二氧化碳加氢制低碳烯烃Fe基催化剂研究进展

doi:10.6023/A24120390

化学学报 ›› 2025, Vol. 83 ›› Issue (5): 535-550.DOI: 10.6023/A24120390 上一篇

综述

二氧化碳加氢制低碳烯烃Fe基催化剂研究进展

胡博^a, 肖霞^a^,^*(), 王鹏^a^,^b, 束小龙^a, 卞梦琪^a, 王健捷^a, 赵震^a^,^b^,^*()

^a 沈阳师范大学化学化工学院能源与环境催化研究所沈阳 110034
^b 中国石油大学(北京) 重质油国家重点实验室北京 102249

投稿日期:2024-12-31 发布日期:2025-04-16

作者简介:

胡博, 本科生, 就读于沈阳师范大学化学化工学院, 主要从事分子筛多孔材料合成、二氧化碳烷烃耦合转化方面的研究工作.

肖霞, 博士, 沈阳师范大学化学化工学院副教授, 硕士研究生导师, 主要从事分子筛多孔材料的合成及其能源催化方面的研究工作. 主持国家自然科学基金、辽宁省自然科学基金等各类科研项目7项, 参与科技部重点研发计划、国家自然科学基金重大重点项目、中石油重大科技专项等5项. 已在ACS Catal., Chem. Commun., Micropor. Mesopor. Mat.和中国科学: 化学等国内外学术期刊上发表论文30余篇, 参编《炼油稀土催化》、《化学: 中心科学》和《Heterogeneous Catalysis for Sustainable Energy》著作3部. 荣获辽宁省研究生教学成果奖特等奖、辽宁省高等学校本科教学成果二等奖和沈阳市自然科学学术成果奖等. 入选辽宁省“百千万人才工程”万人层次, 沈阳市中青年科技创新人才支持计划, 沈阳市拔尖人才.

赵震, 教育部国家级高层次人才; 中国石油大学(北京)教授, 博士生导师; 沈阳师范大学特聘教授、沈阳师范大学化学化工学院院长, 能源与环境催化研究所所长. 中国科协“一带一路”国际联合能源与环境催化研究中心主任; 辽宁省高校重大科技平台“能源与环境催化工程技术研究中心”主任. 现兼任中国化学会催化专业委员会委员; 中国稀土学会常务理事和催化专业委员会副主任; 中国能源学会副会长和能源与环境专业委员会主任等多个学术兼职. 入选国际先进材料协会(IAAM)Fellow、国际VEBLEO学会组织Fellow、教育部“长江学者奖励计划”特聘教授、“新世纪百千万人才”国家级人选、“国务院政府特殊津贴”专家、辽宁杰出科技工作者、辽宁省高校攀登学者、辽宁省普通高等学校本科教学名师、辽宁省教书育人模范、辽宁省学术头雁、辽宁省优秀科技工作者、辽宁省课程思政教学名师、沈阳市十大科技英才、沈阳市优秀专家、沈阳市杰出人才等荣誉称号. 主要从事能源与环境催化、稀土催化、催化新材料等方面的研发工作. 主持科技部重点研发计划项目、863主题(专题)项目课题、国家自然科学基金重大研究计划集成、重点项目、国家自然科学基金重点项目等国家级项目(课题)19项; 省市级各类项目30余项; 已在Nature Commun., PNAS, Angew. Chem. Int. Ed., Energy & Environment. Science, AICHE J., Appl. Catal. B: Environment, ACS Catal., J. Catal.和中国科学: 化学等国内外知名学术期刊上发表SCI论文600余篇, 引用23300多次, H因子81 (Scopus); 2014~2024年连续11年入选爱思唯尔公司公布的中国高被引学者榜单(化学工程与技术). 荣获国际纯粹与应用化学联合会(IUPAC)新材料及其合成杰出贡献奖、湖北省科学技术自然科学奖二等奖、中国稀土科学技术奖一等奖、中国化工学会基础研究成果一等奖、侯德榜化工科技奖创新奖、辽宁省高等学校本科教学成果一等奖、二等奖及辽宁省研究生教学成果奖特等奖等多项教学科研奖励.

