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化学进展 2021, Vol. 33 Issue (7): 1188-1200 DOI: 10.7536/PC200716 前一篇   后一篇

• 综述 •

室温催化分解空气中臭氧污染物

李连欣1, 曹冉冉1, 张彭义1,2,*()   

  1. 1 清华大学环境学院 环境模拟与污染控制国家重点实验室 北京 100084
    2 室内空气质量评价与控制北京市重点实验室 北京 100084
  • 收稿日期:2020-07-09 修回日期:2020-11-05 出版日期:2021-07-20 发布日期:2020-12-28
  • 通讯作者: 张彭义
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Catalytic Decomposition of Gaseous Ozone at Room Temperature

Lianxin Li1, Ranran Cao1, Pengyi Zhang1,2,*()   

  1. 1 State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
    2 Beijing Key Laboratory for Indoor Air Quality Evaluation and Control, Beijing 100084, China
  • Received:2020-07-09 Revised:2020-11-05 Online:2021-07-20 Published:2020-12-28
  • Contact: Pengyi Zhang
  • About author:
    * Corresponding anthor e-mail:

臭氧污染是我国目前面临的突出环境问题,臭氧及其室内反应形成的二次污染物危害着人体健康。室温催化分解是避免空气臭氧污染的有效方法,本文首先总结了碳、沸石、贵金属与过渡金属氧化物等材料的臭氧催化分解性能;然后聚焦锰氧化物,比较分析了不同锰氧化物的臭氧催化活性,阐述了锰氧化物催化分解臭氧机理的研究进展。水蒸气导致的失活是当前臭氧催化剂研发面临的主要挑战,对臭氧催化分解与失活机理的深入认识是指导高效抗湿臭氧催化材料研发的关键。

关键词： 臭氧, 催化分解, 锰氧化物, 二氧化锰

Ozone pollution is a serious problem now prevailing in China. Ozone and its secondary pollutants generated indoor severely threaten human health. The catalytic decomposition of ozone at room temperature is an effective way to prevent the pollution. This review firstly summarizes the catalytic activity of carbon, zeolite, noble metal, transitional metal oxides and other materials; then focuses on manganese oxides, compares the activity of manganese oxides with different crystal structures and elaborates the research progress in mechanisms of ozone decomposition on manganese oxides. Currently, the major challenge in this field is the catalyst deactivation caused by water vapor. The comprehensive understanding in mechanisms of ozone decomposition and catalyst deactivation is the essential key to synthesize efficient catalysts.

