新型Ce掺杂MnO<sub><i>x</i></sub>高效低温甲苯催化氧化性能

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Abstract Novel Ce-doped MnO_x bimetallic catalyst was successfully prepared by co-oxidation-precipitation method, and the influence of synergy between Ce and Mn was explored for catalytic toluene oxidation at low temperature. Characterizations by SEM、XRD、N₂ adsorption-desorption、XPS、EPR、H₂-TPR, and in situ DRIFTS were performed for the prepared catalysts. It is found that the catalysts with an optimum Ce/Mn molar ratios of 1:3 had a highest performance with T₅₀ of 215℃ and T₉₀ of 233℃, good durability and water resistance for the toluene oxidation. Meanwhile, the results confirmed that the introduction of Ce was beneficial to adjust the morphology of CeMn₃Ox catalyst with the formation of coral-structure, leading to the increase in the number of interfaces between crystalline-amorphous, which caused more defects and oxygen vacancies in the bulk of catalyst, promoting the conversion of O_latt↔ O_sur↔O_ads and enhancing the reducibility. Finally, in situ DRIFTS spectra verified that toluene oxidation followed two reaction pathways under air conditions,Ⅰ:adsorption→benzyl alcohol→benzaldehyde→benzoate→phenol→ benzene ring C=C breakage→ CO₂ and H₂O,Ⅱ: adsorption → benzene ring C=C cleavage breakage →Maleic anhydride→ CO₂ and H₂O, in which the C=C breakage of the aromatic ring was considered as a rate-controlled step.

Key words： toluene mixed Ce-Mn oxides oxygen vacancy catalytic mechanism

Received: 19 February 2024

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X511

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	Articles by authors
	. WANG Pei-fen
	AN Xiao-wei
	MA Xu-li
	GUAN Guo-qing
	HAO Xiao-gang

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. WANG Pei-fen,AN Xiao-wei,MA Xu-li等. Novel Ce-doped MnO_x catalysts for highly efficient catalysis of toluene oxidation at low temperature[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(9): 4853-4863.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I9/4853