基金资助:
辽宁省自然科学基金面上项目(2024-MS-110); 辽宁省教育厅基本科研项目(LJKMZ20221476); 广西重大专项项目(GUIKEAA24206022); 辽宁省国际科技合作计划项目(2024JH2/102100004); 沈阳市中青年科技创新人才支持计划项目(RC220357)

Advances in Fe-based Catalysts for the Hydrogenation of CO₂ to Light Olefins

Bo Hu^a, Xia Xiao^a^,^*(), Peng Wang^a^,^b, Xiaolong Shu^a, Mengqi Bian^a, Jianjie Wang^a, Zhen Zhao^a^,^b^,^*()

^a Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, China
^b State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China

Received:2024-12-31 Published:2025-04-16
Contact: * E-mail: xiaoxiacup@126.com; zhenzhao@cup.edu.cn
Supported by:
Liaoning Provincial Natural Science Foundation General Program(2024-MS-110); Basic Scientific Research Project of Liaoning Provincial Department of Education(LJKMZ20221476); Science and Technology Major Program of Guangxi Province(GUIKEAA24206022); Liaoning Province international science and technology cooperation program project(2024JH2/102100004); Shenyang Young and Middle-aged Scientific and Technological Innovation Talents Support Plan(RC220357)

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摘要/Abstract

二氧化碳(CO₂)作为温室效应的主要贡献者, 同时也是廉价且丰富的碳资源. 通过CO₂加氢合成低碳烯烃, 不仅能够实现CO₂的资源化利用, 还能减少低碳烯烃生产对石油资源的依赖, 具有重要的环境和经济意义. 本文综述了铁基(Fe基)催化剂催化CO₂加氢制低碳烯烃的研究进展与反应机理(CO₂-FTS路径和CO₂-甲醇路径), 详细归纳了双金属活性组分(Fe-Co、Fe-Ni、Fe-Ru等)、载体(金属氧化物、金属有机骨架化合物、碳材料、分子筛等)、助剂(碱金属、碱土金属、过渡金属及其氧化物、稀土金属、生物助剂等)以及制备方法和条件对CO₂-FTS路径中铁基催化剂活性和选择性的影响规律, 探讨了铁基催化剂在反应过程中活性位点的结构演变规律(如Fe₃O₄、Fe₅C₂等), 分析了影响催化剂性能的组成与结构因素. 重点阐述了CO₂-FTS路径中逆水煤气变换(RWGS)反应的氧化还原路径和缔合路径, 以及费托合成(FTS)反应中表面碳化物机理、表面烯醇机理和CO插入机理三种可能的作用机制. 最后对CO₂加氢制低碳烯烃铁基催化剂的研究方向进行了展望, 提出了未来可能的研究趋势与挑战, 以期为设计和合成用于CO₂加氢制取高价值化学品的高效催化剂提供科学指导.

关键词: 二氧化碳, 加氢, 低碳烯烃, Fe基催化剂, 催化活性, 选择性

Carbon dioxide (CO₂) is the primary contributor to the greenhouse effect, and its increasing concentration in the atmosphere has become a major driver of global climate change. However, CO₂ is also the most inexpensive and abundant carbon resource in nature. The hydrogenation of CO₂ to produce high-value-added chemicals such as light olefins not only enables the utilization of CO₂ as a resource but also reduces the reliance on non-renewable resources like petroleum for light olefins production. This has profound implications for global energy security and sustainable development. This article reviews the research progress and reaction mechanisms (CO₂-FTS pathway and CO₂-MeOH pathway) of iron-based catalysts for the hydrogenation of CO₂ to produce light olefins. This article comprehensively reviews recent advances in iron-based catalysts for CO₂ hydrogenation to light olefins, with particular emphasis on the CO₂-FTS and CO₂-MeOH pathways: the surface carbide mechanism, the surface enol mechanism, and the CO insertion mechanism. The active sites and structural evolution of Fe-based catalysts during the reaction process are discussed. Based on this, the main factor leading to the deactivation of Fe-based catalysts is identified as the irreversible oxidation of the active phase (Fe₅C₂) to the inactive phase (Fe₃O₄). The article emphasizes the effects of bimetallic active components (Fe-Co, Fe-Ni, Fe-Ru bimetallic catalysts), supports (oxides, metal-organic frameworks, carbon materials, zeolites), promoters (alkali and alkaline earth metals, transition metals and their oxides, rare earth metals, biological promoters), and catalyst preparation methods and conditions on the activity and selectivity of Fe-based catalysts in the CO₂-FTS pathway. The compositional and structural factors influencing the performance of Fe-based catalysts are analyzed. Additionally, representative bifunctional catalysts in both the CO₂-FTS and CO₂-MeOH pathways are introduced, with examples illustrating how bifunctional catalysts can accelerate the reaction process and reduce energy consumption. Finally, we provide an outlook on the research directions of iron-based catalysts for CO₂ hydrogenation to light olefins, proposing potential future research trends and challenges, aiming to offer references and insights for researchers in this field.

