以纳米TiO_2为载体的燃煤烟气脱硝SCR催化剂的研究
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摘要
选择性催化还原(SCR)技术是重要的燃煤烟气脱硝技术,而催化剂是其中的关键技术之一。为了推进SCR脱硝技术在中国的应用,本课题与国内纳米TiO_2生产厂商合作,以其生产的纳米TiO_2为载体联合开发面向燃煤电厂烟气脱硝的V_2O_5/TiO_2基SCR催化剂,研究分为颗粒状催化剂和成型性催化剂两个阶段。
在自制颗粒状SCR催化剂活性试验台测试活性,结合BET、XRD、SEM -EDX、FT-IR、DTG等表观-微观表征技术,对V_2O_5/TiO_2基催化剂载体TiO_2的晶相结构和加工工艺、活性物质V_2O_5的含量、助催化剂和毒物的影响及制备工艺等进行研究,得到了适用于燃煤烟气脱硝催化剂基本粉体的优化配方和制备工艺,并得到基本粉体的本征动力学参数,建立了与试验工况吻合得较好的包括外扩散、内扩散和化学反应在内的动力学模型。以优化配方的粉体为基体,通过与各种成型助剂干混、捏合、成型、干燥和煅烧等得到具有一定机械强度和形状的蜂窝状或板状催化剂,在自制成型性催化剂SCR活性试验台上测试活性,对成型助剂的配比、制备工艺、催化剂的形状及几何尺寸和工况条件等进行优化,得到可以满足燃煤电厂烟气脱硝对SCR催化剂要求的蜂窝状催化剂的配方和制备工艺,建立了有一定应用价值的整体式催化剂数学模型。通过以上研究主要取得以下成果:
(1)通过对7种不同制备工艺和晶相的纳米TiO_2为载体进行研究,确定了以硫酸法制备的含8~10%(重量比)SO_3的锐钛型纳米TiO_2非常适合作为SCR催化剂的载体,而氯化法制备的纳米锐钛型TiO_2由于会和活性物质V_2O_5反应生成V_3Ti_6O_(17)聚合物而不适合作为SCR催化剂载体;
(2)通过对催化剂配方和制备工艺进行研究,得到了SCR催化剂的优化配方为1%V_2O_5-10%WO_3 /TiO_2-8~10%SO_3(重量比);
(3)建立了包括外扩散、内扩散和反应在内的颗粒状催化剂的数学模型预测结果与实验值吻合得较好,可以指导颗粒状催化剂的设计运行;
(4)对成型SCR催化剂膏体的组成和制备工艺进行了研究,其中成型催化剂的膏体的组成包括优化的SCR催化剂基本粉体、水、粘合剂聚丙烯酰胺、助挤剂乙醇胺、扩孔剂活性炭粉体及结构助剂杆状玻璃纤维等,对其含量和成型制备工艺进行了优化研究,得到了具有一定机械强度和活性的蜂窝状催化剂;
(5)对成型催化剂形状、几何尺寸及应用工况的优化:在“干净烟气”条件下,对蜂窝状催化剂和板状催化剂的孔(板)间距、壁厚、长度、氨氮比、空速比等进行研究,发现在优化配方和制备工艺条件下得到的孔径10×10mm、孔数4×4、壁厚1mm的蜂窝状催化剂在空速比(SV比)小于3500h~(-1)、氨氮比0.9~1.0、温度320~420℃范围内的NO脱除率较高、SO_2氧化率较低和氨逃逸量较低,基本达到工业应用的要求,而在相近工况下平板型催化剂NO脱除率较低;而在“肮脏烟气”条件下,低含量(低于2%)水蒸气可以提高高温段NO脱除率,而高含量
Selective catalytic reduction (SCR) is an important technology for denitrification of flue gas from coal-fired power plant, among which catalyst is the key elment of the whole DeNOx system.
In this dissertation, with the help of a domestic manufacturer of nanometer titanium dioxide (TiO_2),SCR catalyst for coal-fired flue gas denitrificaiton was investigated systematically grafted on the domestic nanometer TiO_2. The whole dissertation includes the selection and optimization of the ingredient, geometry, preparation, operation conditions and kinetics of SCR catalyst in the form of powder and ceramic monolith by means of activity measurements and micro- and macro- characterization technologies such as BET, XRD, SEM-EDX, FT-IR, DTG and so on. By thorough investigation, it is found that 1%V_2O_5-10%WO3/ TiO_2 catalyst powder based on nanometer anatase TiO_2 form TiOSO4, which includs 8-10% sulfate (cal. SO_3 ) in the mass, is suitable for the preparation of monolithic SCR catalyst for coal-fired flue gas denitrification by mixing of proper kind and content of water, organic binder, extruding-aid addictive, pore-enlarging addictive, lubricating oil and fiber-glass in the sequences of mixing, kneading, extruding, drying and calcination under suitable conditions. Kinetic parameter of selected SCR catalyst powder was obtained, and then a global mathematical model including kinetics and intra-phase and intra-particle transfer was developed, which can be used for the design and performance of SCR catalyst.
