选择催化还原(SCR)反应机理研究进展
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摘要
简述了NH_3和NO在催化剂表面吸附、转化活化和反应历程及H_2O和SO_2对以上反应行为的影响。分析表明,NH_3氧化脱氢进而与NO反应是决定NH_3反应性和最终产物的关键。NO以气态(Eley-Rideal机理)或硝基类物质等吸附态(Langmuir-Hinshelwood机理)形式参与选择催化还原(SCR)反应。提高催化剂酸性和氧化还原循环性能,利于NH_3和NO吸附和转化及相互间反应。高温时,H_2O影响轻微,而SO_2增强催化剂酸性,提高脱硝活性。低温时,H_2O和SO_2抑制NO吸附和转化活化,导致硫铵盐累积和活性位转变为硫酸盐使催化剂失活。因此,提高抗H_2O、抗SO_2性能是低温脱硝催化剂研发的重要方向。而发展在线升温等再生工艺以解决硝酸盐或含硫化合物导致的失活问题,对保障低温脱硝系统长期稳定运行具有重要意义。
In this work, adsorption, activation, and reactivity of NH_3 and NO on the selective catalytic reduction(SCR) catalysts and the effects of H_2 O and SO_2 on the reaction behaviors of NH_3 and NO were reviewed. The analysis shows that the co-reaction between the H-abstraction products of the adsorbed NH_3 and the adsorbed NO species(or gas phase NO) is the key to determine the NH_3 reactivity and the final SCR product. The gas phase NO could react with the H-abstraction products of the adsorbed NH_3 directly(Eley-Rideal mechanism). In addition, a lot of conversion products, such as nitrites and nitrates species, could form after NO was adsorbed and activated on the catalyst surface. These species could also react with adsorbed NH_3 species(Langmuir-Hinshelwood mechanism). This is another important pathway for NO to participate in the SCR reaction, especially at low temperature. It is beneficial for the adsorption and conversion of NH_3 and NO to enhance the catalyst acidity and redox ability. The effects of H_2 O and SO_2 on the catalyst are influenced by the temperature. At high temperature, the effect of H_2 O on the catalyst is very little, while the catalyst acidity could be enhanced by SO_2, which enhance NH_3 adsorption.At low temperature, however, the adsorption and conversion of NO could be inhibited severely by H_2 O and SO_2, especially the SO_2. The accumulation of ammonia sulphate and the conversion of active sites to sulphate could result in severe deactivation of the catalyst. Therefore, it is still a severe challenge to improve the H_2 O and SO_2 resistance ability for developing low temperature SCR catalyst. It is of great significance to increase the catalyst temperature to decompose the nitrate and sulfate to regenerate the catalyst in operation.
In this work, adsorption, activation, and reactivity of NH_3 and NO on the selective catalytic reduction(SCR) catalysts and the effects of H_2 O and SO_2 on the reaction behaviors of NH_3 and NO were reviewed. The analysis shows that the co-reaction between the H-abstraction products of the adsorbed NH_3 and the adsorbed NO species(or gas phase NO) is the key to determine the NH_3 reactivity and the final SCR product. The gas phase NO could react with the H-abstraction products of the adsorbed NH_3 directly(Eley-Rideal mechanism). In addition, a lot of conversion products, such as nitrites and nitrates species, could form after NO was adsorbed and activated on the catalyst surface. These species could also react with adsorbed NH_3 species(Langmuir-Hinshelwood mechanism). This is another important pathway for NO to participate in the SCR reaction, especially at low temperature. It is beneficial for the adsorption and conversion of NH_3 and NO to enhance the catalyst acidity and redox ability. The effects of H_2 O and SO_2 on the catalyst are influenced by the temperature. At high temperature, the effect of H_2 O on the catalyst is very little, while the catalyst acidity could be enhanced by SO_2, which enhance NH_3 adsorption.At low temperature, however, the adsorption and conversion of NO could be inhibited severely by H_2 O and SO_2, especially the SO_2. The accumulation of ammonia sulphate and the conversion of active sites to sulphate could result in severe deactivation of the catalyst. Therefore, it is still a severe challenge to improve the H_2 O and SO_2 resistance ability for developing low temperature SCR catalyst. It is of great significance to increase the catalyst temperature to decompose the nitrate and sulfate to regenerate the catalyst in operation.
引文
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[3] ZHU M, LAI J, WACHS I. Formation of N2O greenhouse gas during SCR of NO with NH3by supported vanadium oxide catalysts[J].Applied Catalysis B:Environmental, 2018, 224:836-840.
[4] ARFAOUI J, GHORBEL A, PETITTO C, et al. Novel V2O5-CeO2-TiO2-SO42-nanostructured aerogel catalyst for the low temperature selective catalytic reduction of NO by NH3in excess O2[J]. Applied Catalysis B:Environmental, 2018, 224:264-275.
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[10] ZHU M, LAI J K, TUMULURI U, et al. Nature of active sites and surface intermediates during SCR of NO with NH3by supported V2O5-WO3/TiO2catalysts[J]. Journal of the American Chemical Society,2017, 139(44):15624-15627.
