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化学进展 2021, Vol. 33 Issue (12): 2203-2214 DOI: 10.7536/PC201022 前一篇   后一篇

• 综述 •

催化氧化脱除二甲苯的催化剂

李肖静1,2,3, 李永红1,2,3,*(), 宇富航1,2,3, 祁伟岩1,2,3, 姜野1,2,3, 鲁倩文1,2,3   

  1. 1 天津大学化工学院 绿色合成与转化教育部重点实验室 天津 300072
    2 精馏技术国家工程研究中心 天津 300072
    3 天津化学化工协同创新中心 天津 300072
  • 收稿日期:2020-10-19 修回日期:2020-12-23 出版日期:2021-03-04 发布日期:2021-03-04
  • 通讯作者: 李永红
Richhtml ( 118 ) 引用

Catalysts for Removal of Xylene by Catalytic Oxidation

Xiaojing Li1,2,3, Yonghong Li1,2,3(), Fuhang Yu1,2,3, Weiyan Qi1,2,3, Ye Jiang1,2,3, Qianwen Lu1,2,3   

  1. 1 Key Lab for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072, China
    2 National Engineering Research Center for Distillation Technology,Tianjin 300072, China
    3 Collaborative Innovation Center of Chemical Science and Engineering (Tianjin),Tianjin 300072, China
  • Received:2020-10-19 Revised:2020-12-23 Online:2021-03-04 Published:2021-03-04
  • Contact: Yonghong Li

二甲苯是一种有毒挥发性有机化合物(Volatile organic compounds, VOCs),也是常见的工业污染物之一。催化氧化法可将二甲苯分解成CO2和H2O,有效防止有害气体排放到大气中。催化氧化法脱除二甲苯的关键是催化剂的低温活性和反应稳定性。本文从催化剂的制备方法、构效关系、活性组分之间及其与载体相互作用机制对催化性能的影响等方面,介绍了负载型贵金属催化剂、非贵金属氧化物和钙钛矿型氧化物催化剂用于二甲苯低温氧化的研究进展;比较分析了不同催化剂类型对二甲苯及其他种类VOCs的催化效果的偏向性;介绍了含二甲苯的混合VOCs的研究状况,并对未来催化剂研究的有关问题提出了建议。

关键词： 挥发性有机化合物, 二甲苯, 催化氧化, 催化剂, 钙钛矿

Xylene is a toxic volatile organic compound (VOC) and one of the common industrial pollutants. Catalytic oxidation can decompose xylene into CO2 and H2O, effectively preventing harmful gases from being emitted into the atmosphere. The key to the removal of xylene by catalytic oxidation is the low temperature activity and reaction stability of the catalyst. This article introduces the research progress in low-temperature oxidation of xylene with effects of supported noble metal catalysts, non-noble metal oxides and perovskite-type oxide catalysts from the aspects of catalyst preparation methods, structure-activity relationship, interaction between active components and the interaction mechanism with the supports on the catalytic performance. In addition, the catalytic effects on xylene and other VOCs of different catalyst types are compared and analyzed. Finally, the research results of mixed VOCs containing xylene are introduced and suggestions are made on the related issues of future catalyst research.

