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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
Received:25 May 2020,
Revised:2020-08-14,
Published:05 October 2020
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刘洋洋, 孙超, Malhi Haripal Singh, 位重洋, 张振洲, 涂维峰. 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[J]. 化工学报, 2020, 71(10): 4652-4662 DOI: 10.11949/0438-1157.20200653.
LIU Yangyang, SUN Chao, Singh Malhi Haripal, WEI Chongyang, ZHANG Zhenzhou, TU Weifeng. Effects of identities of supports on Fe-based catalyst and their consequences on activities of CO2 hydrogenation to olefins[J]. CIESC Journal, 2020, 71(10): 4652-4662 DOI: 10.11949/0438-1157.20200653.
刘洋洋, 孙超, Malhi Haripal Singh, 位重洋, 张振洲, 涂维峰. 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[J]. 化工学报, 2020, 71(10): 4652-4662 DOI: 10.11949/0438-1157.20200653. DOI:
LIU Yangyang, SUN Chao, Singh Malhi Haripal, WEI Chongyang, ZHANG Zhenzhou, TU Weifeng. Effects of identities of supports on Fe-based catalyst and their consequences on activities of CO2 hydrogenation to olefins[J]. CIESC Journal, 2020, 71(10): 4652-4662 DOI: 10.11949/0438-1157.20200653. DOI:
铁基催化剂CO
2
加氢直接合成烯烃是实现CO
2
减排及CO
2
转化与利用的最佳途径之一。目前铁基催化剂的CO
2
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CO
2
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CO
2
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CO
2
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CO
2
吸附及活化能力;研究结果表明ZrO
2
负载的Fe催化剂展现出最佳的CO
2
加氢合成烯烃催化性能,在温度320℃和反应压力2.0 MPa时,CO
2
转化率
>
30%,C
2
~C
7
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%。
The direct synthesis of olefins by CO
2
hydrogenation with iron-based catalysts is one of the best ways to achieve CO
2
emission reduction and CO
2
conversion and utilization. At present
the CO
2
hydrogenation activity and structural strength of the iron-based catalysts are still relatively low during CO
2
hydrogenation process
which has become an important challenge for the industrialization of CO
2
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 CO
2
hydrogenation. This work found that the support induced the iron species formed during the process of CO
2
hydrogenation
simultaneously affected the order degree of carbon species on the surface of iron-based catalyst
and tuned the capability of CO
2
adsorption and the activities of CO
2
activation. The results shown that the Fe-based catalyst supported on ZrO
2
exhibited the best catalytic performance for CO
2
hydrogenation to olefins at 320℃ and 2.0 MPa. The CO
2
conversion (
>
30%) and the selectivity of olefins in C
2
—C
7
hydrocarbon products were as high as over 85%
the ratio of olefins to paraffins was 8.2
and the CO selectivity was 17.1%.
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