费-托合成制烯烃铁基催化剂的锆(铬)酸锌载体效应  

Effects of Zinc Zirconate(or Chromate)Support on Catalytic Performance of Fe-Based Catalysts in Fischer-Tropsch Synthesis of Olefins

作　　者：刘振新 高玉集 赵晨曦 贾高鹏 田红美 邢宇 LIU Zhenxin;GAO Yuji;ZHAO Chenxi;JIA Gaopeng;TIAN Hongmei;XING Yu(Henan Provincial Key Laboratory of Surface and Interface Science, School of Materials and Chemical Engineering,Zhengzhou University of Light Industry, Zhengzhou 450002, China)

机构地区：[1]郑州轻工业大学材料与化学工程学院河南省表界面科学重点实验室,河南郑州450002

出　　处：《石油学报（石油加工）》2021年第5期1002-1013,共12页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(21571161);省属高校基本科研业务费专项资金项目(19KYYWF0402);河南省高等学校重点科研项目资助计划(20A150044);郑州轻工业大学博士科研基金项目(2016BSJJ034/CLY20170069/LZX2016);郑州轻工业大学博士单位建设财政配套资助经费项目(13308000212)资助。

摘　　要：制备了Fe/K、铬酸锌型载体担载Fe/K、锆酸锌型载体担载Fe/K以及参比催化剂沉淀铁等4种催化剂。使用XRD、ICP-OES、氮气物理吸附、场发射电子显微镜、二氧化碳化学吸附-程序升温脱附等手段对催化剂进行物化表征。在固定床加压反应器上测试了催化剂的合成气费-托反应性能。结果表明:与参比催化剂沉淀铁相比,锆酸锌型载体担载Fe/K的催化剂可将C=2—C=4烃类选择性提高55%;催化剂表面的中等强度碱性位具有促进C-C偶合、抑制加氢的作用,强碱性位则具有抑制C-C偶合、促进加氢的作用。费-托合成制低碳烯烃铁基催化剂的设计需要注重这2种不同强度表面碱性位的制衡问题。Four types of catalysts,such as Fe/K,zinc chromate supported Fe/K,zinc zirconate supported Fe/K and precipitated iron as reference,were prepared.These catalysts were characterized by XRD,ICP-OES,nitrogen physisorption,field emission electron microscopy,and carbon dioxide chemical adsorption-temperature programmed desorption.The Fischer-Tropsch synthesis of syngas was carried out in a fixed bed pressurized reactor to evaluate the catalytic performance of catalysts.Results show that,compared with the reference precipitated iron catalyst,the selectivity of C=2—C=4 hydrocarbons was increased by 55%with zinc zirconate-supported Fe/K catalyst.It is found that the moderate strength basic sites promote C-C coupling and suppress hydrogenation,while the strong base sites on the catalyst surface weaken C-C coupling and facilitate hydrogenation.The design of iron-based catalysts for Fischer-Tropsch synthesis to light olefins lies to the regulation of two kinds of surface basic sites with different strengths.

关 键 词：费-托合成 CO加氢 低碳烯烃 铁催化剂 复合氧化物 

分 类 号：TQ426.64[化学工程]