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Catalytic hydrogenation of tertiary amides at low temperatures and pressures using bimetallic Pt/Re-based catalysts

机译:使用双金属Pt / Re基催化剂在低温和低压下催化叔酰胺加氢

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摘要

Hydrogenation of tertiary amides, in particular, N-methylpyrrolidin-2-one, can be efficiently facilitated by a TiO_2-supported bimetallic Pt/Re catalyst at low temperatures and pressures. Characterisation of the catalysts and kinetic tests have shown that the close interaction between the Re and Pt is crucial to the high activity observed. DFT calculations were used to examine a range of metal combinations and show that the role of the uncoordinated Re is to activate the CO and that of the Pt is as a hydrogenation catalyst, removing intermediates from the catalyst surface. The rate enhancement observed on the TiO_2 support is thought to be due to the presence of oxygen vacancies allowing adsorption and weakening of the CO bond.
机译:TiO_2负载的双金属Pt / Re催化剂在低温和低压下可以有效地促进叔酰胺,特别是N-甲基吡咯烷酮-2-酮的氢化。催化剂的表征和动力学测试表明,Re和Pt之间的紧密相互作用对观察到的高活性至关重要。 DFT计算用于检查各种金属组合,并表明未配位的Re的作用是活化CO,而Pt的作用是作为氢化催化剂,从催化剂表面除去中间体。认为在TiO_2载体上观察到的速率提高是由于存在氧空位,从而允许吸附和削弱CO键。

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