• 综述 •
王晓晗, 刘彩霞, 宋春风, 马德刚, 李振国, 刘庆岭. 金属有机骨架材料在氨低温催化还原氮氧化物反应中的应用[J]. 化学进展, 2020, 32(12): 1917-1929.
Xiaohan Wang, Caixia Liu, Chunfeng Song, Degang Ma, Zhenguo Li, Qingling Liu. Application of Metal-Organic Frameworks for Low-Temperature Selective Catalytic Reduction of NO with NH3[J]. Progress in Chemistry, 2020, 32(12): 1917-1929.
氮氧化物(NO x )是造成大气污染的主要污染物之一,工业窑炉和燃煤电厂等固定源以及以机动车为代表的移动源所排放的氮氧化物对生态环境造成了一系列的危害。为此控制并降低NO x 排放是当前十分艰巨的任务。金属有机骨架材料(MOFs)这种新型的多孔聚合材料由于其多活性位点、高比表面积、结构可修饰、易于功能化而表现出突出的多相催化性能近年来在低温工业脱硝领域逐渐受到关注。本文总结了MOFs材料在氨低温催化还原氮氧化物反应中的应用进展,重点阐述了单金属和双金属的MOFs材料的应用以及MOFs衍生物催化剂的研究。最后对MOFs在低温脱硝领域中目前存在的问题并对其发展方向和前景进行了展望。
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Catalyst | Reaction condition | Catalytic performance | ref |
---|---|---|---|
Cu-BTC(pre-treated at 230 ℃) | [NO]=500 ppm, [O2]=5 vol%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=100 mL/min, GHSV=30 000 h-1 | Max conversion: 100% (220~280 ℃) | |
Cu-MOF-74 | [NO]=1000 ppm, [O2]=2%, [NH3]=1000 ppm, Ar as balance gas, total gas flow rate=100 mL/min, GHSV=50 000 h -1 | Max NO conversion: 97.8%(230 ℃); 100% N 2 selectivity(230 ℃) | |
Mn-MOF-74 | [NO]=1000 ppm, [O2]=2%, [NH3]=1000 ppm, Ar as balance gas, total gas flow rate=100 mL/min | Max conversion: 99% (220 ℃) | |
P123-Mn-MOF-74 | [NO]=500 ppm, [O2]=5 vol%, [NH3]=500 ppm, Ar as balance gas, 5 vol% H2O(when used), total gas flow rate=100 mL/min | Max conversion: 92.1% (250 ℃) | |
Co-MOF-74 | [NO]=1000 ppm, [O2]=2%, [NH3]=1000 ppm, Ar as balance gas, total gas flow rate=100 mL/min | Max conversion: 70% (210 ℃) | |
Co/Mn-MOF-74 | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, Ar as balance gas, [SO2]=100 ppm(when used), 5 vol% H2O(when used), total gas flow rate=100 mL/min, GHSV=50 000 h-1 | Max conversion: 99%(200 ℃) 180~240 ℃ | |
MIL-100(Fe) | [NO]=500 ppm, [O2]=4%, [NH3]=500 ppm, N2 as balance gas, GHSV=30 000 h-1 | Max conversion: 100% (260 ℃) | |
MIL-100(Fe-Mn) | [NO]=500 ppm, [O2]=4%, [NH3]=500 ppm, N2 as balance gas, GHSV=30 000 h-1 | Max conversion: 96% (260 ℃) | |
IM-CeO 2/MIL-100(Fe) | [NO]=500 ppm, [O2]=4%, [NH3]=500 ppm, N2 as balance gas, [SO 2]=500 ppm(when used), 5 vol% H2O(when used), GHSV=30 000 h-1 | Max conversion: 100% 196~300 ℃ | |
Mn-Ce/UiO-67 | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=450 mL/min, GHSV=45 000 h-1 | Max conversion: 98% (200~300 ℃) | |
Mn/Cu 3(BTC) 2 | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, GHSV=30 000 h-1 | Max conversion: 100% 230~260 ℃ | |
