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化学进展 2019, Vol. 31 Issue (2/3): 311-321 DOI: 10.7536/PC180435 前一篇   后一篇

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用于甲醛催化氧化的锰基催化剂及协同效应的影响

刘喆1, 张晓岚1, 蔡婷1,2, 袁静2,3,**(), 赵昆峰2, 何丹农1,2,**()   

  1. 1. 上海交通大学材料科学与工程学院 上海 200240
    2. 纳米技术及应用国家工程研究中心 上海 200241
    3. 上海健康医学院 上海 201318
  • 收稿日期:2018-04-23 出版日期:2019-02-15 发布日期:2018-12-20
  • 通讯作者: 袁静, 何丹农
  • 基金资助:
    国家自然科学基金项目(21607098); 上海市青年科技启明星计划(17QB1402800)
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Catalytic Oxidation of Formaldehyde over Manganese-Based Catalysts and the Influence of Synergistic Effect

Zhe Liu1, Xiaolan Zhang1, Ting Cai1,2, Jing Yua2,3,**(), Kunfeng Zhao2, Dannong He1,2,**()   

  1. 1. School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
    2. National Engineering Research Center for Nanotechnology, Shanghai 200241, China
    3. Shanghai University of Medicine & Health Sciences, Shanghai 201318, China
  • Received:2018-04-23 Online:2019-02-15 Published:2018-12-20
  • Contact: Jing Yua, Dannong He
  • About author:
    ** E-mail: (Jing Yuan);
    (Dannong He)
  • Supported by:
    National Natural Science Foundation of China(21607098); Shanghai Youth Science and Technology Rising-Star Project(17QB1402800)

甲醛作为主要的室内空气污染气体,正在严重威胁着人类的健康。甲醛的治理引起了人们的广泛关注,其中催化氧化技术是目前最有效和环境友好的手段之一。因氧化锰结构多变和氧化能力强的特点,围绕锰基催化剂在甲醛深度氧化中应用的研究日渐成为热点。本文主要从单一组分MnOx催化剂、锰基复合氧化物催化剂、多孔材料负载MnOx催化剂以及MnOx负载贵金属催化剂四方面归纳总结了近年来锰基催化剂在甲醛氧化方面的研究进展,阐述了以Mars-van Krevelen机理为基础的甲醛催化氧化机制。在具体反应过程中,不同的表面氧物种和活性位点产生特定的中间相。重点分析了催化剂组分之间存在的协同作用对催化剂的影响,组分间的相互活化以及不同组分在多步反应中分别或依次发挥催化作用是实现锰基催化剂协同的主要方式。最后,展望了锰基催化剂在甲醛氧化反应中的未来发展方向和趋势。

关键词： 锰基催化剂, 催化氧化, 甲醛, 协同作用

Formaldehyde is one of the major indoor pollutants and has threatened the human health seriously. The treatment of formaldehyde has attracted broad attention. Catalytic oxidation is one of the most effective and environment-friendly technology. Presently, the catalytic deep oxidation of formaldehyde over manganese-based catalysts has become the research hotspot owing to the structure flexibility and good oxidation ability of manganese oxides(MnOx). The review mainly summarizes the recent progress in formaldehyde oxidation over manganese-based catalysts from four perspectives: pure MnOxcatalysts, manganese-based composite oxides, MnOx immobilization on porous material and MnOx supported noble-metal catalysts. Catalytic mechanisms are elaborated based on Mars-van Krevelen mechanism. Specified surface oxygen species and active sites in variety of catalysts produce corresponding intermediates during the catalytic oxidation of formaldehyde and consequently induce different reaction pathways. The influence of synergistic catalytic effect is emphatically discussed between catalyst components. The synergistic effect of manganese-based catalysts is achieved through one component activation by the other between two catalytic components for enhanced activity, or successional catalytic functioning of two components in catalytic reactions probably involving multi-step for enhanced activity and/or selectivity. Finally, the challenges and outlook are featured based on such catalysts in the application of HCHO removal.

