Chinese Journal of Catalysis ›› 2013, Vol. 34 ›› Issue (5): 956-963.DOI: 10.1016/S1872-2067(12)60559-2

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Hydrogenation of carbon dioxide to light olefins over non-supported iron catalyst

YOU Zhenya, DENG Weiping, ZHANG Qinghong, WANG Ye   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Production of Alcohols, Ethers, and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
  • Received:2013-01-12 Revised:2013-05-20 Online:2013-05-06 Published:2013-05-06
  • Supported by:

    This work was supported by the National Basic Research Program of China (973 Program, 2013CB933100), the National Natural Science Foundation of China (21173174, 20923004, 21033006, and 21161130522), the Specialized Research Fund for the Doctoral Program of Higher Education (20090121110007), and the Program for Innovative Research Team in University (IRT1036).

Abstract:

The hydrogenation of CO2 to light olefins was investigated over non-supported Fe catalysts. It was found that the addition of alkali metal ions to the Fe catalyst led to significant increases in both the CO2 conversion and the selectivity for olefins. Over K- or Rb-modified catalysts, about 40% CO2 conversion and more than 50% olefin selectivity were obtained. The yield of C2-C4 olefins exceeded 10% over these modified catalysts. Catalyst characterization suggested that the formation of iron carbide species was accelerated by the modification of the Fe catalyst with alkali metal ions, and this enhancement may be one of the key reasons for the enhanced catalytic performance. For the K-modified Fe catalysts, K content has a major influence on the catalyst behavior. An increase in the K content from 1 to 5 wt% increased both CO2 conversion and olefin selectivity. However, too high a K content led to a decrease in the activity, probably because of decreases in the surface area and CO2 chemisorption capacity of the catalyst. The presence of an appropriate amount of B in the K-modified Fe catalyst was found to be beneficial to the olefin selectivity, without significantly decreasing the conversion of CO2.

Key words: Carbon dioxide, Hydrogenation, Light olefin, Iron catalyst