催化学报

催化学报 ›› 2014, Vol. 35 ›› Issue (8): 1337-1346.DOI: 10.1016/S1872-2067(14)60187-X

• 论文 • 上一篇    下一篇

Self-cleaning perovskite type catalysts for the dry reforming of methane

Marí Natividad Pérez-Camachoa, Jehad Abu-Dahrieha, Alexandre Gogueta, Kening Sunb, David Rooneya   

  1. a. CenTACat, School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast, Northern Ireland, BT9 5AG, UK;
    b. Department of Chemistry, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China
  • 收稿日期:2014-06-13 修回日期:2014-07-01 出版日期:2014-08-01 发布日期:2014-08-05
  • 通讯作者: David Rooney

Self-cleaning perovskite type catalysts for the dry reforming of methane

Marí Natividad Pérez-Camachoa, Jehad Abu-Dahrieha, Alexandre Gogueta, Kening Sunb, David Rooneya   

  1. a. CenTACat, School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast, Northern Ireland, BT9 5AG, UK;
    b. Department of Chemistry, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China
  • Received:2014-06-13 Revised:2014-07-01 Online:2014-08-01 Published:2014-08-05

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摘要：

Gas-to-liquid processes are generally used to convert natural gas or other gaseous hydrocarbons into liquid fuels via an intermediate syngas stream. This includes the production of liquid fuels from biomass-derived sources such as biogas. For example, the dry reforming of methane is done by reacting CH4 and CO2, the two main components of natural biogas, into more valuable products, i.e., CO and H2. Nickel containing perovskite type catalysts can promote this reaction, yielding good conversions and selectivities; however, they are prone to coke laydown under certain operating conditions. We investigated the addition of high oxygen mobility dopants such as CeO2, ZrO2, or YSZ to reduce carbon laydown, particularly using reaction conditions that normally result in rapid coking. While doping with YSZ, YDC, GDC, and SDC did not result in any improvement, we show that a Ni perovskite catalyst (Na0.5La0.5Ni0.3Al0.7O2.5) doped with 80.9 ZrO2 15.2 CeO2 gave the lowest amount of carbon formation at 800 ℃ and activity was maintained over the operating time.

关键词: Biogas, Reforming, Perovskite, Oxygen mobility, Dopant

Abstract:

Gas-to-liquid processes are generally used to convert natural gas or other gaseous hydrocarbons into liquid fuels via an intermediate syngas stream. This includes the production of liquid fuels from biomass-derived sources such as biogas. For example, the dry reforming of methane is done by reacting CH4 and CO2, the two main components of natural biogas, into more valuable products, i.e., CO and H2. Nickel containing perovskite type catalysts can promote this reaction, yielding good conversions and selectivities; however, they are prone to coke laydown under certain operating conditions. We investigated the addition of high oxygen mobility dopants such as CeO2, ZrO2, or YSZ to reduce carbon laydown, particularly using reaction conditions that normally result in rapid coking. While doping with YSZ, YDC, GDC, and SDC did not result in any improvement, we show that a Ni perovskite catalyst (Na0.5La0.5Ni0.3Al0.7O2.5) doped with 80.9 ZrO2 15.2 CeO2 gave the lowest amount of carbon formation at 800 ℃ and activity was maintained over the operating time.

Key words: Biogas, Reforming, Perovskite, Oxygen mobility, Dopant