Key words: manganese-based catalysts, catalytic oxidation, formaldehyde, synergistic effect
()
图1 不同氧化锰结构:(a)软锰矿;(b)斜方锰矿;(c)水钠锰矿;(d)尖晶石[18]
Fig. 1 Different MnO2 structures:(a)pyrolusite β-MnO2;(b)ramsdellite;(c)birnessite δ-MnO2;(d)spinel λ-MnO2[18]. ?Electrochemical Society.
表1 用于甲醛氧化的基于单一组分氧化锰催化剂代表性研究成果
Table 1 Catalytic oxidation of formaldehyde on pure MnOx catalysts
Catalyst Reaction condition HCHO conversion/removal ref
Cryptomelane-type MnO2 nanorods 50 mg catalyst, 100 ppm HCHO, 20% O2, 50 000/h 295.1% at 140 ℃ 20
Birnessite-type MnO2 nanospheres 50 mg catalyst, 100 ppm HCHO, 20% O2, 50 000/h 2100% at 140 ℃ 20
Ramsdellite MnO2 nanorods 50 mg catalyst, 100 ppm HCHO, 20% O2, 50 000/h 287.2% at 140 ℃ 20
Monoclinic MnOOH 50 mg catalyst, 100 ppm HCHO, 20% O2, 50 000/h 290.1% at 140 ℃ 20
Pyrolusite 200 mg catalyst, 400 ppm HCHO, 10% O2,18 000 mL/(g h) 1100% at 180 ℃ 21
Cryptomelane 200 mg catalyst, 400 ppm HCHO, 10% O2,18 000 mL/(g h) 1100% at 140 ℃ 21
Todorokite 200 mg catalyst, 400 ppm HCHO, 10% O2,18 000 mL/(g h) 1100% at 160 ℃ 21
Cocoon-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% over 200 ℃ 22
Urchin-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% over 200 ℃ 22
Nest-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% at 200 ℃ 22
α-MnO2 60 mg catalyst, 170 ppm HCHO, 20% O2, 100 000 mL/(g h) 1100% at 125 ℃ 23
β-MnO2 60 mg catalyst, 170 ppm HCHO, 20% O2, 100 000 mL/(g h) 1100% at 200 ℃ 23
γ-MnO2 60 mg catalyst, 170 ppm HCHO, 20% O2, 100 000 mL/(g h) 1100% at 150 ℃ 23
δ-MnO2 60 mg catalyst, 170 ppm HCHO, 20% O2, 100 000 mL/(g h) 1100% at 80 ℃ 23
MnO2 / 299% at 25 ℃ 24
MnOx 100 mg catalyst, air, 30 000 mL/(g h) 1100% at 40 ℃ 25
MnO2 / 299% at 25 ℃ 26
3D-MnO2 200 mg catalyst, 400 ppm HCHO,20% O2, 30 000 mL/(g h) 1100% at 130 ℃ 27
α-MnO2 nanorods 200 mg catalyst, 400 ppm HCHO,20% O2, 30 000 mL/(g h) 1100% at 140 ℃ 27
β-MnO2 nanorods 200 mg catalyst, 400 ppm HCHO,20% O2, 30 000 mL/(g h) 1100% at 180 ℃ 27
Ag-OMS-2 / 280% at 25 ℃ 28
Ag-OMS-2 200 mg catalyst, 400 ppm HCHO,10% O2 190% at 100 ℃ 29
K-OMS-2 nanorods 100 mg catalyst, 460 ppm HCHO, 21% O2, 30 000 mL/(g h) 1100% at 200 ℃ 30
K-OMS-2 nanoparticles 100 mg catalyst, 460 ppm HCHO, 21% O2, 30 000 mL/(g h) 154% at 200 ℃ 30
表2 用于甲醛氧化的锰基复合氧化物催化剂代表性研究成果
Table 2 Catalytic oxidation of formaldehyde on manganese-based composite oxides
Catalyst Reaction condition HCHO conversion/removal ref
MnOx-CeO2 200 mg catalyst, 400 ppm HCHO, 20% O2, 30 000 mL/(g h) 1100% at 140 ℃ 43
Ce-MnO2 100 mg catalyst, 190 ppm HCHO, air, 90 000 mL/(g h) 1100% at 100 ℃ 44
MnOx-CeO2 200 mg catalyst, 580 ppm HCHO,18% O2, 21 000 mL/(g h) 1100% at 100 ℃ 45
MnxCe1-xO2 300 mg catalyst, 61 ppm HCHO, air, 10 000/h 283.3% at 25 ℃ 46
MnOx-Co3O4-CeO2 50 mg catalyst, 200 ppm HCHO, 21% O2, 36 000 mL/(g h) 1100% at 100 ℃ 47
MnxCo3-xO4 150 mg catalyst, 80 ppm HCHO, 21% O2, 60 000/h 1100% at 75 ℃ 48