Key words: carbon dioxide, hydrogenation, light olefins, Fe-based catalysts, catalytic activity, selectivity

引用此文

胡博, 肖霞, 王鹏, 束小龙, 卞梦琪, 王健捷, 赵震. 二氧化碳加氢制低碳烯烃Fe基催化剂研究进展[J]. 化学学报, 2025, 83(5): 535-550.

Bo Hu, Xia Xiao, Peng Wang, Xiaolong Shu, Mengqi Bian, Jianjie Wang, Zhen Zhao. Advances in Fe-based Catalysts for the Hydrogenation of CO₂ to Light Olefins[J]. Acta Chimica Sinica, 2025, 83(5): 535-550.

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图/表 18

Entry	Catalysts	CO₂ Conversion/%	CO Selectivity/%	Hydrocarbon distribution^a/%				GHSV/ (mL•g^-1•h^-1)	Temperature./℃	Pressure/ MPa	Ref.
Entry	Catalysts	CO₂ Conversion/%	CO Selectivity/%	CH₄	C₂⁰~C₄⁰	C₂⁼~C₄⁼	C₅⁺	GHSV/ (mL•g^-1•h^-1)	Temperature./℃	Pressure/ MPa	Ref.
1	Co-Fe	31.4	—	20.4		57.3	22.3	9600	320	1	[12]
2	Na/Fe@CoCo-3	50.3	4.6	13.9	41.3		44.8	—	330	3	[13]
3	Fe-Co(0.17)/K(1.0)	31.0	18.0	15.9	84.1			3600	300	1.1	[14]
4	Ni/Fe=1:99	32.6	89.1	57.0	7.4	35.6	0	5000	350	—	[15]
5	CM-Al₂O₃	41.0	12.4	33.7	6.4	41.1	18.7	—	320	2	[20]
6	Fe/CeO₂ rods	20.6	61.2	80.6	6.2	12.3	0.6	1600	390	—	[21]
7	Fe(12.9)	12.8	49.5	67.7	28.5	1.4	2.4	18000	320	3	[22]
8	Fe/ZrO₂	42	15	20.0	8.2	46.0	26.8	1200	340	2	[23]
9	N-600-0	46	17.5	32.2	17.6	23.3	26.9	3600	400	3	[26]
10	Fe/C-K@NC-350/500	35.1	28.1	23.8	7.9	37.7	30.6	5000	340	3	[28]
11	40FeK/SMC	44.7	85.5	4.8	6.5	13.6	75.1	—	260	2	[34]
12	Fe-K/HPCMs1	33.4	38.9	22.1	18.8	29.5	29.6	3600	400	3	[35]
13	IO@gC-1.0	21.9	78.3	50.5	46.3		3.2	—	370	—	[36]
14	FeNa/EG-A	42.4	8.3	12.6	7.8	38.0	41.6	2000	320	3	[37]
15	Fe-Cu-K/ZSM-5(Si/Al=25)	37.7	80.7	18.3	24.9		56.8	2000	300	1	[41]
16	Mn15Na32im	31.9	97.2	12.4	6.2	33.0	48.4	11000	320	1.5	[47]
17	IWI200	22.4	17.8	46.3	33.0	7.8	12.9	36000	300	—	[49]
18	3% (w) Rb/Fe₃O₄	39.7	8.1	19.5	4.4	47.4	28.7	2500	300	0.5	[50]
19	FeMnZr4K	39.0	81.5	15.4	4.7	28.4	51.5	12000	320	1	[51]
20	1Fe-1Zn-K	51.0	6.0	34.9	7.8	53.6	3.7	1000	300	0.5	[55]
21	5Mn-Na/Fe	38.6	11.7	13.5	4.6	34.6	47.2	2040	320	3	[57]
22	0.14Mn/Fe₃O₄-NaAc	27.0	26.8	14.4	6.4	40.3	38.9	—	320	0.5	[58]
23	FeMnNd	49.3	74.9	20.2	9.1	36.0	34.3	4000	300	1	[62]
24	20Fe0.5Cu0.5Nd/MOR	23.3	28.3	34.9	27.1	25.4	12.6	—	350	1	[63]
25	35Fe-7Zr-1Ce-K	57.34	3.05	20.64	7.86	55.62	15.87	1000	320	2	[64]
26	Fe@C-1.0	52.3	92.6	8.5	4.2	26.0	61.3	3000	300	2	[67]

