Research progress of low temperature catalytic oxidation of VOCs by metal oxides

doi:10.16085/j.issn.1000-6613.2022-1312

Abstract

Abstract:

Metal oxide catalysts with strong oxidation activity and high resistance are hot research topics in catalytic removal of volatile organic compounds (VOCs). In this paper, the effects of preparation factors such as composition ratio, morphology, calcination temperature, preparation method and carrier on catalytic VOCs oxidation activity and carbon dioxide selectivity was compared and analyzed from the perspectives of oxygen vacancies, active oxygen species, structure and crystalline surface. The poisoning mechanism of water vapor, nitrogen oxides and sulfur dioxide during the oxidation reactions in the actual working conditions was elaborated. The action mechanism of oxygen vacancies, lattice oxygen and surface adsorbed oxygen explored in depth by DFT calculations was prospected, and some key factors such as active component dispersion, high active crystalline surface ratio and oxygen vacancy strength can be considered in the optimization of catalysts. This review has provided scientific reference for the research and development of related catalytic systems.

Key words: activity, resistance, metal oxide, volatile organic compounds, catalytic oxidation, carbon dioxide, selectivity

摘要：

一直以来，开发强氧化活性和高抗性的金属氧化物催化剂都是催化脱除挥发性有机化合物（VOCs）领域的研究热点。本文从氧空位、活性氧物种、结构和晶面等角度，比较分析了催化剂的组成比例、形貌、焙烧温度、制备方法和载体等制备因素对增强催化氧化VOCs活性和二氧化碳选择性的影响。阐述了实际工况中的水蒸气、氮氧化物和二氧化硫在氧化反应过程中的中毒机制。展望了利用DFT计算，深入探索氧空位、晶格氧和表面吸附氧在VOCs催化氧化过程中的作用机理，并从活性组分分散度、高活性晶面占比、氧空位强度等关键方面来指导优化催化剂，为相关催化体系的研发提供了科学参考。

关键词: 活性, 抗性, 金属氧化物, 挥发性有机化合物, 催化氧化, 二氧化碳, 选择性

CLC Number:

X511

WANG Keju, ZHAO Cheng, HU Xiaomei, YUN Junge, WEI Ninghan, JIANG Xueying, ZOU Yun, CHEN Zhihang. Research progress of low temperature catalytic oxidation of VOCs by metal oxides[J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2402-2412.

王科菊, 赵成, 胡晓玫, 云军阁, 魏凝涵, 姜雪迎, 邹昀, 陈志航. 金属氧化物低温催化氧化VOCs的研究进展[J]. 化工进展, 2023, 42(5): 2402-2412.

Figures/Tables 11

催化剂	污染物	浓度/μL·L^-1	空速/mL∙g^-1∙h^-1	T₉₀/℃	O_ads/O_latt	参考文献
MnO₂	甲苯	1000	40000	228	0.78	[26]
Co-MnO₂	甲苯	1000	40000	227	0.86	[26]
Ce-MnO₂	甲苯	1000	40000	234	0.57	[26]
Cu-MnO₂	甲苯	1000	40000	219	1.07	[26]
Co₃O₄	甲苯	1000	78000	249	0.88	[27]
CuCo₂O₄	甲苯	1000	78000	221	1.12	[27]
NiCo₂O₄	甲苯	1000	78000	234	1.07	[27]
ZnCo₂O₄	甲苯	1000	78000	279	0.80	[27]

催化剂	金属比例	污染物	浓度 /μL·L^-1	空速 /mL∙g^-1∙h^-1	T₉₀/℃	参考文献
CuMnO _x	Cu/Mn=0∶1	甲苯	500	22500	229	[30]
CuMnO _x	Cu/Mn=0.06∶1	甲苯	500	22500	226	[30]
CuMnO _x	Cu/Mn=0.08∶1	甲苯	500	22500	225	[30]
CuMnO _x	Cu/Mn=0.10∶1	甲苯	500	22500	216	[30]
CuMnO _x	Cu/Mn=0.12∶1	甲苯	500	22500	223	[30]
MnCoO _x	Mn/Co=0∶1	甲苯	1000	40000	246	[31]
MnCoO _x	Mn/Co=0.2∶0.8	甲苯	1000	40000	227	[31]
MnCoO _x	Mn/Co=0.3∶0.7	甲苯	1000	40000	220	[31]
MnCoO _x	Mn/Co=0.4∶0.6	甲苯	1000	40000	215	[31]
MnCoO _x	Mn/Co=0.5∶0.5	甲苯	1000	40000	219	[31]
FeMnO _x	Fe/Mn=0∶1	氯苯	600	20000^①	310	[33]
FeMnO _x	Fe/Mn=1∶8	氯苯	600	20000^①	340	[33]
FeMnO _x	Fe/Mn=1∶1	氯苯	600	20000^①	197	[33]
FeMnO _x	Fe/Mn=2∶1	氯苯	600	20000^①	295	[33]
FeMnO _x	Fe/Mn=1∶0	氯苯	600	20000^①	>400	[33]

催化剂	焙烧温度 /℃	污染物	浓度 /μL·L^-1	空速 /mL∙g^-1∙h^-1	T₉₀/℃	I_D/I_2g	参考文献
Co₃O₄	300	甲苯	1000	40000	240	—	[34]
Co₃O₄	350	甲苯	1000	40000	251	—	[34]
Co₃O₄	400	甲苯	1000	40000	260	—	[34]
Fe₁Mn₄	300	甲苯	500	100000	—	0.93	[35]
Fe₁Mn₄	400	甲苯	500	100000	—	0.91	[35]
Fe₁Mn₄	500	甲苯	500	100000	—	0.87	[35]
Cu₁Co₂Fe₁O _x	400	甲苯	800	60000	238	—	[36]
Cu₁Co₂Fe₁O _x	500	甲苯	800	60000	246	—	[36]
Cu₁Co₂Fe₁O _x	600	甲苯	800	60000	289	—	[36]
Cu₁Co₂Fe₁O _x	700	甲苯	800	60000	322	—	[36]

