4.7 Article

Efficient hydrogenation of CO2-derived ethylene carbonate to methanol and ethylene glycol over Mo-doped Cu/SiO2 catalyst

期刊

CATALYSIS TODAY
卷 371, 期 -, 页码 113-119

出版社

ELSEVIER
DOI: 10.1016/j.cattod.2020.07.070

关键词

Copper-based catalyst; Ethylene carbonate; Methanol; Ethylene glycol; Hydrogenation; Carbon dioxide

资金

  1. National Key R&D Program of China [2018YFB0605801]
  2. National Natural Science Foundation of China [21706184, 21938008]
  3. Natural Science Foundation of Tianjin City [18JCQNJC06100]
  4. National Postdoctoral Program for Innovative Talents of China [BX20180211]

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A series of Mo-doped Cu/SiO2 catalysts were prepared and used for the hydrogenation of ethylene carbonate (EC), with the 0.5 wt% Mo-doped catalyst exhibiting the highest catalytic performance. The addition of Mo can enhance copper dispersion and prevent aggregation, leading to improved activation of EC. The insights gained from this study may help in designing more efficient copper-based catalysts for the hydrogenation of carbon-oxygen bonds.
Hydrogenation of ethylene carbonate (EC) to methanol and ethylene glycol is an attractive method for indirect hydrogenation of CO2 to methanol. Copper-based catalysts have been studied in EC hydrogenation because of their good selective activation ability for carbon-oxygen bonds. Herein, a series of Mo-doped Cu/SiO2 catalysts were prepared and used for EC hydrogenation. The catalyst with 0.5 wt% Mo dopant exhibited the highest catalytic performance of 80.9 % MeOH yield and 98.6 % EG yield with an excellent stability for at least 140 h. Detailed characterizations revealed that a proper amount of Mo addition could be beneficial to enhancing the copper dispersion and preventing them from aggregation. Moreover, it is demonstrated that the amount of surface Cu+ species was increased with some electron-deficient ones generated resulting from the strong interaction between copper and molybdenum species, which may effectively promote the activation of EC. The optimal 0.5 wt% Mo-doped catalyst showed remarkably enhanced efficiency and the apparent activation energy barrier of 115.8 kJ mol-1 is much lower than that of the Mo-free sample in EC hydrogenation. The insights may bring new possibilities to further design efficient copper-based catalysts for the hydrogenation of carbon-oxygen bonds.

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