Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究

doi:10.11949/0438-1157.20250482

化工学报 ›› 2025, Vol. 76 ›› Issue (11): 5604-5616.DOI: 10.11949/0438-1157.20250482

• 专栏：能源利用过程中的多相流与传热 • 上一篇下一篇

Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究

邱家齐¹^,²(), 杨仲卿¹^,²(), 张志刚³, 甘海龙³, 霍春秀³, 窦志帅¹^,², 冉景煜¹^,²

^1.低品位能源利用技术及系统教育部重点实验室（重庆大学），重庆 400044
^2.重庆大学能源与动力工程学院，重庆 400044
^3.中煤科工集团重庆研究院有限公司，重庆 400039

收稿日期:2025-05-06 修回日期:2025-07-10 出版日期:2025-11-25 发布日期:2025-12-19
通讯作者: 杨仲卿
作者简介:邱家齐（1998—），男，博士研究生，qjq@cqu.edu.cn
基金资助:
国家自然科学基金项目(52276099);中煤科工集团科技计划项目(2024-TD-ZD020);中煤科工集团重庆研究院有限公司自立项目(2024ZDYF19)

Mechanistic study of Mn/Ce co-doping for enhanced oxygen species conversion and catalytic combustion of dilute methane

Jiaqi QIU¹^,²(), Zhongqing YANG¹^,²(), Zhigang ZHANG³, Hailong GAN³, Chunxiu HUO³, Zhishuai DOU¹^,², Jingyu RAN¹^,²

^1.Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Ministry of Education, Chongqing University, Chongqing 400044, China
^2.School of Energy and Power Engineering, Chongqing University, Chongqing 400044, China
^3.China Coal Technology and Engineering Group Chongqing Research Institute, Chongqing 400039, China

Received:2025-05-06 Revised:2025-07-10 Online:2025-11-25 Published:2025-12-19
Contact: Zhongqing YANG

摘要/Abstract

摘要：

合成了一系列具有不同Mn/Ce掺杂比例的Cu基整体式催化剂，并使用其进行了稀薄甲烷催化燃烧活性测试。其中，4Cu-3Mn-1Ce催化剂展现出最佳的甲烷催化活性，在550℃下转化率达85.0%，并且在600℃下实现了完全转化。利用包括原位红外光谱（in situ FTIR）在内的一系列表征分析与密度泛函理论（DFT）模拟计算探究了Mn/Ce掺杂对Cu基整体式催化剂理化性质的作用机制，Mn/Ce掺杂强化Cu基整体式催化剂稀薄甲烷催化燃烧活性可以归因为：Ce掺杂构建Ce-Cu固溶体，弱化Cu—O键合，促进高温下晶格氧的扩散，从而强化高温催化活性；Mn掺杂促进催化剂对O₂的吸附，强化低温下甲烷的催化活性；Mn/Ce共掺杂强化O₂活化并解离为*O，*O填补进入氧空位再生为晶格氧，共掺杂强化了氧物种循环，从而显著提高稀薄甲烷催化燃烧活性。

关键词: 催化, 甲烷, 活化, 燃烧, 掺杂

Abstract:

In this study, a series of Cu-based monolithic catalysts with different Mn/Ce doping ratios were synthesized and used for catalytic combustion activity testing of dilute methane. Among them, the 4Cu-3Mn-1Ce catalyst exhibited the best methane catalytic activity with a conversion of 85.0% at 550℃ and achieved complete conversion at 600℃. The mechanism of the effect of Mn/Ce doping on the physicochemical properties of Cu-based monolithic catalysts was investigated by characterization analysis, including in situ Fourier Transform infrared spectroscopy (in situ FTIR), and density functional theory (DFT) simulation calculations. The enhanced methane catalytic combustion activity of the Cu-based monolithic catalysts can be attributed to the following: Ce doping forming a Ce-Cu solid solution, weakening the Cu—O bond, and promoting lattice oxygen diffusion at high temperatures, thus enhancing high-temperature catalytic activity; and Mn doping promotes the adsorption of O₂ on the catalysts, which strengthens methane oxidation at low temperatures; Mn/Ce co-doping strengthens the activation of O₂ and its dissociation to *O, which fills the oxygen vacancies and regenerates into lattice oxygen, the co-doping strengthens the cycle of oxygen species and thus significantly improves the catalytic combustion activity of thin and dilute methane.

Key words: catalysis, methane, activation, combustion, doping

中图分类号:

TQ 426.83

邱家齐, 杨仲卿, 张志刚, 甘海龙, 霍春秀, 窦志帅, 冉景煜. Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究[J]. 化工学报, 2025, 76(11): 5604-5616.

