monatomic site in a sea of inert Au atoms. This is desirable for both inhibiting overoxidation and promoting reductive elimination.

収録刊行物

被引用文献 (1)*注記

もっと見る

参考文献 (101)*注記

もっと見る

関連プロジェクト

もっと見る

詳細情報 詳細情報について

問題の指摘

ページトップへ