甲烷完全催化氧化研究进展

doi:10.15541/jim20230117

无机材料学报 ›› 2023, Vol. 38 ›› Issue (11): 1245-1256.DOI: 10.15541/jim20230117 CSTR: 32189.14.10.15541/jim20230117

所属专题：【能源环境】污染物去除(202312)

• 综述 • 下一篇

甲烷完全催化氧化研究进展

孙晨¹^,²(), 赵昆峰²(), 易志国¹^,²()

1.上海理工大学材料与化学学院, 上海 200093
2.中国科学院上海硅酸盐研究所, 上海 201899

收稿日期:2023-01-27 修回日期:2023-04-25 出版日期:2023-11-20 网络出版日期:2023-05-04
通讯作者: 易志国, 研究员. E-mail: zhiguo@mail.sic.ac.cn;
赵昆峰, 副研究员. E-mail: zhaokunfeng@mail.sic.ac.cn
作者简介:孙晨(1996-), 男, 硕士研究生. E-mail: 895029730@qq.com
基金资助:
科技部高端外专项目(G2022055014L)

Research Progress in Catalytic Total Oxidation of Methane

SUN Chen¹^,²(), ZHAO Kunfeng²(), YI Zhiguo¹^,²()

1. School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China
2. Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China

Received:2023-01-27 Revised:2023-04-25 Published:2023-11-20 Online:2023-05-04
Contact: YI Zhiguo, professor. E-mail: zhiguo@mail.sic.ac.cn;
ZHAO Kunfeng, associate professor. E-mail: zhaokunfeng@mail.sic.ac.cn
About author:SUN Chen (1996-), male, Master candidate. E-mail: 895029730@qq.com
Supported by:
Top Foreign Expert Project of the Ministry of Science and Technology of China(G2022055014L)

摘要/Abstract

摘要：

甲烷是对全球温升贡献仅次于二氧化碳的温室气体, 且其全球增温潜势是CO₂的80倍以上。在全球变暖和大气中甲烷含量不断增长的背景下, 完全催化氧化大气甲烷对于减缓温室效应和全球变暖具有重要价值。然而, 由于甲烷具有较高的结构稳定性, 在温和条件下将其催化氧化一直面临巨大的挑战。本文综述了近年来甲烷完全氧化在热催化、光催化以及光热协同催化三种反应条件下的研究进展, 热催化中高温增大了能耗并加速了催化剂的失活, 开发低温反应条件下的催化剂已经成为甲烷完全热催化的重点; 光催化提供了一种常温常压条件下利用光能氧化甲烷的方法, 但是相对热催化来说反应速率较低; 光热协同催化在光能和热能的协同作用下, 可实现温和条件下的甲烷高效完全催化氧化, 表现出潜在的应用前景。本文就三种反应催化剂的发展进行综述, 系统分析了不同反应的原理, 以及不同反应条件下甲烷完全催化氧化的优势与不足, 同时总结了催化氧化甲烷所面临的挑战, 并提供潜在的解决方案, 期望为今后的甲烷氧化研究提供借鉴。

关键词: 甲烷完全氧化, 热催化, 光催化, 光热协同, 综述

Abstract:

Methane is the second greenhouse gas contributing greatly to global warming, about 80 times of CO₂. Considering background of global warming and atmospheric methane growth, to catalyze total oxidation of atmospheric methane is of great importance to mitigate greenhouse effects and slow this global warming. However, catalytic oxidation of methane has always been a big challenge due to its high structural stability. In this article, research progress in total oxidation of methane under thermal-, photo- and photothermal-catalysis was reviewed. High temperature in thermal catalysis increases the energy loss and accelerates the deactivation of catalysts speedingly. Therefore, development of catalysts that oxidize methane under moderate temperatures is the main research interests. Photocatalysis provides a way to eliminate methane at ambient conditions with the assistance of solar energy, but the reaction rates are lower than that in thermal catalysis. It is worth mentioning that photothermal catalysis, developed in recent years, can achieve efficiently catalytic total oxidation of methane under mild conditions, showing a high potential application prospect. This article reviews development of three modes of catalysis, analyzes their different reaction mechanisms, advantages and disadvantages under different reaction conditions. Finally, prospects and challenges of this catalytic total oxidation are pointed out, which is expected to provide references for future research on this field.

Key words: catalytic oxidation of methane, thermal catalysis, photocatalysis, photothermal catalysis, review

中图分类号:

O643

孙晨, 赵昆峰, 易志国. 甲烷完全催化氧化研究进展[J]. 无机材料学报, 2023, 38(11): 1245-1256.