Entry	Catalysts	CO₂ Conversion/%	CO Selectivity/%	Hydrocarbon distribution^a/%				GHSV/ (mL•g^-1•h^-1)	Temperature./℃	Pressure/ MPa	Ref.
Entry	Catalysts	CO₂ Conversion/%	CO Selectivity/%	CH₄	C₂⁰~C₄⁰	C₂⁼~C₄⁼	C₅⁺	GHSV/ (mL•g^-1•h^-1)	Temperature./℃	Pressure/ MPa	Ref.
1	Co-Fe	31.4	—	20.4		57.3	22.3	9600	320	1	[12]
2	Na/Fe@CoCo-3	50.3	4.6	13.9	41.3		44.8	—	330	3	[13]
3	Fe-Co(0.17)/K(1.0)	31.0	18.0	15.9	84.1			3600	300	1.1	[14]
4	Ni/Fe=1:99	32.6	89.1	57.0	7.4	35.6	0	5000	350	—	[15]
5	CM-Al₂O₃	41.0	12.4	33.7	6.4	41.1	18.7	—	320	2	[20]
6	Fe/CeO₂ rods	20.6	61.2	80.6	6.2	12.3	0.6	1600	390	—	[21]
7	Fe(12.9)	12.8	49.5	67.7	28.5	1.4	2.4	18000	320	3	[22]
8	Fe/ZrO₂	42	15	20.0	8.2	46.0	26.8	1200	340	2	[23]
9	N-600-0	46	17.5	32.2	17.6	23.3	26.9	3600	400	3	[26]
10	Fe/C-K@NC-350/500	35.1	28.1	23.8	7.9	37.7	30.6	5000	340	3	[28]
11	40FeK/SMC	44.7	85.5	4.8	6.5	13.6	75.1	—	260	2	[34]
12	Fe-K/HPCMs1	33.4	38.9	22.1	18.8	29.5	29.6	3600	400	3	[35]
13	IO@gC-1.0	21.9	78.3	50.5	46.3		3.2	—	370	—	[36]
14	FeNa/EG-A	42.4	8.3	12.6	7.8	38.0	41.6	2000	320	3	[37]
15	Fe-Cu-K/ZSM-5(Si/Al=25)	37.7	80.7	18.3	24.9		56.8	2000	300	1	[41]
16	Mn15Na32im	31.9	97.2	12.4	6.2	33.0	48.4	11000	320	1.5	[47]
17	IWI200	22.4	17.8	46.3	33.0	7.8	12.9	36000	300	—	[49]
18	3% (w) Rb/Fe₃O₄	39.7	8.1	19.5	4.4	47.4	28.7	2500	300	0.5	[50]
19	FeMnZr4K	39.0	81.5	15.4	4.7	28.4	51.5	12000	320	1	[51]
20	1Fe-1Zn-K	51.0	6.0	34.9	7.8	53.6	3.7	1000	300	0.5	[55]
21	5Mn-Na/Fe	38.6	11.7	13.5	4.6	34.6	47.2	2040	320	3	[57]
22	0.14Mn/Fe₃O₄-NaAc	27.0	26.8	14.4	6.4	40.3	38.9	—	320	0.5	[58]
23	FeMnNd	49.3	74.9	20.2	9.1	36.0	34.3	4000	300	1	[62]
24	20Fe0.5Cu0.5Nd/MOR	23.3	28.3	34.9	27.1	25.4	12.6	—	350	1	[63]
25	35Fe-7Zr-1Ce-K	57.34	3.05	20.64	7.86	55.62	15.87	1000	320	2	[64]
26	Fe@C-1.0	52.3	92.6	8.5	4.2	26.0	61.3	3000	300	2	[67]