Contents

1 Introduction

2 Supported noble metal catalyst

2.1 Catalysts with inert carriers

2.2 Catalysts with active carriers

2.3 Catalysts with zeolite carriers

3 Metal oxide catalyst

3.1 Manganese-based catalysts

3.2 Cerium-based catalysts

3.3 Cobalt-based catalysts

3.4 Mixed-metal catalysts

3.5 Perovskite catalysts

4 Catalytic oxidation of VOCs mixtures containing xylene

5 Conclusion and outlook

Key words: volatile organic compounds, xylene, catalytic oxidation, catalyst, perovskite
()
图1 邻二甲苯在不同催化剂作用下的转化率随温度的变化(PdO/MOx表示未被处理的催化剂,MOx-H2和MOx-NaBH4分别表示不同的预处理方式,实验在10 vol%水蒸气含量条件下进行)[31]
Fig.1 Conversions of o-xylene as a function of temperature over PdO/MOx.(Pd/MOx-H2 and Pd/MOx-NaBH4 catalysts in the condition of 10 vol% water vapor addition)[31]
表1 部分贵金属催化剂制备方法与催化氧化邻二甲苯活化能的对比
Table 1 Comparison of the preparation method of some metal oxide catalysts and the activation energy of catalytic oxidation to o-xylene
Catalyst Preparation method Ea(VOC)/(kJ·mol-1) ref
meso-CoO a nanocasting strategy and PVA-protected reduction route 112.7 ± 5.1 30
Pd/meso-CoO 74.1 ± 3.4
meso-Co3O4 126.7 ± 4.5
Pd/meso-Co3O4 79.4 ± 3.7
Ag/NiOx-MnO2 redox and deposition-precipitation methods 21 32
NiOx-MnO2 33
OMS-2 68
Au-Pd/3DOM Mn2O3 PVA-protected reduction and the gas bubble-assisted adsorption strategies 71.7 34
Au-Pd-0.19Cr/3DOM Mn2O3 77.1
Au-Pd-0.21Mn/3DOM Mn2O3 65.3
Au-Pd-0.22Fe/3DOM Mn2O3 58.2
Au-Pd-0.21Co/3DOM Mn2O3 69.3
Ru/m-HZ(1) post-steaming treatment method and subsequent wetness impregnation method 149 36
Ru/m-HZ(2) 100
Ru/m-HZ(3) 74
图2 meso-Mn2O3转变为meso-γ-MnO2的过程[42]
Fig.2 Schematic Illustration of Transformation Process from meso-Mn2O3 to meso-γ-MnO2[42]
图3 邻二甲苯氧化速率与O2浓度的关系曲线(反应速率在230 ℃下测量,O2的浓度在5 vol%~30 vol%,邻二甲苯的浓度为200 ppm,通过改变空速将邻二甲苯转化率调节至低于15%)[49]
Fig.3 Rates of o-xylene oxidation as a function of O2 overCeO2 nanocubes. (The reaction rates were measured at 230 ℃. The concentration of O2 was varied in the range of 5~30 vol% and the concentration of o-xylene was 200 ppm. The o-xylene conversion was adjusted to below 15% by varying the space velocity)[49]
图4 三种催化剂上的CO2收率随温度的变化曲线图(邻二甲苯浓度为500 ppm,20% O2/N2作平衡气,气体流速50 mL·min-1,W/F = 0.60 g·s·mL-1)[65]
Fig.4 CO2 yield over the catalysts. Reaction conditions: o-xylene 500 ppm, 20% O2/N2 balance, total flow rate 50 mL·min-1, W/F = 0.60 g· s· mL-1 [65]
表2 部分金属氧化物催化剂制备方法及催化氧化二甲苯活化能的对比
Table 2 Comparison of the preparation method of some metal oxide catalysts and the activation energy of catalytic oxidation to o-xylene
Catalyst Preparation method Ea(VOC)/(kJ·mol-1) Ea(CO2)/(kJ·mol-1)a ref
3MnOx-CeOy hydrolysis driving redox 59 103.1 64
2.6Co3O4-MnO2 the polymethyl methacrylate microspheres-templating, incipient wetness impregnation, and acid treatment methods 80 - 66
8.8Co3O4-MnO2 72 -
13.3Co3O4-MnO2 82 -
8.5Co3O4-MnO2 78 -
MnO2 98 -
Co3O4 102 -
MnCo2O4 81 -
γ-MnO2/SmMnO3 one-step calcination and in situ fabrication 87.3 143.9 80
La2NiO4/Co3O4/cordierite two-step combination method of
hydrothermal synthesis and impregnation		 21.57 - 81
LaMnO3.15/Co3O4/cordierite 48.33 -
LaCoO3/Co3O4/cordierite 45.73 -
表3 部分金属氧化物对二甲苯的催化氧化研究对比
Table 3 Comparison of catalytic oxidation of some mixed metal oxides to xylene
Catalyst VOC type content(ppm) SV(h-1) T90(℃) ref
CoCeOx o-xylene 500 34 500 <275 59
3MnOx-CeOy o-xylene 1000 60 000 268 66
Ag/OMS-2 o-xylene 500 6000 <190 80
Cu/OMS-2 o-xylene 500 6000 <195
8.8Co3O4-MnO2 o-xylene 1000 10 000 mL/g 273 66
13.3Co3O4-MnO2 296
8.5Co3O4-MnO2 284
MnO2 297
Co3O4 308
MnCo2O4 295
MnCeCuOx/monolith o-xylene
1000
10 000		 277 67
MnCeCoOx/monolith 325
MnCeNiOx/monolith 308
Mn-Ce o-xylene 700 8000 <240 68
Mn/OMS-2 o-xylene 500 8000 <190 69
CuO-CeO2 xylene 10 000 66 000 <220 70
Fe0/Cu2O-zeolite o-xylene 4.97a 31.33b 360 71
p-xylene 10.30a 64.87b 340
m-xylene 6.95a 43.77b 350
表4 不同催化剂类型对二甲苯及其他VOCs的效果比较
Table 4 Comparison of catalytic oxidation effects of xylene and other VOCs on different catalyst types
Catalyst Catalytic activity sequence ref
1 wt% Pd/γ-Al2O3 o-xylene>toluene>benzene 11
Pt/CNT o-xylene>ethylbenzene>toluene>benzene 14
Pt/HRM hexane>toluene>o-xylene>benzene 22
Ru/HZSM-5 toluene≈o-xylene>TMB 36

Au-Pd/α-MnO2		 toluene≈m-xylene(mixed) 37
m-xylene>acetone(mixed)
m-xylene>ethyl-acetate(mixed)
MnOx xylene>ethylbenzene>toluene>benzene 44
Mn/Al benzene>toluene>o-xylene 4
CeOy/MnOx benzene>toluene>o-xylene 64
CuO-CeO2 ethylbenzene>xylene>toluene>benzene 70
SmMnO3 toluene>benzene>o-xylene 77
γ-MnO2/SmMnO3 toluene>ethylbenzene>benzene>o-xylene 80
0.96(AuPd1.92)/Co3O4 toluene≈o-xylene 82
CuO/Mn2O3 toluene>benzene>ethylbenzene>p-xylene>m-xylene>o-xylene 83
Au/Co3O4 toluene>o-xylene 84
CuO-CeO2/NaX o-xylene>toluene>benzene 85
Au-Pd-0.22Fe/3DOM Mn2O3 o-xylene>methane 88
Au-Pd-0.2Co/3DOM Mn2O3 methane>o-xylene
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