甲烷的脱氢芳构化及其与丙烷共芳构化: 反应机理、催化剂设计、积碳和过程强化

doi:10.1016/S1872-2067(26)65006-1

催化学报 ›› 2026, Vol. 84: 25-60.DOI: 10.1016/S1872-2067(26)65006-1

甲烷的脱氢芳构化及其与丙烷共芳构化: 反应机理、催化剂设计、积碳和过程强化

顾宇^a(), 张淑嘉^a, 徐铭潞^a, 闫昊^b, 周铭昊^a, 王磊^a(), 施慧^a

^a 扬州大学化学化工学院, 江苏扬州 225009
^b 中国石油大学(华东)化学化工学院, 山东青岛 266580

收稿日期:2025-09-24 接受日期:2025-11-16 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: guyu@yzu.edu.cn (顾宇),
leiwang88@yzu.edu.cn (王磊).
基金资助:
国家自然科学基金(22308301);国家自然科学基金(22072128);国家自然科学基金(22301267)

Dehydroaromatization of methane and methane co-aromatization process with propane: Reaction mechanism, catalyst design, carbon deposition and process optimization

Yu Gu^a(), Shujia Zhang^a, Minglu Xu^a, Hao Yan^b, Minghao Zhou^a, Lei Wang^a(), Hui Shi^a

^a School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225009, Jiangsu, China
^b College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, Shandong, China

Received:2025-09-24 Accepted:2025-11-16 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: guyu@yzu.edu.cn (Y. Gu),
leiwang88@yzu.edu.cn (L. Wang).
About author:Yu Gu (College of Chemistry and Chemical Engineering, Yangzhou University) Yu Gu received his B.S. in Applied Chemistry from China University of Petroleum (East China) in 2015, and Ph. D. in Chemical Engineering & Technology from China University of Petroleum (East China) in 2021. He is currently an associated professor at Yangzhou University, Jiangsu province, China. He focuses on the catalytic conversion of light alkanes such as methane dehydroaromatization, its co-aromatization with propane/butane, propane dehydrogenation & aromatization, etc.; and catalytic upgrading of polyolefin plastics. His research approach combines synthesis, characterizations and mechanism investigation over metal catalysts supported on zeolites, alumina, silica and ceria, etc.
Lei Wang (College of Chemistry and Chemical Engineering, Yangzhou University) Lei Wang received his Ph.D. degree under Prof. Hai-Wei Liang at the University of Science and Technology of China in 2020. Then, he joined the Southern University of Science and Technology as a postdoctoral fellow. Now, he is an Associate Professor at Yangzhou University. His main research interests include the precise synthesis of nanocrystals and the interface of heterogeneous catalysts for catalyzing hydrogenation/dehydrogenation reactions.
Supported by:
National Natural Science Foundation of China(22308301);National Natural Science Foundation of China(22072128);National Natural Science Foundation of China(22301267)

摘要/Abstract

摘要：

作为一种化石能源, 天然气单位热量高、环境污染小、价格相对低廉, 被广泛认为是替代石油的理想选择. 天然气的主要成分为甲烷(其余含少量乙烷、丙烷等高碳数烷烃、氮气及硫化氢等杂质), 是地球上最丰富的烃类资源之一, 地壳储量相当可观. 甲烷作为燃料直接燃烧虽然方便了人们的日常生产生活, 但并没有充分发挥其潜在的化学价值, 附加值相对较低. 如何低成本、高效率地将甲烷催化转化为更具价值的化学品, 成为了科研领域和工业界共同关注的焦点. 甲烷经过脱氢及芳构化反应可转化为苯、甲苯、二甲苯及萘等芳烃, 既能高效利用天然气资源, 也是对传统石油和煤制芳烃路线的有力补充, 在“碳达峰、碳中和”的大背景下具有较大的研究及现实意义.

