合成气/CO2转化制高级醇Fe基催化剂研究进展

doi:10.16085/j.issn.1000-6613.2024-0472

摘要/Abstract

摘要：

合成高级醇是将煤、天然气、生物质、CO/CO₂等非石油资源转化为液体燃料和高附加值化学品的重要途径之一，对推动煤炭清洁高效利用、CO₂资源化利用具有重要意义。近年来，通过改性费托合成催化剂来合成高级醇的研究取得了重要进展，催化剂性能明显提升。因材料廉价易获取且反应机理可借鉴费托合成，Fe基催化剂成为研究热点，但基础理论研究仍待完善。本文概述了近期高级醇合成Fe基催化剂最新的研究进展，重点综述了Fe基催化剂、FeCu基催化剂在合成高级醇反应中活性位点的性质和反应机理。梳理了碱金属、过渡金属、非金属改性对催化剂构效关系的影响，及其对提高催化剂催化活性、高级醇选择性、稳定性的作用。对比了SiO₂、Al₂O₃等常用载体的作用。按浸渍法、特殊结构、复合材料等分别对Fe基催化剂制备方法进行了系统性剖析。

关键词: 醇, 催化剂, 吸附, 活性, 选择性, 载体

Abstract:

The synthesis of higher alcohols is a significant approach for converting non-petroleum resources like coal, natural gas, biomass, CO/CO₂, and others into liquid fuels and high-valued chemicals, which holds great importance in promoting the clean and efficient utilization of coal and CO₂. In recent years, there have been remarkable achievements in the research of modified Fischer-Tropsch synthesis catalysts for higher alcohol synthesis, giving significant enhancements in catalytic performance and selectivity for higher alcohols. Fe-based catalysts have emerged as a research focus in recent years due to their low cost and easy access, and their reaction mechanisms can be drawn upon that of Fischer-Tropsch synthesis. However, basic theoretical research still requires to be strengthened. This article presents an overview of the latest research progress on Fe-based catalysts, with a particular emphasis on the properties and reaction mechanisms of active sites in the synthesis of higher alcohols using Fe-based and FeCu-based catalysts. This article reviews the impact of alkali metals, transition metal additives, and non-metallic doping on the structure-activity relationship of catalysts, as well as on enhancing the catalytic activity, higher alcohol selectivity, and catalyst stability. Comparisons were made for commonly used carriers such as SiO₂ and Al₂O₃. A systematic analysis of the preparation methods of Fe-based catalysts is presented in terms of the impregnation method, special structure design, and material composite.

Key words: alcohol, catalyst, adsorption, reactivity, selectivity, support

中图分类号:

TQ519

张琪, 王涛, 张雪冰, 李为真, 程萌, 张魁, 吕毅军, 门卓武. 合成气/CO₂转化制高级醇Fe基催化剂研究进展[J]. 化工进展, 2025, 44(3): 1323-1337.

ZHANG Qi, WANG Tao, ZHANG Xuebing, LI Weizhen, CHENG Meng, ZHANG Kui, LYU Yijun, MEN Zhuowu. Advances in Fe-based catalysts for conversion of syngas/CO₂ to higher alcohols[J]. Chemical Industry and Engineering Progress, 2025, 44(3): 1323-1337.

图/表 12

图1 CO插入机制[16-17]

图2 推测CO2的HAS途径[21]*—吸附物种

图3 不同Co/Fe（摩尔比）催化剂示意图[26]

图4 Na-Fe@C/K-CuZnAl多功能催化剂HAS反应途径[32]

图5 Na改性的ε′-(Co x Fe1-x )2.2C催化剂[55]

图6 Janus结构Au-Fe2.2C催化剂[66]

图7 CuFe(Cr(x)-CuFe)催化剂与文献对比[68]

表1 不同载体的CuFe催化剂活性和醇分布（质量分数）[77]

催化剂	CO转化率/%	选择性/%			醇分布/%
催化剂	CO转化率/%	CO₂	HC	ROH	甲醇	C_2-5醇	C₆₊醇
CuFe	92.8	29.6	55.2	15.2	27.9	57.1	15.0
CuFe/SiO₂	84.8	22.0	58.2	19.8	26.2	57.4	16.4
CuFe/Al₂O₃	80.4	25.4	58.3	16.3	25.0	61.4	13.6
CuFe/CeO₂	85.8	28.6	56.1	15.3	33.5	54.7	11.8

图8 Cu x Fe y Mg4-LDHs催化剂形貌[65,87]

图9 K-Fe/NC催化剂结构演化[89]

图10 CZA/K-CMZF多功能催化剂上HAS反应途径[90]

图11 制备周期性大孔结构的三种3DOM-胶体晶体模板法[30,95]

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合成气/CO₂转化制高级醇Fe基催化剂研究进展

Advances in Fe-based catalysts for conversion of syngas/CO₂ to higher alcohols

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