CIESC Journal ›› 2020, Vol. 71 ›› Issue (10): 4652-4662.DOI: 10.11949/0438-1157.20200653

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

Effects of identities of supports on Fe-based catalyst and their consequences on activities of CO2 hydrogenation to olefins

Yangyang LIU1(),Chao SUN2,Malhi Haripal Singh1,Chongyang WEI1,Zhenzhou ZHANG2(),Weifeng TU1,2()   

  1. 1.Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education, Zhengzhou University, Zhengzhou 450001, Henan, China
    2.School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China
  • Received:2020-05-25 Revised:2020-08-14 Online:2020-10-05 Published:2020-10-05
  • Contact: Zhenzhou ZHANG,Weifeng TU

载体对铁基催化剂结构及CO2加氢制烯烃反应性能的影响特性

刘洋洋1(),孙超2,Malhi Haripal Singh1,位重洋1,张振洲2(),涂维峰1,2()   

  1. 1.郑州大学先进功能材料制造教育部工程研究中心,河南 郑州 450001
    2.郑州大学化工学院,河南 郑州 450001
  • 通讯作者: 张振洲,涂维峰
  • 作者简介:刘洋洋(1995—),男,硕士研究生,yangyangliu_zzu51@163.com
  • 基金资助:
    国家自然科学基金项目(21606208);河南省高校科技创新团队支持计划资助(18IRTSTHN)

Abstract:

The direct synthesis of olefins by CO2 hydrogenation with iron-based catalysts is one of the best ways to achieve CO2 emission reduction and CO2 conversion and utilization. At present, the CO2 hydrogenation activity and structural strength of the iron-based catalysts are still relatively low during CO2 hydrogenation process, which has become an important challenge for the industrialization of CO2 hydrogenation to olefins. In this work, a series of the supported iron-based catalyst was prepared by the impregnation method to study the influence of the properties of support materials on the structure of iron-based catalysts and the reactivities of the direct synthesis of olefins from CO2 hydrogenation. This work found that the support induced the iron species formed during the process of CO2 hydrogenation, simultaneously affected the order degree of carbon species on the surface of iron-based catalyst, and tuned the capability of CO2 adsorption and the activities of CO2 activation. The results shown that the Fe-based catalyst supported on ZrO2 exhibited the best catalytic performance for CO2 hydrogenation to olefins at 320℃ and 2.0 MPa. The CO2 conversion (>30%) and the selectivity of olefins in C2—C7 hydrocarbon products were as high as over 85%, the ratio of olefins to paraffins was 8.2, and the CO selectivity was 17.1%.

Key words: carbon dioxide, hydrogenation, catalyst, support, olefins, iron species, alkali metal, Na, surface carbon species

摘要:

铁基催化剂CO2加氢直接合成烯烃是实现CO2减排及CO2转化与利用的最佳途径之一。目前铁基催化剂的CO2加氢活性及反应过程中铁基催化剂结构强度仍然较低,成为CO2加氢制烯烃产业化生产的重要挑战。通过浸渍法制备一系列负载型铁基催化剂,研究载体材料性质对铁基催化剂结构及CO2加氢直接合成烯烃的影响特性。研究发现,载体可诱导铁基催化剂在CO2加氢反应过程中形成的铁物种,同时影响铁基催化剂表面碳物种的有序度,调变对CO2吸附及活化能力;研究结果表明ZrO2负载的Fe催化剂展现出最佳的CO2加氢合成烯烃催化性能,在温度320℃和反应压力2.0 MPa时,CO2转化率>30%,C2~C7烃类产物中烯烃选择性高达85%以上,烯烷比为8.2,且CO选择性较低为17.1%。

关键词: 二氧化碳, 加氢, 催化剂, 载体, 烯烃, 铁物种, 碱金属, 钠, 表面碳物种

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