Chinese Journal of Catalysis ›› 2020, Vol. 41 ›› Issue (7): 1140-1151.DOI: 10.1016/S1872-2067(20)63544-6

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Chemical looping partial oxidation over FeWOx/SiO2 catalysts

Rui Liua,b, Chunlei Peia,b, Xianhua Zhanga,b, Sai Chena,b, Hongfang Lia,b, Liang Zenga,b, Rentao Mua,b, Jinlong Gonga,b   

  1. a Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
    b Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China
  • Received:2019-09-30 Online:2020-07-18 Published:2020-04-18
  • Supported by:
    This work was supported by the National Key R&D Program of China (2016YFB0600901), the National Natural Science Foundation of China (51761145012, 21525626, U1663224), and the Program of Introducing Talents of Discipline to Universities (B06006). We also acknowledge the financial support from China National Petroleum Corporation for this research.

Abstract: This paper describes the design of a FeWOx-based oxygen carrier for the chemical partial oxidation of methane (CLPOM). Thermodynamic screening and kinetic analyses both forecast the FeWOx-based oxygen carrier as a promising candidate for the production of syngas. The total methane conversion and syngas yield can be dramatically increased with this catalyst compared to the case with the unmodified WO3/SiO2, thereby enabling CLPOM with 62% methane conversion, 93% CO gas-phase selectivity, 94% H2 selectivity, and a 2.4 H2/CO ratio. The catalyst has the advantages of high availability of lattice oxygen to oxidize carbonaceous intermediates in time, together with the formation of an Fe-W alloy to promote the surface reaction. Consequently, it demonstrates excellent catalytic performance with no catalyst deactivation at 900 ℃ and 1 atm. The excellent structural stability plays an essential role in CLPOM. As revealed via XPS and ICP, the phase segregation has not been observed due to the strong interaction between Fe and W, which resulted in the formation of the Fe-W alloy during the reduction processes and the match between the ion oxidation rates of the Fe and W ions in the oxidation stage. The results provide fundamental information on the reaction mechanism of FeWOx/SiO2, and present it as a promising candidate for CLPOM.

Key words: Fe-W alloy, Methane activation, Lattice oxygen diffusion, Phase segregation, Ion oxidation rate