本文系统总结了甲烷的脱氢芳构化反应, 以及甲烷与以丙烷为代表的高碳烷烃的共芳构化反应的研究进展. 首先从甲烷脱氢芳构化反应入手, 围绕该过程的(1)反应热力学、(2)反应中间体及机理(乙烯、乙烷、乙炔、烃池等)、(3)催化剂脱氢金属组分的选择依据及典型的金属组分(钼、铁)、(4)反应诱导期及脱氢位点的演变、(5)催化剂载体的选择及酸位点的功能、(6)积碳的性质及形成原因、(7)催化剂设计思路(介孔结构、中空结构的构建, 晶粒尺寸、酸位点调节等)及(8)过程强化(共进料、加压、膜反应器、化学循环、反应路径改变、反应器设计及催化剂再生循环等)以提升催化剂抗积碳能力等多个方面进行了阐述, 为读者全面理解该反应提供参考. 以此为基础, 本文还探讨了甲烷与丙烷等高级烃的共芳构化反应, 围绕丙烷芳构化及甲烷-丙烷共芳构化过程的(1)反应热力学、(2)典型催化剂脱氢组分(锌、镓)、(3)反应机理等方面进行了较为系统的介绍, 并全面对比了甲烷单独芳构化、丙烷单独芳构化及共芳构化三个不同过程的异同点, 旨在拓展读者对甲烷芳构化反应的认知边界, 进而为深入理解类似实际天然气组成的原料芳构化过程提供思路. 最后, 本文总结了甲烷芳构化技术的研究现状, 并对未来的研究方向进行展望.

基于以上的总结, 本文认为今后该领域的研究者应重点关注反应条件优化、过程强化、反应路径创新、催化剂理性设计、反应路径机理研究等方面. 希望本文能够为读者系统而全面地理解甲烷脱氢芳构化及其与高碳烃的共芳构化过程提供一些借鉴, 也为致力于推动天然气制烯烃、芳烃技术产业化的潜在从业者们提供一些现实的思路.

关键词: 甲烷脱氢芳构化, 甲烷-丙烷共芳构化, 催化剂设计, 反应机理, 积碳, 过程强化

Abstract:

Natural gas, as a fossil energy source, possesses abundant reserves in nature. It is cleaner and more environmentally benign compared to coal and crude oil. Converting natural gas via catalytic routes into more valuable chemicals, such as benzene and methanol, can both reduce the transportation costs of natural gas and increase the supply of commodity chemicals. It also serves as a significant supplement to the current petrochemical industry, holding broad application prospects. The aromatization reaction of methane is a critical technique in the methane conversion pathway, in which aromatics like benzene, toluene, and naphthalene can be produced via high-temperature dehydrogenation. Such a process has drawn significant research attention over the past three decades. This paper attempts to provide a detailed introduction to the development of research on this reaction. By examining various aspects including reaction thermodynamics, catalyst composition, reaction intermediates/mechanism, coke properties, anti-coking measures and process intensification, it aims to offer readers a comprehensive understanding of this reaction. Additionally, by discussing the co-aromatization of methane with higher hydrocarbons like propane, it tries to expand the cognitive boundaries related to methane aromatization reactions, thereby tending to offer deeper insights into the aromatization process of feedstock with compositions similar to real natural gas. In the end, the current research status in the field of methane aromatization is summarized, and future research directions are outlined as well.

Key words: Methane dehydroaromatization, Methane propane co-aromatization, Catalyst design, Reaction mechanism, Coke, Process optimization

顾宇, 张淑嘉, 徐铭潞, 闫昊, 周铭昊, 王磊, 施慧. 甲烷的脱氢芳构化及其与丙烷共芳构化: 反应机理、催化剂设计、积碳和过程强化[J]. 催化学报, 2026, 84: 25-60.

Yu Gu, Shujia Zhang, Minglu Xu, Hao Yan, Minghao Zhou, Lei Wang, Hui Shi. Dehydroaromatization of methane and methane co-aromatization process with propane: Reaction mechanism, catalyst design, carbon deposition and process optimization[J]. Chinese Journal of Catalysis, 2026, 84: 25-60.

