Chem. J. Chinese Universities ›› 2022, Vol. 43 ›› Issue (6): 20210842.doi: 10.7503/cjcu20210842

• Physical Chemistry • Previous Articles     Next Articles

Effects of Ag,Zn,Pd-doping on Catalytic Performance of Copper Catalyst for Selective Hydrogenation of Dimethyl Oxalate

SONG Youwei, AN Jiangwei, WANG Zheng, WANG Xuhui, QUAN Yanhong, REN Jun, ZHAO Jinxian()   

  1. State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,China
  • Received:2021-12-20 Online:2022-06-10 Published:2022-04-04
  • Contact: ZHAO Jinxian E-mail:zhaojinxian@tyut.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21808154);the Key Research and Development Program of Shanxi Province, China(201901D211059)

Abstract:

The active crystal planes of Cu(111) and Cu2O(111) doped with Ag, Zn and Pd atoms were constructed using a density functional theory to investigate the effects of different metal doping on the activity and selectivity for dimethyl oxalate(DMO) hydrogenation to methyl glycolate(MG). The results showed that Zn-doping can prohibit the deep hydrogenation of MG effectively, and Ag additves could effectively improve hydrogenation activity for DMO. Conversely, the addition of Pd increased the energy barrier of MG generation, thus reduced MG selectivity. The Ag-Cu(111) surface has a suitable d-center and has the highest activity to generate CH3OOCCH2OH. On the surface of Ag, Zn, Pd atom doped Cu2O(111), Ag-Cu2O(111) has a small band gap and high valence band strength, and has the best catalytic activity in DMO hydrogenation reaction. Based on the above results, theoretical methods for structural modulation and performance regulation of copper-based catalysts are proposed, which provide reliable theoretical guidance for the design of highly efficient catalysts.

Key words: Dimethyl oxalate(DMO), Selective hydrogenation, Cu-based catalyst, Metal-doping

CLC Number: 

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