Fe改性CuZnMn催化剂结构和低碳醇合成反应性能研究  

EFFECT OF IRON ON STRUCTURE AND PERFORMANCE OF CuZnMn CATALYST FOR HIGHER ALCOHOL SYNTHESIS

作　　者：定明月[1,2] 丘明煌[1,2,3] 刘琪英[1,2] 王铁军[1,2] 马隆龙[1,2] 吴创之[1,2] 邱珂[1,2,3] 刘建国[1,2,3] 

机构地区：[1]中国科学院可再生能源与天然气水合物重点实验室,广州510640 [2]中国科学院广州能源研究所,广州510640 [3]中国科学院研究生院,北京100049

出　　处：《太阳能学报》2013年第2期299-304,共6页Acta Energiae Solaris Sinica

基　　金：国家自然科学基金(51206172;51036006);国家重点基础研究发展(973)计划(2013CB228105)

摘　　要：采用连续共沉淀法制备费-托(F-T)组元Fe改性的CuZnMn催化剂,采用N_2物理吸附、H_2-TPR/TPD、XRD等表征手段考察催化剂中Fe-Cu协同作用关系,并在固定床反应器中评价Fe-Cu协同作用的改变对低碳醇合成反应性能的影响。结果表明:CuZnMn催化剂主要以CuMn固溶体形式存在,Fe助剂的加入有利于催化剂比表面积的增加,并促进了FeMn固溶体的形成,降低了固溶体中Cu-Mn相互作用力,这有利于CuO单体逐渐从固溶体中析出,加强了催化剂的还原性能;随着Fe含量的逐渐增加,催化剂中CuO单体含量逐渐增多,Fe-Cu之间形成协同作用,这有利于催化剂活性的提高和醇、烃产物的生成,然而Fe助剂的过量加入则导致催化剂主要表现为F-T合成反应能力,降低低碳醇产物的选择性。The iron-modified CuZnMn catalysts for higher alcohol synthesis were prepared by a continuous co-pre- cipitation method. The synergistic effect of Fe-Cu and influence of this effect on higher alcohol synthesis perform- ances of the catalysts were studied by several techniques, such as N2 physical adsorption, temperature-programmed reduction/desorption of hydrogen, X-ray diffraction. The results indicated that CuZnMn catalyst was mainly com- posed of the CuMn solid solution. The addition of iron was propitious to increase of surface area of the catalyst, the formation of CuMn solid solution and the decrease of Cu-Mn interaction. This resulted in the gradual separation of CuO from the CuMn solid solution, and promoted the reduction of the catalysts. With gradual increase of Fe and Cu0 contents in the catalysts, the synergistic effect of Fe-Cu was enhanced, which promoted the catalytic activity and facilitated the formation of higher alcohol and hydrocarbon products. However, the addition of more iron accel- erated the formation of F-T synthesis active sites, reduced the selectivity of higher alcohol.

关 键 词：低碳混合醇合成 Fe改性 CuZnMn催化剂 协同作用 

分 类 号：O643[理学—物理化学]