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图/表 34

Fig. 1. Converting pathway of methane.

Table 1 The temperature at which dehydrogenation reactions occur spontaneously extracted from Ref. [11].

Reaction	Temperature when Δ_rGθ m = 0 (°C)
CH₄ → C + 2H₂	553
2CH₄ → C₂H₄+2H₂	1323
2CH₄ → C₂H₆ + H₂	> 2227
3CH₄ → C₃H₆ + 3H₂	1582
3CH₄ → C₃H₈ + 2H₂	> 2227
6CH₄ → C₆H₆ + 6H₂	1042
7CH₄ → C₇H₈ + 10H₂	1118
10CH₄ → C₁₀H₈ + 16H₂	1017

Table 2 Equilibrium conversion to carbon and other aromatics at various temperature extracted from Ref. [11].

Product	Temperature (°C)
Product	25	327	527	727	927	1127
C	0	4.8%	33.4%	75.5%	93.7%	98.1%
C₆H₆	0	0.1%	2.4%	13.3%	36.9%	63.6%
C₇H₈	0	0.1%	1.9%	10.6%	30.0%	54.2%
C₁₀H₈	0.2%	0.2%	2.3%	13.1%	36.7%	63.6%

Fig. 2. Maximum thermodynamically allowed levels of non-oxidative methane conversion to hydrogen and ethylene, benzene, coronene, and graphite. Reprinted with permission from Ref. [3]. Copyright 2020, John Wiley and Sons.

Fig. 4. Scheme of hydrocarbon pool mechanism in MDA. R: benzene ring; ball in red: 13C atom; ball in blue: 12C atom; ball in black: H atom. Reprinted with permission from Ref. [27]. Copyright 2017, John Wiley and Sons.

Fig. 7. Scheme of possible positions of Fe within ZSM-5: isolated ions either in framework positions (a) or at the exchange sites (b), bi- and oligonuclear iron complexes in extra-framework positions (c), iron oxide FexOy nanoclusters of size ≤0.55 nm (d), and large iron oxide nanoparticles (Fe2O3) either located at the surface of the zeolite crystal (e) or embedded between the zeolite crystallites (f). Reprinted with permission from Ref. [49]. Copyright 2016, Royal Society of Chemistry.

Fig. 8. Benzene yield as a function of methane pulse numbers over Mo/ZSM-5 catalysts with different Mo loadings. The first 17 pulses (No. ?17 to No. 0) during which no benzene production is detected are categorized as the activation period. Then from the onset of benzene production (pulse No. 1) to a maximum yield (about pulse No. 12 to No. 15), the duration is called induction period. Adapted with permission from Ref. [28]. Copyright 2017, John Wiley and Sons.

Fig. 10. (a) Mo?ssbauer spectra of fresh Fe/ZSM-5 catalysts (2 wt% and 4 wt% Fe loadings) synthesized via a co-crystallization (GSM) and impregnation (IWI) method; GSM catalysts mainly exhibit superparamagnetic low-polymerized Fe3+ oxides inside MFI pores, while on IWI catalysts the Fe3+ oxides are mainly magnetic Fe2O3 particles on the external surface. (b) Schematic correlations between Fe active sites and induction period in MDA reaction. It illustrates that the highly dispersed Fe3+ oxides inside MFI pores could be quickly reduced to sub-oxides thus shorten the induction period, while the big iron oxides particles located at the external surface undergo complete reduction and slow carburization, resulting in a longer induction period. Adapted with permission from Ref. [70]. Copyright 2021, American Chemical Society.

Fig. 11. (a) Electronic edge values based on in situ UV-vis spectra of reference Mo oxide compounds, exhibiting a linear correlation with the number of bridging Mo-O-Mo covalent bonds around the central Mo cation. The value of 4.8 eV for 2 wt% Mo/ZSM-5 (Si/Al = 15) corresponds to Mo oxide species with a single Mo atom. In-situ Raman spectra of Mo/ZSM-5 catalysts under oxygen flow at 773 K as a function of Mo loading for constant Si/Al = 15 (b) and Si/Al ratio for constant 1.3 wt% Mo loading (c) with band assignments to Mo oxide species based on DFT calculations. Reprinted with permission from Ref. [45] Copyright 2015, American Association for the Advancement of Science.

