表面胺促进的 Cu/SiO2 催化剂用于草酸二甲酯加氢制乙二醇,Industrial & Engineering Chemistry Research

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表面胺促进的 Cu/SiO2 催化剂用于草酸二甲酯加氢制乙二醇
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-06-27 , DOI: 10.1021/acs.iecr.3c01162
Meilin Wang ₁ , Shixin Hou ₁ , Youwei Yang ₁ , Ziheng Zhen ₁ , Jing Lv ₁ , Shouying Huang _{1,

2} , Yue Wang _{1,

2,

3} , Xinbin Ma _{1,

2}

Affiliation

草酸二甲酯 (DMO) 氢化为乙二醇 (EG) 是合成气制乙二醇路线中的关键步骤。氨蒸发法制备的Cu/SiO _{2催化剂在DMO加氢过程中表现出稳定且高度分散的铜物种，已应用于工业中。}然而，EG的催化活性和选择性需要进一步提高。在此，我们利用有机硅烷偶联剂通过后接枝法制备了一系列胺类表面改性的Cu/SiO _{2催化剂。}详细的表征表明，引入的胺类物质可以减少碱性位点的数量和强度，有助于减少副产物（C ₃ –C ₄OH)选择性，从而提高EG选择性。^{胺类物质还表现出给电子效应并显着增加了Cu 0}类物质的比例。同时，证明TOF _Cu与胺类诱导的中强碱性位点之间存在线性相关性，表明铜类与中强碱性位点之间的协同催化作用导致了DMO氢化中优异的催化活性。这些对引入胺类物质影响的见解可能会为改进用于酯加氢的 Cu/SiO _{2催化剂的工业应用带来新的可能性。}

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Surface Amine Species Promoted Cu/SiO2 Catalysts for the Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) is a critical step in the syngas-to-EG route. Cu/SiO₂ catalysts prepared by ammonia-evaporation method exhibited stable and highly dispersed copper species during the DMO hydrogenation which has been used in the industry. However, the catalytic activity and the selectivity of EG require further enhancement. Herein, we prepared a series of surface modified Cu/SiO₂ catalysts with amine species by postgrafting method using organic silane coupling agents. Detailed characterizations indicated that the introduced amine species could reduce the amounts and intensity of basic sites, contributing to the reduction of byproducts (C₃–C₄OH) selectivity, and consequently improve the EG selectivity. The amine species also showed an electron-donating effect and significantly increased the proportion of Cu⁰ species. Meanwhile, it is demonstrated that there was a linear correlation between the TOF_Cu and medium-strong basic sites induced by amine species, indicating the synergistic catalysis between copper species and medium-strong basic sites accounted for the superior catalytic activity in DMO hydrogenation. These insights into the effects of the introduction of amine species could lead to new possibilities for the improvement of Cu/SiO₂ catalysts for ester hydrogenations toward industrial applications.

更新日期：2023-06-27

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