SUN Chen, ZHAO Kunfeng, YI Zhiguo. Research Progress in Catalytic Total Oxidation of Methane[J]. Journal of Inorganic Materials, 2023, 38(11): 1245-1256.

图/表 11

图1 甲烷完全热催化氧化的催化剂特性总结[17]

Fig. 1 Summary of catalyst properties for the total oxidation of methane by thermal catalysis[17]

图2 催化剂的性能测试及理论计算[28]

Fig. 2 Performance tests and theoretical calculations of catalysts[28] (a) Light-off curves and T50 values of Pd/Al2O3 after O2 (600 ℃), O2-H2, steam (600 ℃), and steam-O2 pretreatments; (b) GB density statistical histogram of laser-generated Pd/Al2O3 and Pd/Al2O3 after steam (600 ℃) and O2-H2 pretreatments; (c, d) Calculated free energy diagrams for breaking the first C-H bond in CH4 on PdO(101) and PdO(110), respectively. Reprinted from Ref. [28] with permission, Copyright 2021 AAAS

图3 化学吸附氧原子饱和的Pt0−Pt4+偶极子上的甲烷解离吸附模型[30]

Fig. 3 Proposed model for the CH4 dissociative adsorption over Pt0−Pt4+ dipoles saturated with chemisorbtion oxygen atoms[30] (a) Reactants: CH4 in the gas phase and 1% Pt/Cr2O3; (b) CH4 polarization by Pt0−Pt4+ site and formation of a transition state; (c) Abstraction of the first hydrogen on the adsorbed CH4 molecule

表1 甲烷完全热催化氧化催化剂的性能比较

Table 1 Comparison of properties of catalysts for total oxidation of methane by thermal catalysis

Catalyst	T_c^*/℃	E_a/(kJ·mol^-1)	Feed gas	GHSV/(mL·g^-1·h^-1)	Stability	Ref.
Pd-Ce@SiO₂	T₁₀₀=350	100.4	1% CH₄, 21% O₂, bal. N₂	36000	25 h	[39]
Pd/TiO₂	T₉₉=370	83.1	1% CH₄, 10% O₂, bal. N₂	30000	4 cycles	[40]
Pd/Na-MOR	T₅₀=335	75	1% CH₄, 4% O₂, bal. N₂	70000	90 h	[41]
Pd-Pt/CeO₂	T₅₀=325	74	680 μg/mL CH₄, 14% O₂, 5% CO₂, bal. N₂	300000	12 h^#	[42]
Au/Al₂O₃	T₅₀=480	73	0.8% CH₄, 3.2% O₂, bal. He,	15000	/	[32]
Rh/ZrO₂	T₅₀=400	/	1% CH₄, 2% O₂, bal. He	15000	/	[31]
Ir/TiO₂-H	T₅₀=267	55.5	1% CH₄, 20% O₂, bal. N₂	30000	50 h	[43]
Ag/MnLaO₃	T₅₀=580	74	2% CH₄, 98% air	12000	/	[44]
Pt/Cr₂O₃	T₅₀=350	/	0.2% CH₄, 10% O₂, bal. N₂	30000	/	[30]
MgO	T₅₀=225	/	1% CH₄, 99% air	6000	70 h	[45]
LaCoO₃	T₅₀=470	/	0.8% CH₄, 5% O₂, bal. N₂	60000	/	[46]
NiCo₂O₄	T₁₀₀=350	/	5% CH₄, 25% O₂, bal. Ar	24000	48 h^#	[47]
La_0.6Sr_0.4MnO₃	T₅₀=566	56.6	2% CH₄, 20% O₂, bal. N₂	30000	/	[48]
CoAlO_x/CeO₂	T₅₀=415	92.2	10% CH₄, 25% O₂, bal. Ar	24000	50 h	[49]

图4 (a)半导体基光催化剂的甲烷活化示意图[1]和(b)常用半导体的能带结构和不同反应物的氧化还原电位示意图[55]

Fig. 4 (a) Schematic diagram of methane activation over semiconductor-based photocatalysts[1]; (b) Schematic diagram of band structures of commonly used semiconductors and redox potentials of different reactants[55]

图5 ZnO基半导体在甲烷完全光催化氧化中的应用

Fig. 5 Application of ZnO-based semiconductor in photocatalytic total oxidation of methane (a) Time evolution of photocatalytic total oxidation of methane over 0.1% Ag-decorated ZnO nanocatalysts at different CH4 concentrations[56] (Reprinted from Ref. [56] with permission, Copyright 2016 Springer Nature); (b) Time evolution of photocatalytic total oxidation of methaneover various catalysts with a CH4 input of 100 μL/L[58] (Reprinted from Ref. [58] with permission, Copyright 2019 Royal Society of Chemistry); (c) Catalytic activity of total oxidation of methane (top) and the crystal morphology (bottom) of a ZnO nanosheet and nanorod[59] (Reprinted from Ref. [59] with permission, Copyright 2019 American Chemical Society)

