不同硅铝比ZSM-5负载铁基催化剂二氧化碳加氢性能
发布时间：2018-08-09 12:16
【摘要】：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。
[Abstract]:It is an important way to make high added value chemicals from CO_2 hydrogenation on iron-based catalysts. Iron based catalysts supported on ZSM-5 with different Si / Al ratios (25 / 70150) were prepared by equal volume impregnation method. The effect of Si / Al ratio on the hydrogenation of CO_2 was investigated. The results showed that with the increase of Si / Al ratio, the activity of the catalyst first increased and then decreased. The optimum ratio of Si to Al was 70.CO_2-DRIFTS and CO_2-TPD. The results showed that the catalyst prepared by ZSM-5 support with Si / Al ratio of 70 had more and stronger surface alkaline sites. Promote the activation and dissociation of CO_2 molecules. The evolution of the catalyst structure was revealed by Raman characterization of the catalyst. The active metal of the catalyst after reduction exists in the form of elemental Fe, and during the reaction, the Fe is transformed into Fe3O4 and FeCx species. The interaction between Fe and C, the formation of FeC_x and the activity and selectivity of CO_2 hydrogenation were affected by the coordination environment of Si / Al ratio.
【作者单位】： 化学工程联合国家重点实验室华东理工大学;
【基金】：国家自然科学基金项目(21576084,91534127) 科技部国际合作项目(2015DFG42570)~~
【分类号】：O643.36
[Abstract]:It is an important way to make high added value chemicals from CO_2 hydrogenation on iron-based catalysts. Iron based catalysts supported on ZSM-5 with different Si / Al ratios (25 / 70150) were prepared by equal volume impregnation method. The effect of Si / Al ratio on the hydrogenation of CO_2 was investigated. The results showed that with the increase of Si / Al ratio, the activity of the catalyst first increased and then decreased. The optimum ratio of Si to Al was 70.CO_2-DRIFTS and CO_2-TPD. The results showed that the catalyst prepared by ZSM-5 support with Si / Al ratio of 70 had more and stronger surface alkaline sites. Promote the activation and dissociation of CO_2 molecules. The evolution of the catalyst structure was revealed by Raman characterization of the catalyst. The active metal of the catalyst after reduction exists in the form of elemental Fe, and during the reaction, the Fe is transformed into Fe3O4 and FeCx species. The interaction between Fe and C, the formation of FeC_x and the activity and selectivity of CO_2 hydrogenation were affected by the coordination environment of Si / Al ratio.
【作者单位】： 化学工程联合国家重点实验室华东理工大学;
【基金】：国家自然科学基金项目(21576084,91534127) 科技部国际合作项目(2015DFG42570)~~
【分类号】：O643.36
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