Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO<sub>2</sub> to high carbon hydrocarbons with ZSM-5

ZHAO Zhihua; XU Chenghua; REN Hong; LUO Jing; DU Lei; LIU Chenlong; CHEN Wenjing; LUO Jing

doi:10.12434/j.issn.2097-2547.20230234

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Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO₂ to high carbon hydrocarbons with ZSM-5

- Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO₂ to high carbon hydrocarbons with ZSM-5
- Vol. 49, Issue 2, Pages: 10-16(2024)
- 作者机构：
  
  成都信息工程大学资源环境学院大气环境模拟与污染控制四川省高校重点实验室，四川成都 610225
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20230234
  CLC： TQ426;X51
- Published：25 February 2024，
  
  Received：30 June 2023，
  
  Revised：25 July 2023，
- 稿件说明：
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赵治华,徐成华,任红等.造孔剂诱导合成FeCoCuAl催化剂及其与ZSM-5复合催化CO₂加氢制高碳烃性能[J].低碳化学与化工,2024,49(02):10-16.

ZHAO Zhihua,XU Chenghua,REN Hong,et al.Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO₂ to high carbon hydrocarbons with ZSM-5[J].Low-carbon Chemistry and Chemical Engineering,2024,49(02):10-16.
赵治华,徐成华,任红等.造孔剂诱导合成FeCoCuAl催化剂及其与ZSM-5复合催化CO₂加氢制高碳烃性能[J].低碳化学与化工,2024,49(02):10-16. DOI： 10.12434/j.issn.2097-2547.20230234.

ZHAO Zhihua,XU Chenghua,REN Hong,et al.Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO₂ to high carbon hydrocarbons with ZSM-5[J].Low-carbon Chemistry and Chemical Engineering,2024,49(02):10-16. DOI： 10.12434/j.issn.2097-2547.20230234.

摘要

加氢制高碳烃（C

）是合成高值化学品和燃料的重要途径之一，这既可以实现碳减排，又有助于缓解能源压力。采用沉淀法和等体积浸渍法制备了K、Na修饰的FeCoCuAl催化剂，考察了造孔剂1

5-苯三甲酸（BTA）对其在CO

催化加氢制高碳烃反应（温度为300 ℃、压力为2.0 MPa、原料气

(CO

) = 3:1且空速为3600 h

-1

、时间为6 h）中催化性能的影响。在FeCoCuAl-20.0BTA催化剂（

(BTA):

(Fe) = 20.0%）中引入ZSM-5分子筛，构建了一系列复合催化剂，并研究了其在CO

催化加氢制高碳烃反应中的催化性能。结合N

吸/脱附、X射线衍射（XRD）、H

-程序升温还原（H

-TPR）、CO

程序升温脱附（CO

-TPD）和H

升温脱附（CO

-TPD）等对催化剂的理化性质进行了表征，采用GC-MS对产物油相成分进行了分析。结果表明，与FeCoCuAl催化剂相比，FeCoCuAl-BTA催化剂的比表面积、孔容等均增大，并生成了更多的表面活性物种（Fe或Fe-Co合金），从而使得FeCoCuAl-BTA催化剂在CO

催化加氢反应中表现出更好的催化性能。FeCoCuAl-20.0BTA催化剂的CO

转化率和C

选择性分别可达70%和42%。FeCoCuAl-20.0BTA催化剂催化CO

加氢生成的产物以C

产物为主，而在FeCoCuAl-20.0BTA催化剂与ZSM-5分子筛以质量比为1.0、颗粒机械混合方式构建的复合催化剂上，FeCoCuAl-20.0BTA上生成的C

产物可在ZSM-5分子筛上发生原位链增长、异构化和芳构化反应，从而提高了CO

转化率和C

选择性，分别达到79%和66%。

Abstract

hydrogenation to high-carbon hydrocarbons (C

) is one of the important ways to synthesize high-value chemicals and fuels

which can achieve carbon emission reduction as well as help to alleviate energy pressure. K- and Na-modified FeCoCuAl catalysts were prepared by precipitation and iso-volumetric impregnation methods

and the effects of the pore-forming agent 1

5-benzenetricarboxylic acid (BTA) on their catalytic performance in CO

-catalyzed hydrogenation to high-carbon hydrocarbons reaction(temperature of 300 ℃

pressure of 2.0 MPa

(CO

) = 3:1 and space velocity of 3600 h

-1

of feed gas

reaction for 6 h) were investigated. ZSM-

5 molecular sieve was introduced into FeCoCuAl-20.0BTA catalyst (

(BTA):

(Fe) = 20.0%) to construct a series of composite catalysts and their catalytic performance in the reaction of catalytic hydrogenation of CO

to high-carbon hydrocarbons was investigated. The physicochemical properties of the catalysts were characterized by combining N

adsorption/desorption

X ray diffraction (XRD)

-temperature programmed reduction (H

-TPR)

temperature programmed desorption (CO

-TPD)

and H

temperature programmed desorption (CO

-TPD)

and the oil-phase compositions of the products were analyzed by GC-MS. The results show that compared with FeCoCuAl catalysts

the specific surface area and pore volume of FeCoCuAl-BTA catalysts increase

and generate more surface-active species (Fe or Fe-Co alloy)

which lead to better catalytic performance of FeCoCuAl-BTA catalysts in CO

catalytic hydrogenation reaction. The CO

conversion rate and C

selectivity of FeCoCuAl-20.0BTA catalyst are up to 70% and 42%

respectively

and the products generated from CO

hydrogenation catalyzed by FeCoCuAl-20.0BTA catalyst are mainly C

products

while on the composite catalyst constructed with FeCoCuAl-20.0BTA catalyst and ZSM-5 molecular sieve in the form of mechanical mixing of particles with the mass ratio of 1.0

the C

products generated on FeCoCuAl-20.0BTA can undergo in situ chain growth

isomerization and aromatization reactions on ZSM-5 molecular sieves

which lead to the improvement of CO

conversion rate and C

selectivity

reaching 79% and 66%

respectively.

关键词

造孔剂FeCoCuAl催化剂ZSM-5CO2加氢高碳烃

Keywords

pore-forming agentFeCoCuAl catalystsZSM-5CO2 hydrogenationhigh-carbon hydrocarbons

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Large Industrial Reactor Engineering Research Center of the Ministry of Education, School of Chemical Engineering, East China University of Science and Technology

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School of Chemistry and Chemical Engineering, Anhui University

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Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO2 to high carbon hydrocarbons with ZSM-5

DOI：10.12434/j.issn.2097-2547.20230234

摘要

Abstract

关键词

Keywords

references

Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO₂ to high carbon hydrocarbons with ZSM-5