Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO<sub>2</sub> hydrogenation

ZHANG Yulong; SHAO Guangyin; ZHANG Zhengpai; LIU Xianglin; ZHANG Chao; XU Jing; HAN Yifan

doi:10.11949/j.issn.0438-1157.20170995

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Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO₂ hydrogenation

更新时间：2025-12-10

- Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO₂ hydrogenation
- CIESC Journal Issue 2, Pages: 690-698(2018)
- 作者机构：
  
  化学工程联合国家重点实验室, 华东理工大学,上海,200237
- 作者简介：
- 基金信息：
- DOI：10.11949/j.issn.0438-1157.20170995
  CLC： Q018
- Online First：05 February 2018，
  
  Published：05 February 2018
- 稿件说明：
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ZHANG Yulong, SHAO Guangyin, ZHANG Zhengpai, et al. Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO₂ hydrogenation[J]. CIESC Journal, 2018, (2): 690-698. DOI: 10.11949/j.issn.0438-1157.20170995.
DOI：

ZHANG Yulong, SHAO Guangyin, ZHANG Zhengpai, et al. Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO₂ hydrogenation[J]. CIESC Journal, 2018, (2): 690-698. DOI: 10.11949/j.issn.0438-1157.20170995. DOI：

摘要

CO2加氢直接制取低碳烯烃是实现其资源化利用的重要途径。通过热分解法制备了5种不同K含量（1%、3%、5%、7%、9%）的Fe-K催化剂用于CO2加氢反应，结果表明Fe95-K5（95% Fe-5% K，质量分数）催化剂具有最优的活性及C2～C4烯烃选择性；随后对Fe95-K5催化剂进行了10% H2/Ar、10% CO/Ar及5% CO/5% H2/Ar 3种不同气氛活化处理以及CO2加氢反应。结果发现，10% CO/Ar活化的催化剂具有最高的C2～C4烯烃选择性（38.1%）及链增长能力（α=0.644）。此外，还通过X射线衍射、Raman、程序升温等表征技术揭示了催化剂在不同活化气氛下的结构演变历程。研究发现，10% CO/Ar与5% CO/5% H2/Ar活化的催化剂会生成γ1型碳化铁结构，而10% H2/Ar活化的催化剂则会在反应过程中生成γ2型碳化铁结构，两种碳化铁结构对CO2解离均有促进作用。

Abstract

Lower olefins synthesis from direct CO2 hydrogenation over Fe-based catalysts is an important process of CO2 utilization. Iron catalysts with different K loading (1%

7% and 9%) prepared by thermal decomposition were used in CO2 hydrogenation. Fe95-K5 (95%Fe-5%K

mass fraction) catalyst showed the highest activity and C2-C4 olefin selectivity. Further enhancement on Fe95-K5 catalytic performance was achieved by pre-treatment under three different activation atmospheres (10%H2/Ar

10%CO/Ar

5%CO/5%H2/Ar) prior to CO2 hydrogenation. 10%CO/Ar-activated catalyst showed the highest C2-C4 olefin selectivity (38.1%) and chain growth probability (α=0.644). In addition

the structure evolution of Fe95-K5 during activation and CO2 hydrogenation was characterized by X-rays diffraction (XRD)

Raman and temperature-programmed hydrogenation (TPH) techniques. CO introduction in pretreat process accelerated formation of iron carbides. γ1-iron carbide was formed after pretreating in 10%CO/Ar and 5%CO/5%H2/Ar

while γ2-iron carbide was produced in the hydrogenation reaction after pretreating in 10%H2/Ar. Both carbides could promote CO2 dissociation on catalyst surface.

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Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO2 hydrogenation

DOI：10.11949/j.issn.0438-1157.20170995

摘要

Abstract

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Keywords

references

Activation atmospheres on structure-performance relationship of K-promoted Fe catalysts for lower olefin synthesis from CO₂ hydrogenation