载体对Fe基催化剂CO<sub>2</sub>催化加氢制低碳烯烃性能的影响

李广辉; 张艳艳; 王萌; 高健; 张振洲; 孙绍晖

doi:10.12434/j.issn.2097-2547.20240125

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载体对Fe基催化剂CO₂催化加氢制低碳烯烃性能的影响

C1化学与催化转化

- 载体对Fe基催化剂CO₂催化加氢制低碳烯烃性能的影响
- Effects of supports on catalytic performances of Fe-based catalysts for CO₂ hydrogenation to light olefins
- 低碳化学与化工 2024, 49(12): 19-26.
- 作者机构：
  
  1.郑州大学炼焦煤资源绿色开发国家重点实验室，河南郑州 450001
  2.郑州大学化工学院先进功能材料制造教育部工程研究中心，河南郑州 450001
- 作者简介：
  
  李广辉（1998—），硕士研究生，研究方向为CO2催化加氢制低碳烯烃，E-mail：13592420562@163.com。
  高健（1980—），博士，副教授，研究方向低碳资源高附加值转化，E-mail：gaojian@zzu.edu.cn。
- 基金信息：
  
  国家自然科学基金青年项目(22208314);科技部“十三五”国家重点研发计划子课题(2018 YFB060450402)
- DOI：10.12434/j.issn.2097-2547.20240125
  中图分类号： TQ221.21;O643.32
- 纸质出版日期：2024-12-25，
  
  收稿日期：2024-03-28，
  
  修回日期：2024-04-11，
- 稿件说明：
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李广辉,张艳艳,王萌等.载体对Fe基催化剂CO₂催化加氢制低碳烯烃性能的影响[J].低碳化学与化工,2024,49(12):19-26.

LI Guanghui,ZHANG Yanyan,WANG Meng,et al.Effects of supports on catalytic performances of Fe-based catalysts for CO₂ hydrogenation to light olefins[J].Low-carbon Chemistry and Chemical Engineering,2024,49(12):19-26.
李广辉,张艳艳,王萌等.载体对Fe基催化剂CO₂催化加氢制低碳烯烃性能的影响[J].低碳化学与化工,2024,49(12):19-26. DOI： 10.12434/j.issn.2097-2547.20240125.

LI Guanghui,ZHANG Yanyan,WANG Meng,et al.Effects of supports on catalytic performances of Fe-based catalysts for CO₂ hydrogenation to light olefins[J].Low-carbon Chemistry and Chemical Engineering,2024,49(12):19-26. DOI： 10.12434/j.issn.2097-2547.20240125.

摘要

选择适宜载体对于合理设计高效CO

催化加氢制低碳烯烃（乙烯、丙烯和丁烯）的新型Fe基催化剂十分重要。采用水热法合成不同载体并浸渍K和Fe制备了一系列Fe基催化剂（K-Fe/ZrO

、K-Fe/ZnO、K-Fe/TiO

和K-Fe/Al

），考察了载体对催化剂CO

催化加氢性能的影响。采用XRD、N

吸/脱附、Raman、CO-TPD、CO

-TPD、原位Raman和水接触角测试等表征方法，研究了载体对Fe活性物种生成的诱导作用。结果表明，在温度320 ℃、压力2.0 MPa、原料气

(CO

(Ar) = 1:3:3和气时空速10000 mL/(g·h)的反应条件下，K-Fe/ZrO

表现出较高低碳烯烃选择性（42.4%）和CO

转化率（36.2%）。与其他催化剂相比，K-Fe/ZrO

对CO和CO

具有适宜强度的吸附性能，有利于CO

活化和碳沉积，在获得更多Fe

活性物种的同时，抑制了烯烃二次加氢。此外，K-Fe/ZrO

在反应过程中因碳沉积而具有较强疏水性，进一步减轻了Fe

被水氧化的程度，提高了低碳烯烃选择性。

Abstract

The selection of suitable support is crucial for the rational design of novel and efficient Fe-based catalysts for CO

hydrogenation to light olefins (ethylene

propylene and butene). Supports were synthesized by hydrothermal method

and impregnated with K and Fe to prepare a series of Fe-based catalysts (K-Fe/ZrO

K-Fe/ZnO

K-Fe/TiO

and K-Fe/Al

). The effects of these supports on the catalytic performance of CO

hydrogenation were investigated. The catalysts were characterized by XRD

absorption/desorption

Raman

CO-TPD

-TPD

in suit Raman and water droplet contact angle tests

and the induction effects of supports on the generation of Fe active species were studied. The results show that under reaction conditions of temperature of 320 ℃

pressure of 2.0 MPa

feed gas

(CO

(Ar) = 1:3:3 and gas hourly space velocity of 10000 mL/(g·h)

K-Fe/ZrO

exhibites superior selectivity of light olefins (42.4%) and CO

conversion rate (36.2%). Compared to other catalysts

K-Fe/ZrO

has a suitable adsorption capacity for CO and CO

which is beneficial for CO

activation and carbon deposition. It also inhibits the secondary hydrogenation of olefins while obtaining more Fe

active species. Additionally

K-Fe/ZrO

exhibites strong hydrophobicity due to carbon deposition during the reaction process

further reducing the degree of water oxidation of Fe

and improving the selectivity of light olefins.

关键词

CO2加氢低碳烯烃载体动态演变Fe基催化剂

Keywords

CO2 hydrogenationlight olefinssupportdynamic evolutionFe-based catalysts

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载体对Fe基催化剂CO2催化加氢制低碳烯烃性能的影响

Effects of supports on catalytic performances of Fe-based catalysts for CO2 hydrogenation to light olefins

DOI：10.12434/j.issn.2097-2547.20240125

摘要

Abstract

关键词

Keywords

references

载体对Fe基催化剂CO₂催化加氢制低碳烯烃性能的影响

Effects of supports on catalytic performances of Fe-based catalysts for CO₂ hydrogenation to light olefins