Contents

1 Introduction

2 Catalysts for ozone decomposition

2.1 Carbon

2.2 Noble metal

2.3 Transitional metal oxides

2.4 Other materials

3 Manganese oxides for ozone decomposition

3.1 α-MnO 2

3.2 γ-MnO 2, ε-MnO 2, ramsdellite and todorokite

3.3 δ-MnO 2

3.4 Amorphous and low-valent manganese oxides

4 Mechanisms of catalytic decomposition of ozone on manganese oxides

4.1 Mechanisms of ozone decomposition

4.2 Mechanisms of catalyst deactivation

4.3 Regeneration and heat treatment of catalyst

5 Conclusion and outlook

Key words: ozone, catalytic decomposition, manganese oxides, manganese dioxide
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表1 α-MnO2类臭氧催化材料的制备方法与臭氧催化性能
Table 1 The synthetic methods and the catalytic performance of α-MnO 2
Year Sample Synthetic method Test conditions Ozone conversion (%) ref
Temperature
( ℃)		 Inlet O3
(ppm)		 Space velocity
(L·g-1·h-1)		 Relative humidity (%) Duration (h)
2015 OMS-2-Ac Hydrothermal method 30 40 600 90 6 75 66
2016 α-MnO2 Hydrothermal method 25 100 540 50 10 36 62
2017 α-MnO2 Hydrothermal and
vacuum method		 25 20 540 50 10 44 71
2017 Ce-OMS-2 Hydrothermal method 25 40 600 90 6 90 67
2018 W-MnO2-0.06 Hydrothermal method 25 120 660 65 4 50 64
2019 V-MnO2-0.15 Hydrothermal method 25 110 600 55 6 50 65
2019 Na-OMS-2 Hydrothermal method, rotary evaporation and calcination 25 45 660 30 6 92 73
2019 Ce-OMS-2 Hydrothermal method 30 40 600 90 6 93 68
2020 Ce-OMS-2-80% Hydrothermal method 30 40 600 45 6 97 70
表2 其他隧道结构二氧化锰的制备方法与臭氧催化性能
Table 2 The synthetic methods and the catalytic performance of MnO2 with other tunnel structures
Year Sample Synthetic method Test conditions Ozone conversion (%) ref
Temperature ( ℃) Inlet O3
(ppm)		 Space velocity
(L·g-1·h-1)		 Relative humidity (%) Duration (h)
2017 Fe-MnOx Hydrothermal method 25 100 660 60 6 73 74
2017 Ce-T-MnO2 Hydrothermal method Room temperature 55 1200 0 3 78 77
2017 Ce-T-MnO2 Hydrothermal method
and calcination		 25 115 1200 0 3 97 78
2018 Ce-γ-MnO2 Hydrothermal method
and calcination		 30 40 840 65 6 96 75
2020 C0.04(FM)0.96 Sol-gel method and calcination 25 21 480 65 6.5 63 76
2020 MnO2-H2 Selective dissolution of
Mn-Li precursor		 25 45 600 50 6 91 79
表3 δ-MnO2类臭氧催化材料的制备方法与臭氧催化性能
Table 3 The synthetic methods and catalytic performance of δ-MnO 2
Year Sample Synthetic method Test conditions Ozone conversion (%) ref
Temperature ( ℃) Inlet O3
(ppm)		 Space velocity
(L·g-1·h-1)		 Relative humidity (%) Duration (h)
2017 H-MnO2 Hydrothermal method,
calcination and acid treatment		 30 3000 600 0 10 100 80
2018 H-MnO2 Room temperature reaction and acid treatment 25 115 600 50 5 60 81
2019 N-MnO2 80 ℃ reaction and
ammonia treatment		 25 115 600 50 10 77 82
表4 无定形与低价态锰氧化物的制备方法与臭氧催化性能
Table 4 The synthetic methods and catalytic performance of amorphous and low-valent manganese oxides
Year Sample Synthetic method Test conditions Ozone conversion (%) ref
Temperature ( ℃) Inlet O3
(ppm)		 Space velocity
(L·g-1·h-1)		 Relative humidity (%) Duration (h)
2015 MnFe0.5Ox-NO3 Hydrothermal method
and calcination		 25 10 000 12 90 8 90 85
2018 MnOx-I Room-temperature reaction 25 40 600 50 10 93 83
2019 MnO2-300 Room-temperature reaction
and calcination		 25 40 600 50 10 98 87
2019 Mn3O4/CNTs 70 ℃ reaction and calcination 25 40 600 50 20 100 84
2019 8%AgMnOx Room-temperature reaction
and calcination		 30 40 840 65 6 81 40
2020 Ce-MnOx-2 Room-temperature reaction 25 100 540 50 10 100 86
2020 CeMn10Ox 90 ℃ reaction and calcination 30 40 840 65 6 96 88
图1 酸性位与氧空位共同参与的锰氧化物臭氧分解机理[81]
Fig. 1 The mechanism of ozone decomposition involving acid sites and oxygen vacancies[81]. Copyright 2018, Elsevier
图2 基于稳定氧物种中间产物的锰氧化物臭氧催化失活机理[73]
Fig. 2 The mechanism of catalyst deactivation during ozone decomposition on manganese oxides based on the stable oxygen intermediates[73]. Copyright 2019, ACS Publications
图3 基于Mn-OH的锰氧化物臭氧催化失活机理[78]
Fig. 3 The mechanism of catalyst deactivation during ozone decomposition on manganese oxides based on Mn-OH[78]. Copyright 2017, ACS Publications
表5 锰氧化物臭氧催化材料的再生条件与再生效果
Table 5 The regeneration effect of manganese oxides for ozone decomposition
Year Sample Synthetic method Regeneration conditions Regeneration effect ref
Atmosphere Temperature ( ℃) Duration (h)
2005 MnOx/Al2O3 Impregnation and calcination O2 450 3 Mn AOS* recovered 90
2017 Ce-MnO2(200) Hydrothermal method
and calcination		 Air 200 3 Activity improved 78
2018 α-MnO2 (KOH-4h) Hydrothermal method Ar 400 2 Activity partly recovered 72
2019 Na-OMS-2 Hydrothermal method,
rotary evaporation
and calcination		 N2 425 0.5 Activity recovered 73
2020 C0.04(FM)0.96 Sol-gel method
and calcination		 Air 200 2 Activity recovered 76
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摘要

室温催化分解空气中臭氧污染物