图6 Ga2O3/AC甲烷完全光催化氧化性能测试及氧化机理示意图[60]

Fig. 6 Ga2O3/AC photocatalytic total oxidation of methane and schematic diagram of oxidation mechanism[60] (a) Recycled test of photocatalytic oxidation of CH4 over 15% Ga2O3/AC; (b) Proposed mechanism for photocatalytic oxidation of CH4 over Ga2O3/AC composites. Reprinted from Ref. [60] with permission, Copyright 2017 Royal Society of Chemistry

图7 不同TiO2表面甲烷吸附能以及DFT计算[61]

Fig. 7 Adsorption energy calculations of surface methane and DFT calculation of different TiO2 [61] (a1-a3) Most stable adsorption configurations of CH4 on (a1) anatase TiO2(001)-(1×4), (a2) anatase TiO2(100)-(1×2), and (a3) anatase TiO2(101) surfaces. Gray and red balls represent Ti and O atoms, respectively; (b1, b2, c1,c2, d1, d2) Calculated PDOS of (b1) bare and (b2) CH4-adsorbed anatase TiO2(001)-(1×4) surfaces, (c1) bare and (c2) CH4-adsorbed anatase TiO2(100)-(12) surfaces, and (d1) bare and (d2) CH4-adsorbed anatase TiO2-(101) surfaces. Reprinted from Ref. 61 with permission, Copyright 2022 American Chemical Society

表2 甲烷完全催化氧化光催化剂的性能比较

Table 2 Comparison of performances of photocatalysts for total oxidation of methane by photocatalysis

Catalyst	Reaction conditions	Yield/(μmol·h^-1)	Ref.
TiO₂	Batch reactor, 3×10⁵Pa CH₄, Xe lamp, RT	1.1	[62]
TiO₂	Batch reactor, 2×10⁶Pa CH₄, 5 bar O₂, Xe lamp, RT	23	[63]
ZnO	Batch reactor, 1×10⁵Pa, 250 μg/mL CH₄ in air, Xe lamp, RT	2	[59]
Ag/ZnO	Batch reactor, 1×10⁵Pa, 250 μg/mL CH₄, Xe lamp, RT	22	[56]
CuO/ZnO	Batch reactor, 1×10⁵Pa, 100 μg/mL CH₄, Xe lamp, RT	4	[58]
Au-CeO₂/ZnO	Batch reactor, 1×10⁵Pa, 250 μg/mL CH₄, Xe lamp, RT	0.6	[57]
Ag/AgCl	Batch reactor, 1×10⁵Pa, 500 μg/mL CH₄, Xe lamp, RT	5.4	[64]
SrCO₃/SrTiO₃	Batch reactor, 1×10⁵Pa, 200 μg/mL CH₄, Xe lamp, RT	0.8	[65]
BiVO₄	Batch reactor, 1×10⁵Pa, 20 μg/mL CH₄, visible light, RT	0.05	[66]

图8 ZnO/LSCO光催化及光热协同催化甲烷完全氧化性能测试[70]

Fig. 8 Tests of ZnO/LSCO photocatalysis and photothermal cocatalysis for methane total oxidation[70] (a) Temperature profiles on these monolithic catalysts under irradiation of Xe lamp; (b) CH4 photothermal conversions over these monolithic catalysts under Xe lamp irradiation; (c) Comparison of CH4 conversion for ZnO/LSCO under Xe lamp irradiation and direct thermal heating (furnace) at the same temperature; (d) Activity comparison of methane oxidation with previous studies by normalized reaction rate constant. Reprinted from Ref. [70] with permission, Copyright 2008 American Chemical Society

图9 HPMC光热协同催化甲烷完全氧化性能(a,b)及其机理示意图(c)[71]

Fig. 9 HPMC photothermal co-catalyzed methane total oxidation performance (a, b) and its mechanism (c)[71] (a) Cycling stability test of HPMC; (b) Methane conversion measured at 200 ℃ with different optical power (OPD); (c) Reaction mechanism of HPMC catalyzed methane combustion. Reprinted from Ref. [71] with permission, Copyright 2021 Wiley

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甲烷完全催化氧化研究进展

Research Progress in Catalytic Total Oxidation of Methane

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