Research progress of SCR medium temperature denitrification catalyst for cement industry
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摘要: 选择性催化还原技术(SCR)在水泥行业脱硝中被广泛应用，其中，高温范围内（280–350 ℃）已有较为完善的SCR技术及体系，但在中温区仍有待突破。本工作以中温脱硝催化剂为重点，综述了Mn、Ce、V系脱硝催化剂的研究进展，并分析了Sm、Nb、Ho、Sb、La、Mo、Pr的掺杂对于脱硝催化剂的改性，结合水泥窑炉烟尘中SO2、H2O、碱金属含量高的特点，分析了脱硝催化剂中毒原因，对催化剂的抗H2O、SO2、碱金属中毒性能进行了探讨，展望了水泥行业SCR中温脱硝催化剂的研究前景。Abstract: Selective catalytic reduction (SCR) technology has been widely used in the denitrification of cement industry, in which a relatively mature system has been formed in the high temperature (280–350 ℃) section, but there is still a breakthrough in the middle temperature zone. Focusing on medium temperature catalysts, this paper reviewed the progress of Mn, Ce and V catalysts, and analyzed the doping of Sm, Nb, Ho, Sb, La, Mo and Pr to improve the performance of catalysts. Combined with the characteristics of the high content of SO2, H2O and alkali metal in cement kiln smoke, the causes of catalyst poisoning were analyzed, and the way to resist sulfur poisoning, water poisoning, and alkali metal poisoning was summarized. The research prospect of SCR medium temperature denitration catalyst in cement industry is prospected.
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Key words:
- selective catalytic reduction /
- de NOx /
- cement denitration /
- alkali metal
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图 4 3DOM结构下Ce-Fe催化剂的SEM图像[78]
Figure 4 SEM image of Ce-Fe catalyst with 3DOM structure
(with permission from Elsevier)
表 1 Mn系催化剂活性
Table 1 Summary of Mn catalyst activity
Catalyst/Carrier GHSV/h−1 Temperature/℃ Catalyst preparation Reference MnOx 47000 80–150 rheological phase reaction [28] MnOx 47000 80–150 solid [29] Tunneled α-MnO2 38000 120–200 hydrothermal [30] γ-MnO2 30000 140–200 thermal decomposition [31] γ-MnO2 nanosheets 35000 150–230 hydrothermal [32] MnOx 36000 120–180 hydrothermal [33] MnOx-γAl2O3 60000 200–350 impregnation [44] Mn/TiO2 30% 100000 200–300 sol-gel [46] MnTiEu-0.3 36000 180–390 coprecipitation [48] 30%Mn/TiO2-3%Nd 40000 100–350 impregnation [49] 20%Mn-10%Sm/TiO2 80000 110–250 impregnation [50] MnOx-C/C 4000 ~150 impregnation [52] MnOx-CeO2 10600 100–150 impregnation [53] Mn/REC 105000 150–250 in-situ synthesis [54] 
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表 2 Ce系催化剂活性
Table 2 Summarizes the activity of Ce catalyst
Catalyst/Carrier GHSV/h−1 Temperature/℃ Catalyst preparation Reference CeO2-Ar 36000 120–400 citric acid [57] 50%CeO2-Ti 30000 180–400 coprecipitation [67] 5%Ce-TiO2 50000 275–400 impregnation [69] Ce0.6Ti 50000 300–400 sol-gel [70] Sn(0.1)Mn(0.4)CeOx 35000 80–230 coprecipitation [71] MnOx(0.3)-CeO2 42000 100–180 citric acid [72] MnOx(0.3)-CeO2 42000 120–150 citric acid [73] Mn1Ce9 64000 100–200 surfactant-template [74] Ce0.6Fe0.4O2 90000 200–400 impregnation [77] Ce-Fe(1:0.35) 6000 200–300 microwave hydrothermal [78] Ce-Fe-Ox 18000 250–450 hydrothermal [79] Ce0.3TiF1.5 41000 180–240 coprecipitation [81] CuO-CeO2-TiO2 30000 150–250 sol-gel [82] CeO2/TiO2-MoO3 60000 200–350 hydrothermal [83] Cu-Ce0.25-Zr0.75/TiO2 100000 165–450 impregnation [84] Ce20Nb20Ti 90000 250–450 sol-gel [85]
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表 3 V系催化剂活性
Table 3 Summarizes the activity of V-type catalysts
Catalyst/carrier GHSV/h−1 Temperature/℃ Catalyst preparation Reference Ti0.9V0.1O2−δ (304/20) 24000 200–400 Stagnation Premixed