Ag/Cu 3(BTC) 2 | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=100 mL/min, GHSV=30 000 h-1 | Max conversion: 100% 200~260 ℃ | |
Ni-MOF(pre-treated at 230 ℃) | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=100 mL/min, GHSV=15 000 h-1 | Max conversion: 92%(275 ℃) 275~440 ℃ | |
Cu+/Ni-MOF | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=100 mL/min, GHSV=15 000 h-1 | Max conversion: 95% 200~300 ℃ | |
MnO x/MIL-125(Ti) | [NO]=500 ppm, [O2]=5%, [NH3]=500 ppm, N2 as balance gas, [SO 2]=200 ppm(when used), 5 vol% H2O(when used), GHSV=30 000 h-1 | Max conversion: 100% 175~425 ℃ | |
MnO x/UiO-66 | [NO]=500 ppm, [O2]=5%, [NH3]=500ppm, Ar as balance gas, [SO2]=100 ppm(when used), 5 vol% H2O(when used), total flow rate=100 mL/min, GHSV=50 000 h-1 | Max conversion: 99% 125~250 ℃ | |
Ce 10/Zr-CAU-24 | [NO]=500 ppm, [O2]=10%, [NH3]=500 ppm, N2 as balance gas, total gas flow rate=150 mL/min. | Max conversion: 88%(210 ℃) | 59 |
Catalyst | Reaction condition | Catalytic performance | ref |
---|---|---|---|
MnO x from Mn-MOF-74 template | [NO]=500 ppm, [O 2]=5%, [NH 3]=500 ppm, N 2as balance gas, total gas flow rate=450 mL/min, GHSV=45 000 h -1 | Max conversion: 98% (220 ℃) | |
Co 3O 4/PC from ZIF-67 | [NO x ]=[NH 3]=500 ppm, [O 2]=5 vol%, [SO 2]=60 ppm(when used), [H 2O]=5 vol%(when used), Ar balance, total gas flow rate=300 mL/min, GHSV=14 000 h -1 | Max conversion: 90% 150~175 ℃ | |
CuO/Cu 2O from Cu-MOF template | [NO]=1000 ppm, [O 2]=3%, [NH 3]=1000 ppm, Ar as balance gas, total gas flow rate=200 mL/min, GHSV=40 000 h -1 | Max conversion: 100% 170~220 ℃ | |
MnO x from Mn-CP template | [NO]=400 ppm, [O 2]=3%, [NH 3]=400 ppm, N 2 as balance gas, total gas flow rate=1000 mL/min, GHSV=15 000 h -1 | Max conversion: 91.3% 100~200 ℃ | |
Mn 3O 4@G-A from Mn-BTC-SA | [NO]=[NH 3]=600 ppm, [O 2]=5 vol%, [SO 2]=50 ppm(when used), [H 2O]=5.6 vol%(when used), N 2as balance gas, GHSV=60 000 h -1 | Max conversion: 100% 140~290 ℃ | |
Fe 2O 3-2S from MIL-100(Fe) | [NO]=[NH 3]=1000 ppm, [O 2]=4 vol%, [SO 2]=500 ppm(when used), [H 2O]=8 vol%(when used), N 2 as balance gas, GHSV=30,000 h -1 | Max conversion: 100% 250~325 ℃ | |
MnO x -FeO x nanoneedles from Mn/Fe-MOF | [NO]=500 ppm, [O 2]=5%, [NH 3]=500 ppm, N 2as balance gas, total gas flow rate=600 mL/min, GHSV=36 000 h -1 | Max conversion: 100% 120~240 ℃ | |
CuO/Cu 3(BTC) 2 | [NO]=[NH 3]=600 ppm, [O 2]=4 vol%, [SO 2]=150 ppm(when used), [H 2O]=4 vol%(when used), N 2 as balance gas, GHSV=60 000 h -1 | Max conversion: 95% 180~240 ℃ | |
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