表1. 二氧化碳加氢生成C2+产物的代表性催化剂及其催化性能结果

Table 1. Representative catalysts and their catalytic performance for hydrogenation of CO2 to C2+ species.

表1. 二氧化碳加氢生成C2+产物的代表性催化剂及其催化性能结果

Table 1. Representative catalysts and their catalytic performance for hydrogenation of CO2 to C2+ species.

图1. S-Al2O3、M-Al2O3和L-Al2O3三种不同孔径载体催化剂的催化性能比较[20]

Figure 1. Comparison of catalytic performance of three different pore size carrier catalysts of S-Al2O3, M-Al2O3 and L-Al2O3[20]

图2. 催化剂的粒径效应[22]

Figure 2. Particle size effect of catalysts[22]

图3. 反应过程示意图[27]

Figure 3. Proposed schematic of the reaction[27]

图4. Fe/C+K(0.75)催化剂上的碳氢化合物分布图和ASF图[29]

Figure 4. Hydrocarbon distribution and ASF plots over Fe/C+K(0.75) catalysts[29]

图5. 二氧化碳加氢反应中IO@gC-0.5、IO@gC-1、IO@gC-1.5、IO@gC-2.0、IO-μ及IO-μ@gC-1.0催化剂的催化活性对比: 时空产率FTY与烯烷比O/P分析[36](反应条件: n(H2)∶n(CO2)=2∶1, 总流量为6 mL•min-1, 反应温度为370 ℃, 反应时间为12 h)

Figure 5. Catalytic activity of IO@gC-0.5, IO@gC-1, IO@gC-1.5, IO@gC-2.0, IO-µ and IO-µ@gC-1.0 in hydrogenation of CO2 showing FTY and O/P ratio[36]. Reaction conditions: n(H2)∶n(CO2)=2∶1, with 6 mL•min-1 total flow rate at 370 ℃ at atmospheric pressure for 12 h

图6. (a) N2物理吸附等温线和孔径分布, (b)扫描电子显微镜(SEM)图像, (c)高角度环形暗场扫描透射电子显微镜(HAADF-STEM)图像, (d)透射电子显微镜(TEM)图像和制备的FeK1.5/HSG催化剂的颗粒分布图, (d)插图显示了催化剂上纳米粒子的晶格条纹[38]

Figure 6. (a) N2 physisorption isotherms and pore size distribution, (b) SEM image, (c) HAADF-STEM image, and (d) TEM image and particle distribution histogram of the as-prepared FeK1.5/HSG catalyst. Inset in (d) shows the lattice fringes of the nanoparticle on the catalyst[38]

图7. Fe2O3@KO2/沸石双功能材料在CO2加氢过程中的催化性能[40]. (a)使用不同沸石的催化性能结果对比; (b)详细对比了与单独的Fe/K催化剂相比, 引入沸石分子筛后净选择性增加(或减少). 反应条件: 3 MPa、375 ℃、n(H2)∶n(CO2)=3∶1、10000 mL•g-1•h-1, 反应时间为48 h)