催化剂	制备方法	污染物	浓度 /μL·L^-1	空速 /mL∙g^-1∙h^-1	T₉₀ /℃	参考文献
CeO₂-M	原位热解法	甲苯	1000	20000	223	[38]
CeO₂-P	沉淀法	甲苯	1000	20000	280	[38]
CeMn-IM	浸渍法	甲苯	500	60000^①	261	[39]
CeMn-CP	共沉淀法	甲苯	500	60000^①	259	[39]
CeMn-SG	溶胶凝胶法	甲苯	500	60000^①	249	[39]
CeMn-HT	水热法	甲苯	500	60000^①	246	[39]
MnCu_0.5	水热氧化还原法	甲苯	1000	40000	210	[40]
MnCu_0.75-H₂O₂	氧化还原沉淀法	甲苯	1000	40000	236	[40]
MnCu_0.75-P	共沉淀法	甲苯	1000	40000	240	[40]
Cu_0.4Ce_0.6-DR	双氧化还原法	甲苯	500	50000	约246	[41]
Cu_0.4Ce_0.6-C	共沉淀法	甲苯	500	50000	约270	[41]

催化剂	载体	污染物	浓度/μL·L^-1	空速/mL∙g^-1∙h^-1	T₉₀/℃	参考文献
MnO _x /HZ-5	纳米中空HZSM-5	甲苯	1000	15000	255	[42]
MnO _x /MZ-5	微米HZSM-5	甲苯	1000	15000	282	[42]
Co₃O₄	—	丙烷	—	80000	>400	[43]
Co₃O₄/ZSM-5	ZSM-5	丙烷	—	80000	360	[43]
Co₃O₄/Silicalite-1	Silicalite-1	二氯甲烷	1000	30000	420	[44]
Co₃O₄/ZSM-5	ZSM-5	二氯甲烷	1000	30000	370	[44]
Co₃O₄/TS-1	TS-1	二氯甲烷	1000	30000	406	[44]
Mn/Ce-Zr(C-T-1)	界面CeO₂-ZrO₂	甲苯	1000	30000	254	[45]
Mn/Ce-Zr-ss	简单CeO₂-ZrO₂	甲苯	1000	30000	288	[45]
Co₃O₄/TiO₂	TiO₂	甲苯	1000	60000	377	[46]
Co₃O₄/YSZ	YSZ	甲苯	1000	60000	280	[46]
Co₃O₄	—	甲苯	1000	60000	312	[46]

催化剂	形貌	污染物	浓度 /μL·L^-1	空速 /mL∙g^-1∙h^-1	T₉₀ /℃	参考文献
CeO₂-S	球形	苯乙烯	600	15000	184	[47]
CeO₂-R	棒状	苯乙烯	600	15000	219	[47]
CeO₂-O	八面体	苯乙烯	600	15000	221	[47]
CeO₂-C	立方体	苯乙烯	600	15000	>350	[47]
Co₃O₄-R	棒状	邻二甲苯	100	120000	270	[48]
Co₃O₄-S	球形	邻二甲苯	100	120000	295	[48]
MnO₂-PS	多孔纳米片	丙烷	2000	30000	235	[49]
MnO₂-R	棒状	丙烷	2000	30000	295	[49]
MnO₂-B	块状	丙烷	2000	30000	318	[49]
Ce₁Mn₂	核壳结构	甲苯	1000	60000	245	[50]
CeO₂	—	甲苯	1000	60000	315	[50]
MnO₂	—	甲苯	1000	60000	290	[50]
CeO₂@Co₃O₄	核壳结构	甲苯	2000	20000	225	[51]
CeO₂	—	甲苯	2000	20000	>300	[51]
Co₃O₄	—	甲苯	2000	20000	285	[51]

催化剂	甲苯浓度/μL·L^-1	NO _x 浓度/μL·L^-1	空速/mL∙g^-1∙h^-1	甲苯转化温度(未引入NO _x )/℃	甲苯转化温度(引入NO _x )/℃	参考文献
Mn/CeO₂	100	500	10000	T₈₀=215	T₈₀=226	[58]
Mn/TiO₂	100	500	10000	T₈₀=239	T₈₀=247	[58]
Mn₂Cu₁Al₁O _x	800	100	60000^①	T₁₀₀=250	T₉₄=250	[59]
MnO _x -CeO₂	50	500	60000	T₄₇=150	T₂₆=150	[60]
CuCeAl _x	1000	600	50000^①	T₉₀≈300	T₉₀≈250	[61]

催化剂	(O_α/O)/%	ΔO_α/%	(V⁵⁺/V)/%	(SO $4 2 -$ /S)/%
V-Cu/ZSM-5	48.86	—	72.25	—
Cu/ZSM-5	38.95	—	—	—
V-Cu/ZSM-5-使用后	53.17	4.31	63.32	52.36
Cu/ZSM-5-使用后	58.89	19.94	—	64.55

催化剂	(O_α/O)/%	ΔO_α/%	(V⁵⁺/V)/%	(SO $4 2 -$ /S)/%
V-Cu/ZSM-5	48.86	—	72.25	—
Cu/ZSM-5	38.95	—	—	—
V-Cu/ZSM-5-使用后	53.17	4.31	63.32	52.36
Cu/ZSM-5-使用后	58.89	19.94	—	64.55

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