挥发性有机化合物催化消除前沿技术及研究进展

doi:10.16085/j.issn.1000-6613.2021-2334

摘要/Abstract

摘要：

挥发性有机化合物（VOCs）是可吸入有害物质形成的重要前体，是大气污染物的重要组成部分。催化氧化法作为末端技术是目前处理VOCs最有效的途径之一。本文讨论了VOCs的热催化氧化、光催化氧化和光热协同催化氧化的研究进展，重点研究常用VOCs的催化氧化机理以及相关催化剂的构筑。其中，热催化燃烧主要以贵金属（Pt、Pd、Au、Ag等）、过渡金属（Mn、Co、Cr等氧化物）及复合型催化剂研究展开；光催化氧化以TiO₂和C₃N₄为典型催化剂进行讨论；光热协同催化研究主要包括碳基催化剂、贵金属负载型以及过渡金属负载型催化剂的开发与应用。此外，本文对基于催化剂的热催化、光催化和光热催化去除VOCs的开发和研究提出了进一步的展望。

关键词: 挥发性有机化合物, 热催化, 光催化, 光热协同催化, 催化剂

Abstract:

Volatile organic compounds (VOCs) are important precursors of inhalable harmful substances and have caused serious air pollution. Catalytic degradation of VOCs is currently one of the most effective end-treatment technologies to control air pollution. The manuscript discusses the research progress of thermal catalytic oxidation, photocatalytic oxidation, and photothermal synergistic catalytic oxidation of the VOCs, focusing on the mechanism of catalytic oxidation of common VOCs and the design of related catalysts. Among them, thermal catalytic combustion researches mainly focuses on noble metal-based catalysts (Pt, Pd, Au, Ag, etc.), transition metal catalysts (oxidation state of Mn, Co, Cr, etc.), and composite catalysts. Photocatalytic oxidation catalysts are discussed by using TiO₂ and C₃N₄ as the typical catalysts, while the research of photothermal synergistic catalysis mainly included carbon-based catalysts, noble metal-supported catalysts and transition metal-supported catalysts. In addition, further prospects for the development and research of thermal catalysis, photocatalysis, and photothermal catalysis for the elimination of VOCs are given.

Key words: volatile organic compounds, thermocatalysis, photocatalysis, photothermal co-catalysis, catalysts

中图分类号:

TQ09

杨福, 刘梦婷, 马淑兰, 魏祎暄, 欧锐, 王旭裕, 李露露, 张武翔, 潘建明. 挥发性有机化合物催化消除前沿技术及研究进展[J]. 化工进展, 2022, 41(9): 4801-4812.

YANG Fu, LIU Mengting, MA Shulan, WEI Yixuan, OU Rui, WANG Xuyu, LI Lulu, ZHANG Wuxiang, PAN Jianming. Advanced in catalytic elimination of volatile organic compounds[J]. Chemical Industry and Engineering Progress, 2022, 41(9): 4801-4812.

图/表 16

图1 Langmuir-Hinshelwood反应机理

图2 不同 Pt 负载量催化剂的甲苯催化活性[10]

表1 MO x 载体和Pt-Fe/MO x 催化剂的物化性能[11]

催化剂	Pt质量分数/%		比表面积 /m²·g^-1	孔容 /m³·g^-1	孔直径 /nm
催化剂	理论	实际	比表面积 /m²·g^-1	孔容 /m³·g^-1	孔直径 /nm
γ-Al₂O₃			170	0.23	6.0
TiO₂			51	0.18	16.4
Co₃O₄			48	0.36	19.1
Ni₂O₃			37	0.26	16.9
Pt-Fe/Al₂O₃	2	1.48	103	0.17	6.6
Pt-Fe/TiO₂	2	1.51	40	0.13	17.2
Pt-Fe/Co₃O₄	2	1.42	43	0.23	18.9
Pt-Fe/Ni₂O₃	2	1.36	21	0.10	11.8

图3 干燥条件下Pt-Fe/MeO x 催化剂氧化HCHO的催化活性[11]

图4 Pd/γ-Al2O3和Pd/CeO2/γ-Al2O3催化剂催化氧化甲苯[20]

图5 不同Ag/CNTs催化剂的HCHO催化性能[29]a—浸渍法；b—甘油还原法；c—二甲基亚砜还原法；d—商业碳纳米管；e—经HNO3处理的CNTs

图6 Mars-van Krevelen机理

表2 Mn基尖晶石催化剂甲苯催化降解性能[3]

催化剂	T₅₀/℃	T₉₀/℃	表观活化能/kJ·mol^-1
SmMnO₃	223	258	90.1
γ-MnO₂/SmMnO₃	187	192	55.0
Mn_3-_x Fe _x O₄	223	258

图7 不同Fe含量催化剂催化氧化甲苯的性能[3]

图8 紫外线照射下的TiO2光催化氧化VOCs过程[3]

图9 制备样品在空气中去除甲苯的可见光催化活性[43]

图10 TiO2负载型光热协同催化反应机理一[3]

图11 TiO2负载型光热协同催化反应机理二[3]

图12 Ag3PO4/Ag/SrTiO3光热催化VOCs氧化[58]

图13 甲苯的转化与时间的关系[55]

图14 催化剂在治理VOCs的应用

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