flame system[86] V1Ce5Ti 12800 325–450 impregnation [93] V/Ce1-xTixO2(x = 0.3, 0.5) 70000 190–300 coprecipitation [94] 5V30Ce/TiO2 10000 180–220 impregnation [95] V-W/Ce/Ti-5% 18000 280–450 impregnation [97] V/7Mo-Ti 180000 300–360 impregnation [98] VWSbTi 10000 350–400 impregnation [99] Cr0.2V0.8/TiO2 60000 160–300 impregnation [100] VWCeCuTi 60000 250–375 impregnation [101] 3V3Nb/WTi 60000 225–400 impregnation [102]
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表 4 其他稀土改性催化剂活性
Table 4 Summary of activities of other rare earth based catalysts
Catalyst/carrier GHSV/h−1 Temperature/℃ Catalyst preparation Reference 20Mn-10Sm/TiO2 80000 110–250 impregnation [50] Sm-Mn-0.1 48600 75–200 coprecipitation [103] SmCeTi 90000 250–425 coprecipitation [104] MnSmZrTiOx 30000 125–274 coprecipitation [105] MnCeNbTiOx 180000 125–275 coprecipitation [106] Nb-VOx/CeO2 50000 175–350 coprecipitation [108] MnNb0.4Ce0.2Ox 30000 120–240 coprecipitation [109] Fe0.3Ho0.1Mn0.4/TiO2 20000 60–200 impregnation [110] Mn0.4Ce0.07Ho0.1/TiO2 10000 140–220 impregnation [111] Fe0.3Ho0.1Mn0.4/TiO2 20000 60–200 impregnation [112] V2.7Sb2Ti 5000 225–375 impregnation [113] SbV10Ce/TiO2 60000 250–400 impregnation [114] CeSbZrOx 50000 225–350 coprecipitation [115] Sb1.0CeZr2Ox 40000 200–360 citric acid [116] La2.6CuMnOx 24000 250–350 coprecipitation [117] LaMnO3/hematite 9000 150–240 impregnation [120] CeMoTiOx 150000 200–425 coprecipitation [122] Ce40Mo10Ti 90000 250–450 coprecipitation [125] Mo/CeTiOx 48000 200–400 coprecipitation [126] V2O5-MoO3/Pr6O11-TiO2 30000 220–400 sol-gel [127] PrOx(0.2)-MnOx/SAPO-34 40000 140–280 solvent dispersion [128] Fe-Mn/TiO2 (0.02Pr) 30000 140–220 impregnation [129] MnPrOx-0.1 30000 120–220 coprecipitation [130]
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表 5 催化剂抗中毒性能
Table 5 Summary of toxic resistance of catalyst
Catalyst/carrier GHSV/h−1 Temperature/℃ Toxic concentration Catalyst preparation Reference Mn-Ce/TiO2 40000 150 1.0×10–4 SO2，3% H2O sol-gel [133] 30Ce6W 36000 250–475 1.0×10–4 SO2 coprecipitation [134] CeSi2 90000 200–400 5.0×10–4 SO2，5% H2O coprecipitation [135] Ce0.6Zr0.4O2 90000 250–300 2.0×10–4 SO2 coprecipitation [137] FeMnOx/Ce 30000 120 1.0×10–4 SO2 citric acid [138] 3V6Nb/WTi 60000 225 5.0×10–4 SO2，5% H2O impregnation [102] MnNb0.4Ce0.2Ox 30000 120–240 2.0×10–4 SO2，7% H2O coprecipitation [109] MnTiEu-0.3 36000 200 5.0×10–5 SO2，5% H2O coprecipitation [48] 2Fe4Co-MCT 12000 200 2.0×10–4 SO2 impregnation [139] Mn0.2Ti0.8O2 60000 150 5% H2O hydrothermal [140] MnCe/GAC-CNTs 10000 150 5.0×10–4 SO2，5% H2O impregnation [143] Mn2Nb1Ox 50000 200 5% H2O coprecipitation [144] MnCo2O4 32000 200 6% H2O coprecipitation [145] MnO2-Co-0.8 50000 200 1.0/2.0×10–4 SO2，5% H2O hydrothermal [146] Ce/TiO2 108000 100–400 Ca/Ce = 0.05 sol-gel [147] Ce/TiO2 108000 100–220 Na:Ce =0.2 sol-gel [148] V/W/Ti 30000 250–400 Ca /V=0, 1, 2, 3 impregnation [149] V2O5/TiO2 96000 310 Ca/V =0–0.2 impregnation [150] P-Ce/TiO2 108000 250–400 K/Ce=0.2 coprecipitation [151] V2O5-WO3/TiO2-CeO2-ZrO2 60000 250–400 K2O=1% coprecipitation [152] V2O5-WO3/TiO2-CeO2-ZrO2 60000 200–450 K2O=1% coprecipitation [153] CeO2-MnOx/TiO2 120000 175–300 K=10/25/50 μmol/g coprecipitation [154] MoO3
(V-HMoO)66000 280–420 K2O=1% hydrothermal [155] K-MnO2 60000 50–200 K=4.22% [156] CeO2-WO3 120000 200–450 CaO=5% impregnation [157]
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