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刘喆, 张晓岚, 蔡婷, 袁静, 赵昆峰, 何丹农. 用于甲醛催化氧化的锰基催化剂及协同效应的影响[J]. 化学进展, 2019, 31(2/3): 311-321.
Zhe Liu, Xiaolan Zhang, Ting Cai, Jing Yua, Kunfeng Zhao, Dannong He. Catalytic Oxidation of Formaldehyde over Manganese-Based Catalysts and the Influence of Synergistic Effect[J]. Progress in Chemistry, 2019, 31(2/3): 311-321.
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。
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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 |
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 |
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 |
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 |
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