Fig. 13. 13C NMR spectra (a) and DTG profile (b) of spent Mo/ZSM-5 catalyst after different time-on-stream of MDA reaction. TEM picture (c), Ar-physisorption isotherm (d) and derived pore size distribution (e) of the carbon materials obtained after HF leaching of spent Mo/ZSM-5. (f) Structural model of MFI-templated carbon material viewing along b-axis. Reprinted with permission from Ref. [99]. Copyright 2018, American Chemical Society.

Fig. 14. (a) Illustration for the synthesis procedure of hollow H-S-Z capsule zeolite. (b) EDS line analysis of Si element on the cross-section of zeolite capsule structure, showing that Si is located only within the shell of the catalyst. (c) SEM picture, blast holes can be seen after the removal of active carbon template via combustion. Benzene formation rate curves as a function of TOS (d) and TG-DTA profiles of Mo-loaded H-S-Z capsule zeolite and conventional Silicalite-1/ZSM-5 after MDA reaction (e). (f) Scheme of the MDA reaction on Mo/H-S-Z catalyst. Reprinted with permission from Ref. [100]. Copyright 2017, Royal Society of Chemistry.

Fig. 15. (a) HR-TEM picture. EDS-mapping analysis of Si (b) and O (c) elements for ZSM-5 after 24 h treatment in TPAOH solutions. Benzene yield curves as a function of TOS (d) and TG profiles of spent Mo-loaded catalysts based on conventional and TPAOH treated ZSM-5 zeolite (e). The number in the parenthesis indicates different treating time (hour). Reprinted with permission from Ref. [101]. Copyright 2023, Elsevier.

Fig. 16. (a) SEM picture of catalyst MFI-10/0 with lamellar morphology and combined microporous-mesoporous structure. (b) SEM picture of catalyst MFI-10/36 showing conventional MFI morphology without lamellar structure. TG profiles (c) and internal/external coke distribution (d) of spent Mo-loaded catalysts. Notes: The numbers 10 and x in sample MFI-10/x represent the molar fraction of C22-6-6 and TPAOH to SiO2 in the synthesis gel (taking SiO2 as 100); with the increase of x, the obtained catalysts gradually lose the characteristics of lamellar structure and resemble conventional MFI morphology, see Fig. (b); In Fig. (c), the carbon deposits of MFI-10/0 is the highest, indicating that the lamellar structure has abundant mesopores that can accommodate carbon deposits, as the lamellar structure gradually disappears, the carbon deposits after MDA reaction also gradually decreases, and the proportion of coke inside the pores increases significantly. Reprinted with permission from Ref. [104]. Copyright 2015, Elsevier.

Fig. 17. (a) HAADF-STEM images of four Mo/HZSM-5 catalysts Mo/Z5(2), Mo/Z5(60), Mo/Z5(400) and Mo/Z5-C with dimensions along the b-axis of 2, 60 and 400 nm, respectively, (Mo/Z5-C means Mo is support on commercial ZSM-5 with b-axis length of ~400 nm but a much longer a-axis length than Mo/Z5(400)). (b) Methane conversion and benzene yield of Mo/Z5(60) and Mo/Z5(400) as a function of TOS during MDA reaction, that Mo/Z5(60) shows a much faster deactivation (2.88h) than Mo/Z5(400) (4.56 h). (c) Integrated NH3-TPD peak areas of parent Z5 (blue dots) and Mo loaded Mo/Z5 (red dots) determined at different TOS, in which acid sites are kept on Mo/Z5(60) during MDA reaction, while they are gradually lost on Mo/Z5(400). (d) HAADF-STEM images of spent Mo/Z5(60) after 300 min and Mo/Z5(400) after 600 min of MDA reaction, that sintered molybdenum carbide particles are obvious on spent Mo/Z5(60) (5?20 nm bright spots) but are barely seen on spent Mo/Z5(400). (e) TEM pictures of spent Mo/Z5(60), showing carbon deposits covering MoCx particles with layers thickness of 3?4 nm. Reprinted with permission from Ref. [109]. Copyright 2021, Elsevier.

