表面改性Fe/CS调控CO加氢产物分布研究

张庆旭; 王康洲; 李财虎; 高新华; 赵天生; 张建利

doi:10.12434/j.issn.2097-2547.20240160

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表面改性Fe/CS调控CO加氢产物分布研究

合成气化工与催化转化

- 表面改性Fe/CS调控CO加氢产物分布研究
- Study on distribution of CO hydrogenation products regulated by surface-modified Fe/CS
- 低碳化学与化工 2024, 49(8): 18-27.
- 作者机构：
  
  1.宁夏大学化学与化工学院,省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏银川 750021
  2.宁夏大学材料与新能源学院,宁夏银川 750021
  3.宁夏计量质量检验检测研究院国家煤化工产业计量测试中心,宁夏银川 750411
- 作者简介：
  
  张庆旭（2000—），硕士研究生，研究方向为CO加氢定向转化，E-mail：1208212575@qq.com。
  王康洲（1992—），博士，副教授，研究方向为低碳资源催化转化，E-mail：kangzhou_wang@163.com；
  张建利（1980—），博士，研究员，研究方向为碳一化学，E-mail：zhangjl@nxu.edu.cn。
- 基金信息：
  
  国家自然科学基金(22368041);中央引导地方科技发展专项(2023FRD05030)
- DOI：10.12434/j.issn.2097-2547.20240160
  中图分类号： TQ426
- 纸质出版日期：2024-08-25，
  
  收稿日期：2024-04-16，
  
  修回日期：2024-05-22，
- 稿件说明：
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张庆旭,王康洲,李财虎等.表面改性Fe/CS调控CO加氢产物分布研究[J].低碳化学与化工,2024,49(08):18-27.

ZHANG Qingxu,WANG Kangzhou,LI Caihu,et al.Study on distribution of CO hydrogenation products regulated by surface-modified Fe/CS[J].Low-carbon Chemistry and Chemical Engineering,2024,49(08):18-27.
张庆旭,王康洲,李财虎等.表面改性Fe/CS调控CO加氢产物分布研究[J].低碳化学与化工,2024,49(08):18-27. DOI： 10.12434/j.issn.2097-2547.20240160.

ZHANG Qingxu,WANG Kangzhou,LI Caihu,et al.Study on distribution of CO hydrogenation products regulated by surface-modified Fe/CS[J].Low-carbon Chemistry and Chemical Engineering,2024,49(08):18-27. DOI： 10.12434/j.issn.2097-2547.20240160.

摘要

CO加氢经费托合成制取高附加值化学品是实现煤炭清洁高效利用的重要途径之一，研发高效催化剂是实现产物分布定向调控、提高目标产物选择性并抑制C1副产物生成的关键。催化剂表面性质对CO的吸附活化、加氢活性和产物分布具有重要影响。以无水葡萄糖为碳源、乙二醇为溶剂，采用溶剂热法制得碳载体，经H

、NH

•H

O表面改性和掺氮处理后，采用浸渍法分别制备了5Fe/CS-H

、5Fe/CS-NH

•H

O和5Fe/CS-N催化剂，探究了表面改性对费托合成产物分布的影响。采用XRD、SEM、TEM、N

吸/脱附、TG-DTG、FT-IR、Zeta电位、XPS和拉曼光谱等对样品进行了表征。结果表明，不同表面改性方式对催化剂表面物化性质和催化性能影响显著。H

改性增加了催化剂表面—OH的数量，增强了表面亲水性，促进了Fe在载体上的分散，催化剂的热稳定性提高。在300 ℃、1.5 MPa、空速为1000 h

-1

和

(CO) = 2的条件下进行CO加氢反应活性测试结果表明，改性后的催化剂显著抑制了CH

的生成，提高了低碳烯烃选择性，从5Fe/CS的24.39%分别提高到5Fe/CS-NH

•H

O的34.94%、5Fe/CS-N的37.63%以及5Fe/CS-H

的43.57%。通过表面改性和掺氮处理调控催化剂表面性质实现了对产物分布的优化。

Abstract

The preparation of high value-added chemicals via CO hydrogenation with Fischer-Tropsch synthesis is one of the important ways to achieve clean and efficient utilization of coal. The development of efficient catalysts is the key to achieve targeted regulation of product distributions

improve the selectivity of target products and inhibit the formation of C1 by-products. The surface properties of catalysts have a significant impact on the adsorption and activation of CO

hydrogenation activation and product distributions. Anhydrous glucose was used as the carbon source and

ethylene glycol was used as the solvent to prepare the carbon support by solvothermal method. After H

and NH

•H

O surface modification and nitrogen doping

5Fe/CS-H

5Fe/CS-NH

•H

O and 5Fe/CS-N catalysts were prepared by impregnation method

respectively. The effect of surface modification on the product distributions of Fischer-Tropsch synthesis was investigated. The samples were characterized by XRD

SEM

TEM

adsorption/desorption

TG-DTG

FT-IR

Zeta potential

XPS and Raman. The results show that different surface modification methods have a significant impact on the surface physicochemical properties and catalytic performances of catalysts. The modification of H

increases the amount of —OH on catalyst surface

enhances the hydrophilicity of catalyst surface

promotes the dispersion of Fe on the support

and improves the thermal stability of catalysts. The activity test of CO hydrogenation reaction was conducted under the conditions of 300 ℃

1.5 MPa

space velocity 1000 h

-1

and

(CO) = 2. The results show that the modified catalysts significantly inhibit the generation of CH

and improve the selectivity of light olefins. The olefin selectivities of 5Fe/CS-NH

•H

5Fe/CS-N and 5Fe/CS-H

increase from 24.39% to 34.94%

37.63% and 43.57%

respectively. The surface properties of the catalyst are adjusted by surface modification and nitrogen-doping treatment

and the product distribution is optimized.

关键词

CO加氢Fe/CS催化剂表面改性低碳烯烃

Keywords

CO hydrogenationFe/CS catalystssurface modificationlight olefins

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