化工学报2018，Vol.69Issue(2)：699-708,10.DOI:10.11949/j.issn.0438-1157.20170996
聚苯胺衍生碳材料负载的Fe基合成气直接制低碳烯烃催化剂:载体碳化温度的影响
Iron-based catalyst on PANI-derived N-containing carbon carriers: effect of carrier carbonization temperature on direct syngas conversion to light olefins
摘要
Abstract
Light olefins are key building blocks for production of many chemical intermediates and polymers in chemical industry, which makes strategically important to produce light olefins directly from non-petroleum syngas resources. It has been found that catalyst carriers significantly affect catalyst performance in CO hydrogenation. A series of Fe-based catalysts on PANI-derived N-containing carbon material, prepared by incipient wetness impregnation at various carbonization temperature, were used to study carbonization temperature on catalytic performance. With the increase of carbonization temperature, both light olefin selectivity and O/P ratio were increased. Fe20/NC-800 catalyst had the highest light olefin selectivity of 41.05%. Catalyst characterization by scanning electron microscope, Raman spectrum and X-ray photoelectron spectrum showed that carbonization temperature increase didn't change carrier structure much, but improved degree of graphitization and decreased total nitrogen content and amount of quaternary nitrogen species. It was also found that amount of pyridinic nitrogen was improved but amount of pyrrole nitrogen species was slightly dropped first and then increased with the increase of carbonization temperature.Moreover,XPS and in situ XRD analysis on surface and bulk structures of catalysts showed that carbonization temperature increase reduced number of high binding energy N species on carrier surface, strengthened electron donating effect on iron, and weakened metal-carrier interaction, which promoted reduction, carbonization and agglomeration of active metal iron and finally enhanced yield of light olefins.关键词
加氢/催化/Fe基催化剂/低碳烯烃/选择性/碳化温度/构-效关系Key words
hydrogenation/catalysis/iron-based catalysts/low olefins/selectivity/carbonization temperature/structure-performance relationship分类
化学化工引用本文复制引用
石变芳,查斌斌,张俊,张征湃,徐晶,韩一帆..聚苯胺衍生碳材料负载的Fe基合成气直接制低碳烯烃催化剂:载体碳化温度的影响[J].化工学报,2018,69(2):699-708,10.基金项目
国家自然科学基金项目(21406062,21576084,91534127).supported by the National Natural Science Foundation of China(21406062,21576084,91534127). （21406062,21576084,91534127）