[1] Wang P F, Wang J, An X W, et al. Generation of abundant defects in Mn-Co mixed oxides by a facile agar-gel method for highly efficient catalysis of total toluene oxidation [J]. Applied Catalysis B: Environmental, 2021,282:119560.
[2] 方宏萍,梁文俊,任思达,等.改性赤泥催化剂制备及其催化燃烧甲苯性能[J]. 中国环境科学, 2021,41:5764-5770. Fang H P, Liang W J, Ren S D, et al. Preparation of modified red mud-based catalysts and their catalytic combustion performance for toluene [J]. China Environmental Science, 2021,41:5764-5770.
[3] Wang P F, Wang J, Zhao J G, et al. Trace holmium assisting delaminated OMS-2catalysts for total toluene oxidation at low temperature [J]. Journal of Colloid and Interface Science, 2022,608: 1662-1675.
[4] 隋美君,柳志刚,杨晨,等.新型CoMn/SBA-15低温催化氧化甲苯性能[J]. 中国环境科学, 2023,43:3396-3403. Sui M J, Liu Z G, Yang C, et al. Novel CoMn/SBA-15 catalyst for highly efficient low-temperature catalytic oxidation of toluene [J]. China Environmental Science, 2022,608:1662-1675.
[5] Malhautier L, Quijano G, Avezac M, et al. Kinetic characterization of toluene biodegradation by Rhodococcus erythropolis: Towards a rationale for microflora enhancement in bioreactors devoted to air treatment [J]. Chemical Engineering Journal, 2014,247:199-204.
[6] Li L, Liu S, Liu J, et al. Surface modification of coconut shell based activated carbon for the improvement of hydrophobic VOC removal [J]. Journal of Hazardous Materials, 2011,192:683-90.
[7] Thevenet F, Sivachandiran L, Guaitella O, et al. Plasma–catalyst coupling for volatile organic compound removal and indoor air treatment: a review [J]. Journal of Physics D: Applied Physics, 2014, 47:224011.
[8] Chen L, Tang J, Song L N. et al. Heterogeneous photocatalysis for selective oxidation of alcohols and hydrocarbons [J]. Applied Catalysis B: Environmental, 2019,242:379-388.
[9] Wang P F, Ma X L, Hao X G, et al. Oxygen vacancy defect engineering to promote catalytic activity toward the oxidation of VOCs: a critical review [J]. Catalysis Reviews Science and Engineering, 2022,66(2):586-639.
[10] Huang H, Xu Y, Feng Q, et al. Low temperature catalytic oxidation of volatile organic compounds: A review [J]. Catalysis Science & Technology, 2015,5:2649-2669.
[11] Chen H L, Removal of volatile organic compounds by single-stage and two-stage plasma catalysis systems: a review of the performance enhancement mechanisms, current status, and suitable applications [J]. Environmental Science & Technology, 2009,43.
[12] Gonet T, Maher B. A, Airborne, Vehicle-derived Fe-bearing nanoparticles in the urban environment: A review [J]. Environmental Science and Technology, 2019,53:9970-9991.
[13] Liotta L F, Catalytic oxidation of volatile organic compounds on supported noble metals [J]. Applied Catalysis B: Environmental, 2010,100:403-412.
[14] Deng H, Kang S, Ma, J, et al. Role of structural defects in MnOx promoted by Ag doping in the catalytic combustion of volatile organic compounds and ambient decomposition of O₃[J]. Environmental Science and Technology, 2019,53:10871-10879.
[15] Yang W, Su Z A, Xu Z, et al. Comparative study of α-, β-, γ- and δ-MnO₂ on toluene oxidation: Oxygen vacancies and reaction intermediates [J]. Applied Catalysis B: Environmental, 2020,260: 118150.
[16] Xu H, Yan N, Qu Z, et al. Gaseous heterogeneous catalytic reactions over Mn-based oxides for environmental applications: A critical review [J]. Environmental Science and Technology, 2017,51:8879-8892.
[17] Trovarelli A, Llorca J, Ceria catalysts at nanoscale: How do crystal shapes shape catalysis? [J]. Acs Catalysis, 2017,7(7):4716–4735.
[18] Wang P F, Wang J, Shi J, et al., Low content of samarium doped CeO₂oxide catalysts derived from metal organic framework precursor for toluene oxidation [J]. Molecular Catalysis 2020,492:111027.
[19] Zhao L, Zhang Z, Li Y, et al. Synthesis of CeaMnOx hollow microsphere with hierarchical structure and its excellent catalytic performance for toluene combustion [J]. Applied Catalysis B: Environmental, 2019,245:502-512.
[20] Zhang C, Chen W, Li F, et al. Effects of cerium precursors on surface properties of mesoporous CeMnOx catalysts for toluene combustion [J]. Ecological restoration, 2020,38.
[21] Quiroz J, Giraudon J M, Gervasini A, et al., Total oxidation of formaldehyde over MnOx-CeO₂ catalysts: The effect of acid treatment [J]. ACS Catalysis, 2015,5:2260-2269.
