Lewis Acid‐Promoted Heterogeneous Platinum Catalysts for Hydrogenation of Amides to Amines
Lewis Acid‐Promoted Heterogeneous Platinum Catalysts for Hydrogenation of Amides to Amines
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DOI：
10.1002/slct.201600088
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发表时间：
2016-04
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影响因子：
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通讯作者：
K. Shimizu;Wataru Onodera;A. S. Touchy;S. H. Siddiki;Takashi Toyao;K. Kon
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文献类型：
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作者：
K. Shimizu;Wataru Onodera;A. S. Touchy;S. H. Siddiki;Takashi Toyao;K. Kon
对于叔酰胺（N-乙酰基哌啶）的氢化，刘易斯酸性载体材料（Nb2O5和MoOx/TiO2）使Pt金属纳米颗粒的催化活性增加> 100倍。原位红外研究表明，酰胺的C = O基团与表面刘易斯酸中心的配位削弱了C = O键，活化后的酰胺发生了氢转移.在所测试的19种多相催化剂中，Pt/Nb_2O_5的催化活性最高。Pt/Nb_2O_5催化剂在无添加剂和无溶剂条件下可有效地将各种叔酰胺和己内酰胺选择性加氢为相应的胺，其转化数（TON）比以前报道的催化剂高。Pt-MoOx/TiO2是第二最有效的，并且在反应后可重复使用10次。
For the hydrogenation of a tertiary amide (N-acetylpiperidine), Lewis acidic support materials (Nb2O5 and MoOx/TiO2) increase the catalytic activity of Pt metal nanoparticles by a factor of >100. In situ infrared (IR) study shows that coordination of the C=O group of amide to surface Lewis acid sites weakens the C=O bond, and the activated amide undergoes hydrogen transfer from H species on Pt sites. Among 19 types of heterogeneous catalysts tested, Pt/Nb2O5 shows the highest catalytic activity. Pt/Nb2O5 is generally effective for the selective hydrogenation of various tertiary amides and ɛ-caprolactam to the corresponding amines under additive-free and solventless conditions and shows an order of higher turnover number (TON) than previously reported catalysts. Pt-MoOx/TiO2 is the secondary most effective and is reusable 10 times after the reaction.