Figure 7. Catalytic performance of the Fe2O3@KO2/zeolite bifunctional material catalyzed hydrogenation of CO2 process[40]. (a) Comparison of catalytic data using different zeolites; (b) Detailed illustration of the (net) selectivity increase (or decrease) of individual hydrocarbon groups upon introducing zeolites with respect to the standalone Fe/K catalyst. Reaction condition: 3 MPa, 375 ℃, n(H2)∶n(CO2)=3∶1, and 10,000 mL•g-1•h-1 at a time on stream of 48 h

图8. xNa/Fe催化剂对CO2加氢的催化性能[48]

Figure 8. Catalytic performance of xNa/Fe catalysts for CO2 hydrogenation[48]

图9. Na和Mn助剂在CO2加氢生产低碳烯烃过程中的作用[58]

Figure 9. Role of Na and Mn additives in the production of low carbon olefins by CO2 hydrogenation[58]

图10. α-Fe2O3与γ-Fe2O3催化剂在CO2加氢活化及反应过程中结构-性能关系的示意图[83]

Figure 10. Scheme of structure-performance relationship of α-Fe2O3 and γ-Fe2O3 catalysts for CO2 hydrogenation during activation and reaction processes[83]

图11. 二氧化碳加氢性能对比[84]. (A)不同催化剂的CO2转化率和C2+生成速率(反应条件: p=3 MPa, T=320 ℃, n(CO2)∶n(H2)=1∶3, TOS=20 min, 气体小时空速(GHSV)=72,000 mL•h-1•gcat-1); (B)不同反应时间(TOS)的模型催化剂(虚线左侧)与真实Fe(0)催化剂(虚线右侧)的产物选择性与CO2转化率对比(GHSV=18,000 mL•h-1•gcat-1, *GHSV=72,000 mL•h-1•gcat-1)

Figure 11. Comparison of CO2 hydrogenation performance[84]. (A) CO2 conversion rate and C2+ formation rate over different model catalysts. Reaction conditions: p=3 MPa, T=320 ℃, n(CO2)∶n(H2)=1∶3, TOS=20 min, and GHSV=72,000 mL•h-1•gcat-1; (B) Product selectivity and CO2 conversion over model catalysts (on the left of the dashed line) and real Fe(0) catalysts with different TOS (on the right); GHSV=18,000 mL•h-1•gcat-1. *GHSV=72,000 mL•h-1•gcat-1

图12. RWGS的氧化还原机理(上)和缔合机理(下)反应途径

Figure 12. Redox (top) and associative (bottom) reaction pathways for the RWGS reaction

图13. RWGS的反应机理[94]

Figure 13. RWGS reaction mechanism[94]

图14. 表面碳化物机理示意图[95]

Figure 14. Representation of the surface carbide mechanism[95]

图15. 表面烯醇机理示意图[95]

Figure 15. Representation of the surface enol mechanism[95]

图16. CO插入机制示意图[95]

Figure 16. Representation of the CO insertion mechanism[95]

图17. CO2通过CO2-MeOH转化为燃料和化学品[97]. (a)双功能催化剂上CO2加氢转化为C2+产物的反应机制示意图; (b)甲醇合成的两种可能反应途径; (c)通过碳氢化合物烃池机制在沸石内部将CH3OH转化为碳氢化合物的示意图

Figure 17. CO2 hydrogenation to fuels and chemicals via the methanol reaction mechanism[97]. (a) Schematic for the reaction mechanism of direct CO2 hydrogenation to C2+ products over bifunctional catalysts; (b) Two possible reaction pathways for methanol synthesis; (c) Schematic for methanol conversion into hydrocarbons inside zeolites via the hydrocarbon-pool mechanism

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二氧化碳加氢制低碳烯烃Fe基催化剂研究进展

Advances in Fe-based Catalysts for the Hydrogenation of CO₂ to Light Olefins

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二氧化碳加氢制低碳烯烃Fe基催化剂研究进展

Advances in Fe-based Catalysts for the Hydrogenation of CO2 to Light Olefins

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Advances in Fe-based Catalysts for the Hydrogenation of CO₂ to Light Olefins