CO_2加氢在铁基催化剂上直接制取高附加值化学品是实现其资源化利用的重要途径。通过等体积浸渍法制备了不同硅铝比(25,70,150)的ZSM-5负载的铁基催化剂,考察硅铝比对铁基催化剂上CO_2加氢性能的影响。结果表明,随着硅铝比的升高,催化剂活性先升高后降低,最优化硅铝比为70。CO_2-DRIFTS和CO_2-TPD结果显示,硅铝比为70的ZSM-5载体制备的催化剂具有较多且较强的表面碱性位,促进CO_2分子的活化解离。通过H2-TPR、XRD、Raman等表征揭示了催化剂结构的演变过程。还原后催化剂的活性金属以单质Fe形式存在,反应过程中单质Fe向Fe3O4和Fe Cx物种转化。不同硅铝比配位环境影响Fe与C的相互作用,影响FeC_x的生成,从而影响CO_2加氢的活性和选择性。
CO_2 hydrogenation directly producing value added chemicals over Fe based catalysts is an important approach to achieve its resource-oriented utilization. In this work, ZSM-5 supported iron catalysts with different ratios of Si/Al(25, 70, 150) were prepared by conventional impregnation method and the effects of supports with different Si/Al ratios on the catalytic performance were investigated. The catalyst activity increased first, then decreased with the increase of Si/Al ratio, and the optimal ratio of Si/Al was 70. With the combination of CO_2-DRIFTS and CO_2-TPD, it was found that ZSM-5(Si/Al=70) zeolite supported Fe catalyst possessed more and stronger basic sites, which promoted the dissociative activation of CO_2. The evolution of catalysts structure was explored using multiple techniques such as H_2-TPR, XRD and Raman spectroscopy. After reduction, Fe_2O_3 on the catalyst surface was converted into metallic iron, which was then transferred to Fe_3O_4 and Fe Cx during the reaction. It was also found that the discrepancy in the interaction between Fe and C under different coordination environments(Si/Al) affects the formation of Fe Cx, thereby affecting the activity and products selectivity of CO_2 hydrogenation.