CO-Mediated Deactivation Mechanism of SiO2-Supported Copper Catalysts during Dimethyl Oxalate Hydrogenation to Ethylene Glycol

CO-Mediated Deactivation Mechanism of SiO2-Supported Copper Catalysts during Dimethyl Oxalate Hydrogenation to Ethylene Glycol
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CO介导的SiO2负载铜催化剂草酸二甲酯加氢制乙二醇失活机制

DOI:
10.1021/acs.jpcc.5b03569
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发表时间:
2015-06
影响因子:
3.7
通讯作者:
Yuan Youzhu
Yuan Youzhu
中科院分区:
化学3区
文献类型:
--
作者:
Zheng Jianwei;Zhou Junfu;Lin Haiqiang;Duan Xinping;Williams Christopher T.;Yuan Youzhu

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在铜(Cu)基催化剂上,由合成气衍生的草酸二甲酯(DMO)选择性加氢制乙二醇(EG)是现代合成气化学工业的一种重要转化。甲醇作为一种产物或溶剂,能够在铜上解离。
Selective hydrogenation of dimethyl oxalate (DMO) derived from syngas to ethylene glycol (EG) over copper (Cu)-based catalysts is an important transformation of modern syngas chemical industry. Methanol, as a product or a solvent, can dissociate on the Cu surfaces by forming adsorbed CO under H2 atmosphere at 473 K. A small amount of adsorbed CO accelerates Cu redox processes, thus inhibiting catalytic activity with a negative kinetic reaction order. The strong interaction between CO and Cu blocks active sites and disrupts the synergy of Cu+ and Cu0 species, which are vital in DMO hydrogenation. The Ostwald ripening of Cu crystallites is induced by CO, resulting in aggregation of Cu crystallites. The imbalance of active species and crystallite aggregation lead to deactivation of the Cu catalysts during DMO hydrogenation to EG.
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