甲烷转化用抗积碳催化材料研究进展

doi:10.15541/jim20250439

无机材料学报 ›› 2026, Vol. 41 ›› Issue (6): 739-750.DOI: 10.15541/jim20250439

甲烷转化用抗积碳催化材料研究进展

王俊卜¹^,²(), 黄泽皑¹^,²(), 杨茗凯², 蒙颖², 周明炜², 周莹¹^,²()

¹ 西南石油大学油气藏地质及开发工程全国重点实验室, 成都 610500
² 西南石油大学新能源与材料学院, 成都 610500

收稿日期:2025-10-31 修回日期:2025-12-10 出版日期:2026-06-20 网络出版日期:2026-01-22
通讯作者: 黄泽皑, 副教授. E-mail: zeai.Huang@swpu.edu.cn;
周莹, 教授. E-mail: yzhou@swpu.edu.cn
作者简介:王俊卜(1996-), 女, 博士研究生. E-mail: wangjb0401@163.com
基金资助:
国家杰出青年科学基金(52325401);国家重点研发计划(2025YFE0112700);国际合作项目(W2412080)

Research Progress on Anti-coking Catalytic Materials for Methane Conversion

WANG Junbu¹^,²(), HUANG Zeai¹^,²(), YANG Mingkai², MENG Ying², ZHOU Mingwei², ZHOU Ying¹^,²()

¹ National Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China
² School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China

Received:2025-10-31 Revised:2025-12-10 Published:2026-06-20 Online:2026-01-22
Contact: HUANG Zeai, associate professor. E-mail: zeai.Huang@swpu.edu.cn;
ZHOU Ying, professor. E-mail: yzhou@swpu.edu.cn
About author:WANG Junbu (1996-), female, PhD candidate. E-mail: wangjb0401@163.com
Supported by:
National Science Fund for Distinguished Young Scholars of China(52325401);National Key R&D Program of China(2025YFE0112700);International Cooperation Project(W2412080)

摘要/Abstract

摘要：

甲烷是天然气、页岩气、沼气及天然气水合物等资源中的主要组分, 因其含氢量高、资源丰富而成为生产高附加值化学品的重要原料。然而, 甲烷具有较高的化学稳定性, 其催化转化面临高活化能和复杂的积碳问题, 常导致催化剂失活、寿命缩短和选择性下降, 成为制约其高效利用的关键瓶颈。在全球能源结构转型与化工产业升级的背景下, 开发高性能甲烷催化体系具有重要意义。近年来, 热催化、光热催化和光电催化等外场驱动技术为甲烷在温和条件下的转化提供了新的可能, 但不同反应路径均涉及复杂的积碳形成机制。本文在总结氧化性与非氧化性气氛中甲烷催化转化过程的积碳形成机制基础上, 系统阐述了催化剂在热催化材料体系、光热/光电催化材料体系及熔融催化材料体系中的作用, 重点探讨了活性位点设计、金属-载体界面调控等策略对积碳生成、催化寿命和选择性的影响。最后, 本文归纳了催化剂抗积碳及再生策略, 并展望了未来甲烷催化转化技术的发展方向。

关键词: 甲烷转化, 抗积碳, 催化剂, 反应机理, 综述

Abstract:

Methane, a primary component of natural gas, shale gas, biogas, and gas hydrates, constitutes a vast hydrogen-rich resource for production of high-value chemicals. However, its intrinsic chemical inertness poses significant challenges for catalytic conversion, primarily due to high activation barriers and severe carbon deposition (coking). These challenges result in rapid catalyst deactivation and reduced selectivity, thereby hindering industrial viability. Consequently, developing high-performance catalytic systems for methane conversion is of strategic importance against the backdrop of global chemical industry upgrading and the demand for efficient energy utilization. While emerging externally driven strategies, including thermocatalysis, photothermal catalysis, and photo-electrocatalysis, enable methane conversion under milder conditions, managing complex carbon deposition remains a persistent challenge. This review systematically categorizes the formation mechanisms of carbon species under both oxidative and non-oxidative environments. Performances of various catalytic systems are examined, ranging from solid-state thermocatalytic and photocatalytic materials to molten-phase frameworks. Special attention is devoted to active site design and metal-support interface engineering as key determinants of carbon resistance, catalytic stability, and product selectivity. Furthermore, mitigation strategies are critically evaluated. Finally, this review outlines future opportunities through the integration of structural optimization, kinetic modulation, field-assisted catalysis, and intelligent design to develop robust, selective, and long-life catalysts for methane valorization.

Key words: methane conversion, anti-coking, catalyst, reaction mechanism, review

中图分类号:

O643

王俊卜, 黄泽皑, 杨茗凯, 蒙颖, 周明炜, 周莹. 甲烷转化用抗积碳催化材料研究进展[J]. 无机材料学报, 2026, 41(6): 739-750.