Jiaqi QIU, Zhongqing YANG, Zhigang ZHANG, Hailong GAN, Chunxiu HUO, Zhishuai DOU, Jingyu RAN. Mechanistic study of Mn/Ce co-doping for enhanced oxygen species conversion and catalytic combustion of dilute methane[J]. CIESC Journal, 2025, 76(11): 5604-5616.

图/表 13

图1 稀薄甲烷催化燃烧实验测试系统

Fig.1 Experimental test system for catalytic combustion of dilute methane

图2 (a)不同Mn/Ce掺杂比例样品的催化活性测试；(b)4Cu-3Mn-1Ce对不同初始浓度甲烷的催化活性

Fig.2 (a) Catalytic activity test of samples with different Mn/Ce doping ratios; (b) Catalytic activity of 4Cu-3Mn-1Ce for different initial concentrations of methane

表1 不同Mn/Ce掺杂比例样品的特征温度

Table 1 Characteristic temperatures of samples with different Mn/Ce doping ratios

序号	催化剂种类	T₁₀/℃	T₅₀/℃	T₉₀/℃
1	8 Cu	459.1	541.9	619.9
2	4Cu-4Mn	419.8	515.9	584.9
3	4Cu-3Mn-1Ce	404.8	513.1	558.1
4	4Cu-2Mn-2Ce	418.6	520.6	574.9
5	4Cu-1Mn-3Ce	424.4	520.6	571.9
6	4Cu-4Ce	427.7	520.6	573.2

图3 (a)4Cu-3Mn-1Ce样品的稳定性测试；(b)稳定性实验后样品的循环稳定性

Fig.3 (a) 4Cu-3Mn-1Ce sample stability test; (b) Cyclic stability of samples after stability testing

图4 样品的SEM及EDS能谱面扫图像

Fig.4 SEM and EDS images of samples

图5 不同Mn/Ce掺杂比例样品的XRD谱图

Fig.5 XRD patterns of samples with different Mn/Ce doping ratios

图6 不同Mn/Ce掺杂比例样品的O 1s轨道的XPS精细谱

Fig.6 XPS spectra of O 1s orbitals of samples with different Mn/Ce doping ratios

表2 不同Mn/Ce掺杂比例样品的O物种含量分布

Table 2 Distribution of O species content in samples with different Mn/Ce doping ratios

样品	含量/%
样品	O_latt	O_sur	O_ads
4Cu-4Ce	22.5	34.1	43.4
4Cu-4Mn	10.8	32.2	57.0
4Cu-3Mn-1Ce	19.0	44.0	37.0

图7 (a)不同Mn/Ce掺杂比例样品的O2-TPD谱图；(b)Ce掺杂前后样品的EPR谱图；(c)不同Mn/Ce掺杂比例样品的Cu 2p轨道的XPS精细谱

Fig.7 (a) O2-TPD spectra of samples with different Mn/Ce doping ratios; (b) EPR spectra of samples before and after Ce doping; (c) XPS spectra of Cu 2p orbitals of samples with different Mn/Ce doping ratios

图8 (a)Mn掺杂对O2吸附能的强化；(b)O2吸附在Cu-O与Cu-Mn-O上的PDOS分析

Fig.8 (a) Enhancement of O2 adsorption energy by Mn doping; (b) PDOS analysis of O2 adsorption on Cu-O and Cu-Mn-O

表3 不同Mn/Ce掺杂比例样品的Cu物种含量分布

Table 3 Distribution of Cu species content in samples with different Mn/Ce doping ratios

样品	含量/%
样品	Cu⁺	Cu²⁺
4Cu-4Ce	9.0	91.0
4Cu-4Mn	16.9	83.1
4Cu-3Mn-1Ce	14.7	85.3

图9 4Cu-3Mn-1Ce在450℃富氧（3%甲烷、21% O2、余N2）与缺氧（3%甲烷、余N2）氛围反应的in situ FTIR谱图

Fig.9 In situ FTIR spectra of 4Cu-3Mn-1Ce reacting in an oxygen-rich atmosphere (3% methane, 21% O2, remainder N2) and an oxygen-deficient atmosphere (3% methane, remainder N2) at 450℃

图10 Cu-Mn-Ce催化剂表面CH4催化燃烧强化机制

Fig.10 Enhanced mechanism of CH4 catalytic combustion on the surface of Cu-Mn-Ce catalysts

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Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究

Mechanistic study of Mn/Ce co-doping for enhanced oxygen species conversion and catalytic combustion of dilute methane

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