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Hydrogenation of diesters on copper catalyst anchored on ordered hierarchical porous silica: Pore size effect
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-12-14 , DOI: 10.1016/j.jcat.2017.11.006
Yujun Zhao , Ziyuan Guo , Haojie Zhang , Bo Peng , Yuxi Xu , Yue Wang , Jian Zhang , Yan Xu , Shengping Wang , Xinbin Ma

An ordered hierarchical porous silica (HPS) presenting both mesopores and micropores was fabricated and used for supporting copper catalysts (Cu/HPS). In the prepared Cu/HPS catalysts, high dispersion of both Cu0 and Cu+ species together with ordered porous structure were achieved. The anchoring effect of micropores hindered the agglomeration of copper species, while the formation of Cu-O-Si species, derived from the strong interaction between surface silica and copper precursor, was prompted by the ammonia evaporation approach. The Cu/HPS catalysts were tested in the hydrogenation of diesters to diols. It shows excellent activity on dimethyl adipate hydrogenation with a 1,6-hexanediol space-time yield of 0.72 g/(g∙h) under WHSV = 1.2 h−1. It was further investigated that the activity in dimethyl adipate hydrogenation, in contrast to that of dimethyl oxalate hydrogenation, would be readily limited by pore diffusion, due to the porous structure of HPS.



中文翻译:

固定在有序多孔二氧化硅上的铜催化剂上二酯的加氢:孔径效应

制备了同时具有中孔和微孔的有序的分级多孔二氧化硅(HPS),并用于支撑铜催化剂(Cu / HPS)。在制备的Cu / HPS催化剂中,Cu 0和Cu +物种的高分散性以及有序的多孔结构均得以实现。微孔的锚固作用阻碍了铜物质的团聚,而氨蒸发法促使了表面二氧化硅与铜前体之间强烈的相互作用而形成了Cu-O-Si物质。在将二酯氢化成二醇中测试了Cu / HPS催化剂。在WHSV = 1.2 h -1时,它对己二酸二甲酯加氢显示出优异的活性,1,6-己二醇的时空产率为0.72 g /(g∙h)。进一步研究了由于草甘膦的多孔结构,与草酸二甲酯加氢相反,己二酸二甲酯加氢的活性很容易受到孔扩散的限制。

更新日期:2017-12-14
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