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Synergic catalysis by a CuO-like phase and Cu0 for anaerobic dehydrogenation of 2,3-butanediol
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-01-09 , DOI: 10.1016/j.jcat.2019.12.016
Enxian Yuan , Ping Ni , Wanli Zhuang , Ruiqi Jian , Panming Jian

This paper describes an emerging synthetic route for acetoin production via the anaerobic dehydrogenation of 2,3-butanediol to give a deep understanding of the specific dehydrogenation behavior of diols. Cu/SBA-15-x-T prepared by the ammonia evaporation method was applied to the dehydrogenation of 2,3-butanediol. The results of XRD, FTIR, H2-TPR, XPS, and NH3-TPD characterization verified that the CuO-like phase, with a Cu2+O2− pair, existed in the form of -Si-O-Cu-O-Si- structures in Cu/SBA-15-x-T catalysts. The amounts of the CuO-like phase and Cu0 can be tuned simultaneously by adjusting the synthetic solution alkalinity and reduction temperature to achieve an optimal synergic effect between the CuO-like phase and Cu0 sites. Compared with the catalytic inertness of Cu catalysts prepared by the conventional impregnation method, the resulting Cu/SBA-15-10.0-300 showed superior catalytic performance (reaction rate: 9.90 × 10−3 mol·min−1g−1) in 2,3-butanediol dehydrogenation. Studies on the structure–performance correlation based on the kinetic study revealed that the catalytic activity of Cu/SBA-15-x-T catalysts is attributable to synergic catalysis between the interfacial CuO-like phase and Cu0 sites, which favors the bond cleavage of O-H and α-C-H, respectively.



中文翻译:

类CuO相和Cu 0协同催化2,3-丁二醇的厌氧脱氢

本文介绍了一种新兴的合成路线,该路线是通过2,3-丁二醇的厌氧脱氢来生产乙醛的方法,以使人们对二醇的特定脱氢行为有更深入的了解。通过氨蒸发法制备的Cu / SBA-15-xT被用于2,3-丁二醇的脱氢。XRD,FTIR,H 2 -TPR,XPS和NH 3 -TPD表征的结果证实,具有Cu 2+ O 2−对的CuO样相以-Si-O-Cu-的形式存在。 Cu / SBA-15-xT催化剂中的O-Si-结构。类CuO和Cu 0的量通过调节合成溶液的碱度和还原温度,可同时调节H 2 O 3,以在CuO样相和Cu 0位之间实现最佳协同作用。与通过常规浸渍方法制备的Cu催化剂的催化惰性相比,所得到的Cu / SBA-15-10.0-300在2中显示出优异的催化性能(反应速率:9.90×10 -3  mol·min -1 g -1)。 ,3-丁二醇脱氢。基于动力学研究的结构-性能相关性研究表明,Cu / SBA-15-xT催化剂的催化活性归因于界面CuO类相与Cu 0之间的协同催化作用。 个位点,分别有利于OH和α-CH的键裂解。

更新日期:2020-01-11
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