[22] Jiang Y, Gao J, Zhang Q, et al. Enhanced oxygen vacancies to improve ethyl acetate oxidation over MnOx-CeO₂ catalyst derived from MOF template [J]. Chemical Engineering Journal, 2019,371:78-87.
[23] Wang J, Yoshida A, Wang P F, et al. Catalytic oxidation of volatile organic compound over cerium modified cobalt-based mixed oxide catalysts synthesized by electrodeposition method [J]. Applied Catalysis B: Environmental, 2020,271:118941.
[24] Li L, Liu Y, Deng J, et al. Pt/CeMnOx/Diatomite: A highly active catalyst for the oxidative removal of toluene and ethyl acetate [J]. Catalysts, 2023,13:676.
[25] Wang P F, Zhao J G, Zhao Q, et al. Microwave-assisted synthesis of manganese oxide catalysts for total toluene oxidation [J]. Journal of Colloid and Interface Science, 2022,607:100-110.
[26] Chen, X., Cai E Q, Jia S C, et al. In situ pyrolysis of Ce-MOF to prepare CeO₂catalyst with obviously improved catalytic performance for toluene combustion [J]. Chemical Engineering Journal, 2018,344: 469-479.
[27] Wang H L, Liu S, Zhao Z, et al. Activation and deactivation of Ag/CeO₂ during soot oxidation: Influences of interfacial ceria reduction [J]. Catalysis Science & Technology, 2017,7(10):2129-2139.
[28] Luo Y, Zheng Y, Zuo J, et al., Insights into the high performance of Mn-Co oxides derived from metal-organic frameworks for total toluene oxidation [J]. Journal of Hazardous Materials, 2018,349:119-127.
[29] Dong C, Qu Z, Jiang X, et al. Tuning oxygen vacancy concentration of MnO₂ through metal doping for improved toluene oxidation [J]. Journal of Hazardous Materials, 2020,391:122181.
[30] Zhang X, Zhao H, Song Z, et al. Insight into the effect of oxygen species and Mn chemical valence over MnO on the catalytic oxidation of toluene [J]. Applied Surface Science, 2019,493:9-17.
[31] Wang Q, Wang W, Zhong L, et al. Oxygen vacancy-rich 2D/2D BiOCl-g-C₃N₄ ultrathin heterostructure nanosheets for enhanced visible-light-driven photocatalytic activity in environmental remediation [J]. Applied Catalysis B: Environmental, 2018,220: 290-302.
[32] Rao K T V, Rogers J L, Souzanchi S, et al. Inexpensive but highly efficient Co-Mn mixed-oxide catalysts for selective oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid [J]. ChemSusChem, 2018,11:3323-3334.
[33] Hernández A M D, Tejedor T I, Coronado J M, et al. Operando FTIR study of the photocatalytic oxidation of methylcyclohexane and toluene in air over TiO₂–ZrO₂ thin films: Influence of the aromaticity of the target molecule on deactivation [J]. Applied Catalysis B: Environmental, 2011,101:283-293.
[34] Li J J, Yu E Q, Cai S C, et al. Noble metal free, CeO₂/LaMnO₃ hybrid achieving efficient photo-thermal catalytic decomposition of volatile organic compounds under IR light [J]. Applied Catalysis B: Environmental, 2019,240:141-152.
[35] Chen X, Chen X, Yu E, et al. In situ pyrolysis of Ce-MOF to prepare CeO₂ catalyst with obviously improved catalytic performance for toluene combustion [J]. Chemical Engineering Journal 2018,344:469-479.
[36] Bongiorno A, Landman U, Water-enhanced catalysis of CO oxidation on free and supported gold nanoclusters [J]. Physical Review Letters, 2005,95(10).
[37] Li J, Na H, Zeng X, et al. In situ DRIFTS investigation for the oxidation of toluene by ozone over Mn/HZSM-5, Ag/HZSM-5 and Mn–Ag/HZSM-5catalysts [J]. Applied Surface Science, 2014,311: 690-696.
[38] Rainone F, Bulushev D A, Kiwi M L, et al. DRIFTS and transient-response study of vanadia/titania catalysts during toluene partial oxidation [J]. Physical Chemistry Chemical Physics, 2003,5:4445-4449.
[39] Mo S, Zhang Q, Li J, et al. Highly efficient mesoporous MnO₂ catalysts for the total toluene oxidation: Oxygen-Vacancy defect engineering and involved intermediates using in situ DRIFTS [J]. Applied Catalysis B: Environmental, 2020,264:118464.
[40] Zhang H, Zhu F, Li X, et al. Steam reforming of toluene and naphthalene as tar surrogate in a gliding arc discharge reactor [J]. Journal of Hazardous Materials, 2019,369:244-253.
[41] Wang Y, Wang F, Song Q, et al. Heterogeneous ceria catalyst with water-tolerant Lewis acidic sites for one-pot synthesis of 1,3-diols via Prins condensation and hydrolysis reactions [J]. Journal of the American Chemical Society, 2013,135:1506-15.