Fig. 18. Methane conversion (a) and cumulative selectivity of main products (b) for nano-sized ellipsoid, hexagonal bar and coffin shaped Mo/ZSM-5 catalyst during MDA, respectively. (c) TG profiles of spent Mo-loaded catalysts. (d) Schematic structure-performance relationships in the three catalysts: although the smallest nano-sized ellipsoid catalysts possess the shortest intra-diffusion, it generated largest coke accumulation due to the inter-diffusional restrictions. The elongated coffin-shaped zeolite could suffer from longest intra-diffusion, but the lowest coke accumulation could be expected due to the homogeneous coke distribution. Reprinted with permission from Ref. [110]. Copyright 2023, Elsevier.

Fig. 19. Cumulative hydrocarbon selectivities and methane conversion on a 2 wt% Mo/H-ZSM-5 after 14 hours of MDA reaction at 725 °C under different feeding water partial pressure. This picture shows that methane conversion together with aromatics selectivity increase with water partial pressure increasing from 0 to 0.037, along with a decaying coking selectivity. However, the trend reverses when water partial pressure is further elevated to 0.107. Reprinted with permission from Ref. [26]. Copyright 2021, American Chemical Society.

Fig. 20. (a) Scheme of the current-controlled co-ionic membrane reactor, that CH4 is converted to benzene and hydrogen catalyzed by a 6Mo/MCM-22 catalyst packed within the interlayer outside the membrane. H2 generated there is transported as protons through the membrane to the sweep side, and oxide ions from the reduction of steam in the sweep side are transported through the membrane to the MDA reaction side to react with H2 and form steam to remove coke deposition. (b) Aromatics yield versus time in both the membrane reactor and a conventional fixed bed reactor in MDA. (c) Corresponding coke amount and cumulative aromatics production in 6Mo/MCM-22 within the above two reactors. Reprinted with permission from Ref. [129]. Copyright 2016, American Association for the Advancement of Science.

Fig. 21. Simplified (a) and detailed (b) piping and instrumentation diagram of the constructed looping reactor system used for methane recirculation, and the states in the three reactors marked in dashed red squares in section 1, 2 and 3 correspond to processes of methane dehydroaromatization, Fe3O4 being reduced to FeO by H2, and water being adsorbed by molecular sieves, respectively; meanwhile, the states in the three reactors marked in dashed blue squares in section 1, 2 and 3 corresponds to the opposite processes parallel to their counterparts, namely carbon combustion of coked MDA catalysts, FeO being oxidized to Fe3O4 by H2O, and water desorption from molecular sieves, respectively. (c) CH4 conversion and main product yields in a 2 cycle testing. Reprinted with permission from Ref. [132]. Copyright 2021, Elsevier.

Fig. 22. (a) STEM-HAADF image and computational model (inset) of the Fe@SiO2 catalyst. (b) Methane conversion and ethylene, benzene and other aromatics selectivity versus TOS over this catalyst at 1090 °C. Negligible coke was observed. Reprinted with permission from Ref. [2]. Copyright 2014, American Association for the Advancement of Science.

Fig. 23. (a) Temperature and gas flow profiles used for all tests. (b) Time-courses of methane conversions as a function of TOS in the tests with different cycle periods over 5 wt% Mo/HZSM-5 at 1073 K and 21080 mL/(g·h), while only CH4 flow times were accounted and accumulated in the figure. (c) TPO profiles of spent catalysts exposed to CH4 for different durations. (d) Time-courses of benzene and naphthalene formation rates obtained in a large degree of deactivation-long time regeneration cycle test over 5%Mo/HZSM-5 at 1073 K and 21080 mL/(g·h). (e) Schematic diagram of a proposed triple-bed circulating fluidized bed reactor system: (1) CH4 converter, (2) regenerator in the main stream with a short mean residence time of catalyst particles and (3) regenerator in the sub-stream with a long mean residence time. Reprinted with permission from Ref. [123]. Copyright 2011, Elsevier.