[11] LIU Q, LIU Z, LI C. Adsorption and activation of NH3during selective catalytic reduction of NO by NH3[J]. Chinese Journal of Catalysis,2006, 27(7):636-646.
[12] ZHANG Q, FAN J, NING P, et al. In situ DRIFTS investigation of NH3-SCR reaction over CeO2/zirconium phosphate catalyst[J].Applied Surface Science, 2018, 435:1037-1045.
[13] ZHA K, CAI S, HU H, et al. In situ DRIFTs investigation of promotional effects of tungsten on MnOx-CeO2/meso-TiO2catalysts for NOx reduction[J]. Journal of Physical Chemistry C, 2017, 121(45):25243-25254.
[14] ZHANG L, SUN J, XIONG Y, et al. Catalytic performance of highly dispersed WO3loaded on CeO2in the selective catalytic reduction of NO by NH3[J]. Chinese Journal of Catalysis, 2017, 38(10):1749-1758.
[15] PENG Y, LI K, LI J. Identification of the active sites on CeO2-WO3catalysts for SCR of NOx with NH3:an in situ IR and Raman spectroscopy study[J]. Applied Catalysis B:Environmental, 2013, 140-141(2):483-492.
[16] GAO F, WASHTON N M, WANG Y, et al. Effects of Si/Al ratio on Cu/SSZ-13 NH3-SCR catalysts:implications for the active Cu species and the roles of Br?nsted acidity[J]. Journal of Catalysis, 2015, 331:25-38.
[17] PE?A D A, UPHADE B S, REDDY E P, et al. Identification of surface species on titania-supported manganese, chromium, and copper oxide low-temperature SCR catalysts[J]. Journal of Physical Chemistry B,2004, 108(28):9927-9936.
[18] LIU F, HE H, ZHANG C, et al. Mechanism of the selective catalytic reduction of NOx with NH3over environmental-friendly iron titanate catalyst[J]. Catalysis Today, 2011, 175(1):18-25.
[19] KIJLSTRA W S, BRANDS D S, SMIT H I, et al. Mechanism of the selective catalytic reduction of NO with NH3over MnOx/Al2O3:Ⅱ.Reactivity of adsorbed NH3and NO complexes[J]. Journal of Catalysis,1997, 171(1):219-230.
[20] KIJLSTRA W S, BRANDS D S, POELS E K, et al. Mechanism of the selective catalytic reduction of NO by NH3over MnOx/Al2O3:Ⅱ.Adsorption and desorption of the single reaction components[J].Journal of Catalysis, 1997, 171(1):208-218.
[21] TOPS?E N Y, TOPS?E H, DUMESIC J A. Vanadia/titania catalysts for selective catalytic reduction(SCR)of nitric-oxide by ammonia:Ⅱ.Combined temperature-programmed in-situ FTIR and on-line mass spectroscopy studies[J]. Journal of Catalysis, 1995, 151(1):226-240.
[22] SCHNEIDER H, TSCHUDIN S, SCHNEIDER M, et al. In situ diffuse reflectance FTIR study of the selective catalytic reduction of NO by NH3over vanadia-titania aerogels[J]. Journal of Catalysis, 1994,147(1):5-14.
[23] RAMIS G, BUSCA G, BREGANI F, et al. Fourier transform-infrared study of the adsorption and coadsorption of nitric oxide, nitrogen dioxide and ammonia on vanadia-titania and mechanism of selective catalytic reduction[J]. Applied Catalysis, 1990, 64(1/2):259-278.
[24] ZHU M, LAI J K, TUMULURI U, et al. Reaction pathways and kinetics for selective catalytic reduction(SCR)of acidic NOx emissions from power plants with NH3[J]. ACS Catalysis, 2017, 7(12):8358-8361.
[25] LIETTI L, SVACHULA J, FORZATTI P, et al. Surface and catalytic properties of vanadia-titania and tungsta-titania systems in the selective catalytic reduction of nitrogen oxides[J]. Catalysis Today,1993, 17(1/2):131-140.
[26] RAMIS G, YI L, BUSCA G, et al. Adsorption, activation, and oxidation of ammonia over SCR catalysts[J]. Journal of Catalysis, 1995, 157(2):523-535.
[27]刘清雅.蜂窝状堇青石基Cu-Al2O3催化剂的制备及其烟气脱硫脱硝的研究[D].太原:中国科学院山西煤炭化学研究所,2004.LIU Q Y. Study on the preparation of honeycomb cordierite based CuAl2O3catalyst and its application in flue gas desulfurization and denitrification[D]. Taiyuan:Shanxi Institute of Coal Chemistry,Chinese Academy of Sciences, 2004.
[28] QI G, YANG R T. Characterization and FTIR studies of MnOx-CeO2catalyst for low-temperature selective catalytic reduction of NO with NH3[J]. Journal of Physical Chemistry B, 2004, 108(40):15738-15747.
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