Tuning the product selectivity of dimethyl oxalate hydrogenation over WO_(x) modified Cu/SiO_(2) catalysts  

作　　者：Zheng Li Zhuo Ma Yihui Li Ziang Zhao Yuan Tan Ziyin Liu Xingkun Chen Nian Lei Huigang Wang Wei Lu Hejun Zhu Yunjie Ding 

机构地区：[1]Hangzhou Institute of Advanced Studies,Zhejiang Normal University,Hangzhou 311231,Zhejiang,China [2]Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [3]University of Chinese Academy of Sciences,Beijing 100049,China [4]Shaanxi Key Laboratory of Clean Energy Technology Utilization,Yulin Branch,Dalian National Laboratory For Clean Energy,CAS,Yulin 719199,Shaanxi,China [5]State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China

出　　处：《Journal of Energy Chemistry》2024年第10期128-138,I0004,共12页能源化学（英文版）

基　　金：supported by National Natural Science Foundation of China (No.22102147 and 22002151);State Key Laboratory of Chemical Engineering (No.SKL-ChE-22A02);Zhejiang Provincial Natural Science Foundation of China under Grant No.LQ21B030009;the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDA29050300);Qinchuang Yuan high-level innovation and entrepreneurship talents implementing project (No.QCYRCXM-2022-177)。

摘　　要：Product selectivity and reaction pathway are highly dependent on surface structure of heterogeneous catalysts.For vapor-phase hydrogenation of dimethyl oxalate(DMO),"EG route"(DMO→methyl glycolate(MG)ethylene glycol(EG)→ethanol(ET))and"MA route"(DMO→MG→methyl acetate(MA))were proposed over traditional Cu based catalysts and Mo-based or Fe-based catalysts,respectively.Herein,tunable yield of ET(93.7%)and MA(72.1%)were obtained through different reaction routes over WO_(x) modified Cu/SiO_(2) catalysts,and the corresponding reaction route was further proved by kinetic study and in-situ DRIFTS technology.Mechanistic studies demonstrated that H_(2) activation ability,acid density and Cu-WO_(x) interaction on the catalysts were tuned by regulating the surface W density,which resulted in the different reaction pathway and product selectivity.What's more,high yield of MA produced from DMO hydrogenation was firstly reported with the H_(2) pressure as low as 0.5 MPa.

关 键 词：ETHANOL Dimethyl oxalate Selective hydrogenation Methyl acetate WCu/SiO_(2)catalyst 

分 类 号：TQ225.24[化学工程—有机化工] O643.36[理学—物理化学]