Co-MnOx/ZSM-5+O3 / 2100% at 25 ℃ 49
CoxMny 100 mg catalyst, 550 ppm HCHO 1<40% at 80 ℃ 50
3D-Co-Mn 250 mg catalyst, 80 ppm HCHO, 21% O2, 36 000/h 1100% at 70 ℃ 51
MnOx-SnO2 200 mg catalyst, 400 ppm HCHO,10% O2, 30 000 mL/(g h) 1100% at 180 ℃ 52
CuMn/HBC 800 mg catalyst, 100 ppm HCHO, 6% O2, 13 000/h 289% at 175 ℃ 53
Cu-Mn/γ-Al2O3 / 2100% at 150 ℃ 54
Cu-Mn/TiO2 / 2100% at 230 ℃ 54
CuO-MnO2 100 mg catalyst, 2.5 ppm HCHO, air, 125 000/h 2<40% at 25 ℃ 55
Fe2O3-MnO2 100 mg catalyst, 2.5 ppm HCHO, air, 125 000/h 2<40% at 25 ℃ 55
MnOx/TiO2+O3 600 mg catalyst, 45 ppm HCHO, 20 000/h 1100% at 25 ℃ 56
Zn/Mn/Mg / 263% at 25 ℃ 57
Zn/Mn/Ti / 277% at 25 ℃ 57
MnO2/CeO2/Al2O3 / 150% at 170 ℃ 58
表3 用于甲醛氧化的多孔材料负载氧化锰催化剂代表性研究成果
Table 3 Catalytic oxidation of formaldehyde on MnOx immobilization on porous material
Catalyst Reaction condition HCHO conversion/removal ref
MnOx/AC 10 ppm HCHO, air, 65 000/h 2100% at 25 ℃ 60
MnOx/AC 500 mg catalyst, 0.5 mg/m3 HCHO, air 2>70% at 25 ℃ 31
MnOx/ACF 200 mg catalyst, 300 ppm HCHO, 60 000 mL/(g h) 2100% at 25 ℃ 61
MnOx/GAC / 283% at 25 ℃ 62
MnO2/PAN / 2<50% at 60 ℃ 63
MnOx@PAN-ACNF 50 mg catalyst, 20 ppm HCHO, 20% O2 151% at 25 ℃ 64
MnOx/PET 500 mg catalyst, 0.6 mg/m3 HCHO, air, 17 000 /h 2100% at 25 ℃ 65
Graphene-MnO2 100 mg catalyst, 100 ppm HCHO, air, 30 000 mL/(g h) 1100% at 65 ℃ 32
RGO/MnO2 / 262.5% at 25 ℃ 66
MnOx/Cordierite honeycomb 100 mg catalyst, 20 ppm HCHO, air 280% at 85 ℃ 67
MnOx/SBA-15 200 mg catalyst,120 ppm HCHO, 20% O2/He 190% at 127 ℃ 68
表4 用于甲醛氧化的氧化锰负载贵金属催化剂代表性研究成果
Table 4 Catalytic oxidation of formaldehyde on MnOx supported noble-metal catalysts
Catalyst Reaction condition HCHO conversion/removal ref
Pt/MnO2/TiNT 200 mg catalyst, 50 ppm HCHO,20% O2, 30 000 mL/(g h) 195% at 30 ℃ 70
Pt/MnO2
 100 mg catalyst, 200 ppm HCHO, air, 30 000 mL/(g h) 1100% at 50 ℃/
~35% at 25 ℃		 71
Pt/cocoon-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% at 90 ℃ 22
Pt/urchin-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% at 80 ℃ 22
Pt/nest-like MnO2 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% at 70 ℃ 22
0.25Pd/20Mn/Beta 100 mg catalyst, 40 ppm HCHO, 20% O2, 90 000 mL/(g h) 1100% at 40 ℃ 72
Au/MnO2 100 mg catalyst, 200 ppm HCHO, air, 30 000 mL/(g h) 159.2% at 25 ℃ 73
Au0.5Pt0.5/MnO2/cotton 100 mg catalyst, 460 ppm HCHO, air, 20 000 mL/(g h) 1100% at 120 ℃ 74
3D-Ag/MnO2 200 mg catalyst, 500 ppm HCHO, 20% O2, 60 000/h 1100% at 110 ℃ 75
Ag/Fe-MnOx 200 mg catalyst, 400 ppm HCHO, 21% O2 1100% at 90 ℃ 76
Ag/CeO2-MnOx/SiO2 145 mg catalyst, 18 000~22 000 ppm HCHO, air, 69 000 mL/(g h) 2100% at 180 ℃ 77
图2 干燥条件下MnOx催化氧化甲醛的可能机理[67]
Fig. 2 The possible mechanism of catalytic oxidation of HCHO to CO2 on MnOx under dry condition[67] . ?Elsevier.
图3 Pd/Mn/Beta催化剂催化氧化甲醛可能的反应路径[72]
Fig. 3 A possible reaction pathway of HCHO oxidation over Pd/Mn/Beta catalyst[72]. ?Elsevier.
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