CO₂-to-Methanol Hydrogenation on Zirconia-Supported Copper Nanoparticles: Reaction Intermediates and the Role of the Metal-Support Interface

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• 作者：Dr. Kim Larmier ; Wei-Chih Liao ; Dr. Shohei Tada ; Erwin Lam ; Dr. René ; Verel ; Dr. Atul Bansode ; Prof. Atsushi Urakawa ; Dr. Aleix Comas-Vives and Prof. Christophe Copé ; ret
• 刊名：Angewandte Chemie International Edition
• 出版年：2017
• 出版时间：February 20, 2017
• 年：2017
• 卷：56
• 期：9
• 页码：2318-2323
• 全文大小：2074K
• ISSN：1521-3773

文摘

Methanol synthesis by CO₂ hydrogenation is a key process in a methanol-based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO₂ to methanol still remain unknown. A mechanistic study of the hydrogenation of CO₂ on Cu/ZrO₂ is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO₂ hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.