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Progress in Chemistry 2019, Vol. 31 Issue (2/3): 311-321 DOI: 10.7536/PC180435 Previous Articles   Next Articles

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: Online: Published:
  • 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)
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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
Fig. 1 Different MnO2 structures:(a)pyrolusite β-MnO2;(b)ramsdellite;(c)birnessite δ-MnO2;(d)spinel λ-MnO2[18]. ?Electrochemical Society.
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
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
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
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
Fig. 2 The possible mechanism of catalytic oxidation of HCHO to CO2 on MnOx under dry condition[67] . ?Elsevier.
Fig. 3 A possible reaction pathway of HCHO oxidation over Pd/Mn/Beta catalyst[72]. ?Elsevier.
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