Fig. 24. (a) Schematic illustration of the selective removal of Ga from impregnated Ga/Z catalysts by hydrochloric acid (HA) treatment. (b) Ga content and textural properties of Ga/Z-xHA, and the number before HA stands for the molar concentration of the treating HCl solution. It could be seen that after HA treatment the catalyst loses most of its Ga loading, and more micropores are dug up. (c) Propane conversion and BTX yield of Ga/Z-xHA catalysts as a function of TOS. Reprinted with permission from Ref. [171]. Copyright 2022, Elsevier.

Fig. 25. Scheme of π-complex and σ-allylzinc species as intermediates during propane conversion to aromatics over Zn supported on Beta zeolite. Reprinted with permission from Ref. [175]. Copyright 2010, American Chemical Society.

Fig. 26. Proposed propane aromatization processes mediated by cyclopentenyl cations over Ga/ZSM-5: direct dehydroaromatization (a) and carbocation promoted dehydroaromatization (b). Reprinted with permission from Ref. [178]. Copyright 2021, John Wiley and Sons.

Fig. 28. Catalytic performance of GaOy/meso-XHZSM-5 (X means Si/Al ratio) catalysts: conversion of methane and propane (a) and BTX yield (b). Reprinted with permission from Ref. [194]. Copyright 2019, Royal Society of Chemistry.

Fig. 29. (a) Scheme of one step synthesis (OSS) procedure of Ga/ZSM-5 catalysts. (b) 71Ga NMR spectra of OSS catalysts and impregnated ones, showing that most of the Ga species are in tetrahedral coordination within or in close contact with zeolite framework in OSS catalysts, while Ga resides mainly on the external surface of ZSM-5 as big Ga2O3 particles. (c) Schematic illustration of improved MPCA performance via highly dispersed Ga sites within the zeolite channels. (d) Total aromatic yield as a function of TOS, that OSS catalysts exhibit higher yield than their impregnated counterparts. (e) Methane conversion, propane conversion and benzene selectivity on OSS catalysts with different Si/Al ratio, that methane conversion increases gradually with Si/Al while propane shows a reversed trend, and benzene selectivity is barely affected by Si/Al. (f) Schematic illustration of the role of BAS in MPCA. Reprinted with permission from Ref. [196]. Copyright 2024, American Chemical Society.

Fig. 30. Calculated equilibrium methane conversion as functions of CH4/C3H8 molar ratio in the feed, based on two different reaction models: (a) Model I, in which no limitation is imposed on reaction pathways among the reacting species, or that is to say under which methane formation via propane cracking could happen. (b) Model II, in which methane formation by propane cracking is inhibited. Reaction temperature: 600 °C, pressure: 1.01 bar. Reprinted with permission from Ref. [199]. Copyright 2014, American Chemical Society.

Table 3 Comparison between MDA, PDA and MPCA.

Process	Feed	Reaction temperature	Used catalyst	Thermodynamic upper limit of methane conversion to benzene	Industrialized
MDA	Methane	> 700 °C	Mo/ZSM-5	About 12% at 700 °C	No
PDA	Propane	500‒600 °C	Ga/ZSM-5, Zn/ZSM-5, Pt/ZSM-5	—	Yes
MPCA	Methane & propane	500‒600 °C	Ga/ZSM-5, Zn/ZSM-5	No widely-accepted value ¹	No

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甲烷的脱氢芳构化及其与丙烷共芳构化: 反应机理、催化剂设计、积碳和过程强化

Dehydroaromatization of methane and methane co-aromatization process with propane: Reaction mechanism, catalyst design, carbon deposition and process optimization

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