WANG Junbu, HUANG Zeai, YANG Mingkai, MENG Ying, ZHOU Mingwei, ZHOU Ying. Research Progress on Anti-coking Catalytic Materials for Methane Conversion[J]. Journal of Inorganic Materials, 2026, 41(6): 739-750.

图/表 6

图1 甲烷转化为高附加值产品的抗积碳催化剂分类

Fig. 1 Classification of anti-coking catalysts for methane conversion to value-added products

图2 不同热催化剂的积碳性能及抗积碳示意图[15,24,26,32]

Fig. 2 Carbon deposition performance and schematic of anti-coking of different thermocatalysts[15,24,26,32] (a) Catalytic performance of 2% (in mass) Pt/Mo2TiC2Tx for non-oxidative coupling of methane[15]; (b) Raman spectra of the catalysts after the DRM stability test[24]; (c) High resolution transmission electron microscopy (HR-TEM) images and corresponding contact angles with a schematic diagram of the different metal-support interaction (MSI) exsolution catalysts[24]; (d) Carbon deposition rate and catalyst schematic diagram of Ni/BCN[26]; (e) Schematic diagram of multielement oxide (MEO) thin layer constrained stable nickel catalyst[32]

表1

Table 1 Comparison of the stability of photothermal catalysts[38-45]

Catalyst	Reaction condition	Stability	Ref.
Ni/CeO₂	CH₄/CO₂/Ar=1/1/3, 20 mL·min⁻¹, 25 mg, 2.4 W·cm^-2	230 h	[38]
Ni/Pr₅-CeO₂	CH₄/CO₂/Ar=1/1/3, 20 mL·min⁻¹, 25 mg, 2.4 W·cm^-2	110 h	[39]
NiMo/MgO	CH₄/CO₂/Ar=1/1/3, 20 mL·min⁻¹, 25 mg, 2.4 W·cm^-2	60 h	[40]
Pd-Bi/Ga₂O₃	CH₄/Ar=1/9, 30 mL·min⁻¹, 800 mg, 20 W·cm^-2	100 h	[41]
Ni/CeO₂(100)	CH₄/CO₂=1/1, 10 mL·min⁻¹, 200 mg, 6.8 W·cm^-2	800 h	[42]
Cu-Ru/MgO-Al₂O₃	CH₄/CO₂=1/1, 16 mL·min^-1, 1.5 mg, 19.2 W·cm^-2	50h	[43]
(Ni/CeO₂)@SiO₂	CH₄/CO₂/N₂=3/3/4, 50 mL·min^-1, 25 mg, 300 W Xe lamp	40 h	[44]
Pd-Ni/Al₂O₃	CH₄/CO₂/Ar=3/3/4, 89.6 mL·min^-1, 8 mg, 80.3 kW·cm^-2	50 h	[45]

图3 光热催化剂催化机理与抗积碳性能[38,40,42]

Fig. 3 Mechanism and anti-coking performance of photothermal catalysts[38,40,42] (a) Long-term stability of the thermo-photo catalytic DRM reaction over NiSA/CeO2 and NiNP/CeO2 catalysts at 472 ℃[38]; (b) Comparison of the anti-coking mechanism and coking mechanism of Ni single-atom sites under synergistic photothermal catalysis[38];(c, d) In situ DRIFTS spectra over NiMo/MgO under (c) photothermal and (d) thermal conditions[40]; (e) Solar-concentrating catalytic system[42]; (f) Solar-concentrated catalytic DRM performance by using sunlight over Ni/CeO2(100) catalyst (the test was performed on November 16, 2022, at 104°11'15.0936'' E and 30°49'56.82'' N)[42]

图4 在电场调控下催化剂的合成机理、积碳性能及抗积碳示意图[53-55,57]

Fig. 4 Diagrams of the synthesis mechanism of the catalyst under electric field regulation, carbon deposition performance, and anti-coking illustration[53-55,57] (a) Time-on-stream stability at 800 ℃ and 200mA·cm-2 using a CO2/CH4 feed ratio of two[53]; (b) Schematic diagram of the catalyst preparation[54]; (c) CO2 conversion[55]; (d) Network of surface reaction pathways for plasma-catalytic CH4/CO2 reforming over Ni-based catalyst[57]

图5 不同类型熔融介质的催化活性与反应机理[61,68 -69]

Fig. 5 Catalytic activity and reaction mechanism diagrams for different types of molten media[61,68 -69] (a) Catalytic activity of various mono-metallic and alloy systems for methane pyrolysis under molten conditions[61]; (b) Mechanistic schematic of methane decomposition over molten metals/alloys[61]; (c) Molten salts[68]; (d) Molten salt-metal composite catalysts[69]

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甲烷转化用抗积碳催化材料研究进展

Research Progress on Anti-coking Catalytic Materials for Methane Conversion

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