温室气体CH4和CO2可作为原料,通过CH4/CO2重整反应制备合成气(CO+H2),合成气可用于通过费-托反应生产高附加值化学品。也就是说,CH4/CO2重整反应可以提供合理利用CH4/CO2的有效途径。分别采用浸渍法和研磨法制备了CoCe催化剂,并用H2-TPR、XRD、BET、Quasi in-situ XPS和CO2-TPD对其物理化学性质进行了表征。Co和Ce物种之间的协同作用可以促进CH4和CO2分子的连续快速活化,从而使CoCe催化剂对CH4/CO2重整反应表现出良好的催化活性。制备方法会影响CoCe催化剂上Co物种的分散和氧空位的热稳定性,从而影响催化活性。浸渍法有利于Co物种溶解在CeO2晶格中形成热稳定性高的氧空位,且CeO2表面处于高度分散的状态的Co物种,可以提供更稳定的催化活性中心。因此,浸渍法制备的催化剂对CH4/CO2重整反应表现出优异的催化性能。在反应温度为600 °C时,CH4和CO2的转化率分别可达43.4%和29.0%。
Hongmei Xie(谢红梅), Na Liu, Juan Huang, Shuang Chen, Guilin Zhou*. CoCe composite catalyst for the CH4/CO2 reforming reaction: synergistic effects between Co and Ce species [J]. Journal of the Energy Institute, 2023, 111: 101389. https://doi.org/10.1016/j.joei.2023.101389
The greenhouse gases CH4 and CO2 can be use as feedstock to prepare syngas (CO + H2) by CH4/CO2 reforming reaction, and the syngas can be used to produce high value-added chemicals through Fischer-Tropsch reaction. That is, the CH4/CO2 reforming reaction can provide an effective way to rationally use CO2 and CH4. The CoCe catalysts were prepared by impregnation method and grinding method, respectively, and the physicochemical properties were characterized by H2-TPR, XRD, BET, Quasi in-situ XPS and CO2-TPD. The synergistic effects between Co and Ce species can promote the CH4 and CO2 molecules to be continuously and rapidly activated, so that the CoCe catalysts exhibited good catalytic activity for the CH4/CO2 reforming reaction. The preparation methods can affect the dispersion of the Co species and the thermal stability of the oxygen vacancies on the CoCe catalysts to affect catalytic activity. The impregnation method is conducive to the Co species dissolving into the CeO2 lattice to form oxygen vacancies with high thermal stability, and the Co species on the CeO2 surface were in a highly dispersed state, which can provide more stable catalytic activity centers. Thus, the catalysts prepared by impregnation method displayed superior catalytic performances for CH4/CO2 reforming reaction. And the CH4 and CO2 conversions can reach 43.4% and 29.0% at the reaction temperature of 600 °C, respectively.