化工学报2018,Vol.69Issue(2):690-698,9.DOI:10.11949/j.issn.0438-1157.20170995
活化气氛对CO2加氢制取低碳烯烃Fe-K催化剂构-效关系
Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO2hydrogenation
摘要
Abstract
Lower olefins synthesis from direct CO2 hydrogenation over Fe-based catalysts is an important process of CO2 utilization. Iron catalysts with different K loading (1%, 3%, 5%, 7% and 9%) prepared by thermal decomposition were used in CO2 hydrogenation. Fe95-K5 (95%Fe-5%K,mass fraction) catalyst showed the highest activity and C2—C4 olefin selectivity. Further enhancement on Fe95-K5 catalytic performance was achieved by pre-treatment under three different activation atmospheres (10%H2/Ar, 10%CO/Ar, 5%CO/5%H2/Ar) prior to CO2 hydrogenation. 10%CO/Ar-activated catalyst showed the highest C2—C4olefin selectivity (38.1%) and chain growth probability (α=0.644). In addition, the structure evolution of Fe95-K5 during activation and CO2 hydrogenation was characterized by X-rays diffraction (XRD), Raman and temperature-programmed hydrogenation (TPH) techniques. CO introduction in pretreat process accelerated formation of iron carbides. Γ1-iron carbide was formed after pretreating in 10%CO/Ar and 5%CO/5%H2/Ar, while γ2-iron carbide was produced in the hydrogenation reaction after pretreating in 10%H2/Ar. Both carbides could promote CO2 dissociation on catalyst surface.关键词
CO2加氢/Fe-K催化剂/活化气氛/低碳烯烃/构-效关系Key words
CO2hydrogenation/Fe-K/activation atmospheres/lower olefins/structure-performance relationship分类
化学化工引用本文复制引用
张玉龙,邵光印,张征湃,刘向林,张超,徐晶,韩一帆..活化气氛对CO2加氢制取低碳烯烃Fe-K催化剂构-效关系[J].化工学报,2018,69(2):690-698,9.基金项目
国家自然科学基金项目(21576084,91534127).supported by the National Natural Science Foundation of China(21576084,91534127). (21576084,91534127)