文献类型：期刊文献

中文题名：不同硅铝比ZSM-5负载铁基催化剂二氧化碳加氢性能

英文题名：CO_(2)hydrogenation over Fe catalysts supported on ZSM-5 zeolite with different ratios of Si/Al

作者：邵光印[1];张玉龙[1];张征湃[1];张俊[1];苏俊杰[1];刘达[1];赫崇衡[1];徐晶[1];韩一帆[1]

机构：[1]化学工程联合国家重点实验室,华东理工大学,上海200237

年份：2017

卷号：68

期号：2

起止页码：670

中文期刊名：化工学报

外文期刊名：CIESC Journal

收录：CSTPCD;;EI(收录号：20172103693184);Scopus;北大核心:【北大核心2014】；CSCD:【CSCD2017_2018】；

基金：国家自然科学基金项目(21576084,91534127);科技部国际合作项目(2015DFG42570)

语种：中文

中文关键词：CO_(2)加氢;Fe基催化剂;ZSM-5;硅铝比;催化;催化剂载体;相变

外文关键词：CO_(2)hydrogenation;Fe based catalysts;ZSM-5;Si/Al ratio;catalysis;catalyst support;phase change

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H_(2)-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Fe_(3)O_(4)和Fe C_(x)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_(2)O_(3)on the catalyst surface was converted into metallic iron,which was then transferred to Fe_(3)O_(4)and Fe C_(x)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 C_(x),thereby affecting the activity and products selectivity of CO_(2)hydrogenation.