Si对Fe-Zr-O催化CO_2与甲醇合成碳酸二甲酯反应性能的影响  

Effect of Si on the Catalytic Properties of Fe-Zr-O for Synthesis of Dimethyl Carbonate from CO_2 and Methanol

作　　者：陈红萍[1,2] 郑小满[1] 梁英华[1] 赵新强[2] 

机构地区：[1]河北联合大学化学工程学院,河北唐山063009 [2]河北工业大学化工学院,天津300130

出　　处：《石油化工》2014年第10期1149-1155,共7页Petrochemical Technology

基　　金：河北省教育厅项目(2010133);唐山市科技局项目(09110202A-1-1)

摘　　要：采用溶胶-凝胶法制备了Si-Fe-Zr-O催化剂,利用N2吸附-脱附、SEM-EDX、TEM、XRD和NH3-TPD等方法对Si-Fe-Zr-O催化剂的织构性质、组成和酸性进行了表征,并考察了Si-Fe-Zr-O催化剂催化CO2与甲醇合成碳酸二甲酯的性能.实验结果表明,随Si加入量的增加,催化剂的比表面积增大,孔径减小且孔分布集中;当n（Fe）∶n（Zr）∶n（Si）=5∶1∶2时,存在便于传质的5～11 nm的孔且孔体积最大,催化活性最高;较大的比表面积和合适的孔径是引入Si后催化剂活性提高的主要原因.si的加入所形成的锆硅和铁硅固溶体可与铁锆固溶体协同作用,提高Si-Fe-Zr-O催化剂的活性.Si-Fe-Zr-O catalysts were prepared by sol-gel method and characterized by means of N2 adsorption-desorption,SEM-EDX,TEM,XRD and NH3-TPD.The effects of the addition of Si on the structure,acidity and catalytic activity of the catalysts in the synthesis of dimethyl carbonate from methanol and carbon dioxide were investigated.The results showed that,with increasing the silicon content,the BET specific surface area increased,and the pore diameter became small and concentrated.When n（Fe） ∶ n（Zr） ∶ n（Si） was 5 ∶ 1 ∶ 2,the pore volume was the biggest and there were the pores with the pore size of 5-11 nm,which was beneficial to mass transfer.So the big specific surface area and suitable pore size were the major reasons for the high activity of the Si-FeZr-O catalysts.In addition,the synergistic effects between the solid solutions,namely zirconiumsilicon,iron-silicon and iron-zirconium,could improve the performances of the Si-Fe-Zr-O catalysts.

关 键 词：碳酸二甲酯 甲醇 二氧化碳 铁-锆-氧催化剂 二氧化硅 

分 类 号：TQ426.82[化学工程]