1. Among commercial anantase TiO_2, anatase and rutile nanometer TiO_2 from TiOSO4 ,TiCl4 and mixture of anatase and rutile nanometer TiO_2, anatase nanometer TiO_2 including 8-10% sulfate form TiOSO4, are proper as SCR catalyst support while anatase nanometer TiO_2 form TiCl4 are not suitable due to its reaction with V_2O_5 to form V_3Ti_6O_(17).
2. Ingredient optimization study of SCR catalyst by DeNOx activity and characterization technologies shows 1%V_2O_5-10%WO3/TiO_2-9.2%SO_3 catalyst, whose nano-grade support is made from TiOSO4, has large BET area and textile construction, high DeNOx efficiency, broad window temperature and good selectivity, whose performance is even superior to commercial catalyst in some areas.
3. Kinetic parameter of selected SCR catalyst powder was obtained, and then a global mathematical model including kinetics and intra-phase and intra-particle transfer was developed, which can be used for the design and performance of SCR catalyst.
在自制颗粒状SCR催化剂活性试验台测试活性,结合BET、XRD、SEM -EDX、FT-IR、DTG等表观-微观表征技术,对V_2O_5/TiO_2基催化剂载体TiO_2的晶相结构和加工工艺、活性物质V_2O_5的含量、助催化剂和毒物的影响及制备工艺等进行研究,得到了适用于燃煤烟气脱硝催化剂基本粉体的优化配方和制备工艺,并得到基本粉体的本征动力学参数,建立了与试验工况吻合得较好的包括外扩散、内扩散和化学反应在内的动力学模型。以优化配方的粉体为基体,通过与各种成型助剂干混、捏合、成型、干燥和煅烧等得到具有一定机械强度和形状的蜂窝状或板状催化剂,在自制成型性催化剂SCR活性试验台上测试活性,对成型助剂的配比、制备工艺、催化剂的形状及几何尺寸和工况条件等进行优化,得到可以满足燃煤电厂烟气脱硝对SCR催化剂要求的蜂窝状催化剂的配方和制备工艺,建立了有一定应用价值的整体式催化剂数学模型。通过以上研究主要取得以下成果:
(1)通过对7种不同制备工艺和晶相的纳米TiO_2为载体进行研究,确定了以硫酸法制备的含8~10%(重量比)SO_3的锐钛型纳米TiO_2非常适合作为SCR催化剂的载体,而氯化法制备的纳米锐钛型TiO_2由于会和活性物质V_2O_5反应生成V_3Ti_6O_(17)聚合物而不适合作为SCR催化剂载体;
(2)通过对催化剂配方和制备工艺进行研究,得到了SCR催化剂的优化配方为1%V_2O_5-10%WO_3 /TiO_2-8~10%SO_3(重量比);
(3)建立了包括外扩散、内扩散和反应在内的颗粒状催化剂的数学模型预测结果与实验值吻合得较好,可以指导颗粒状催化剂的设计运行;
(4)对成型SCR催化剂膏体的组成和制备工艺进行了研究,其中成型催化剂的膏体的组成包括优化的SCR催化剂基本粉体、水、粘合剂聚丙烯酰胺、助挤剂乙醇胺、扩孔剂活性炭粉体及结构助剂杆状玻璃纤维等,对其含量和成型制备工艺进行了优化研究,得到了具有一定机械强度和活性的蜂窝状催化剂;
(5)对成型催化剂形状、几何尺寸及应用工况的优化:在“干净烟气”条件下,对蜂窝状催化剂和板状催化剂的孔(板)间距、壁厚、长度、氨氮比、空速比等进行研究,发现在优化配方和制备工艺条件下得到的孔径10×10mm、孔数4×4、壁厚1mm的蜂窝状催化剂在空速比(SV比)小于3500h~(-1)、氨氮比0.9~1.0、温度320~420℃范围内的NO脱除率较高、SO_2氧化率较低和氨逃逸量较低,基本达到工业应用的要求,而在相近工况下平板型催化剂NO脱除率较低;而在“肮脏烟气”条件下,低含量(低于2%)水蒸气可以提高高温段NO脱除率,而高含量
Selective catalytic reduction (SCR) is an important technology for denitrification of flue gas from coal-fired power plant, among which catalyst is the key elment of the whole DeNOx system.
In this dissertation, with the help of a domestic manufacturer of nanometer titanium dioxide (TiO_2),SCR catalyst for coal-fired flue gas denitrificaiton was investigated systematically grafted on the domestic nanometer TiO_2. The whole dissertation includes the selection and optimization of the ingredient, geometry, preparation, operation conditions and kinetics of SCR catalyst in the form of powder and ceramic monolith by means of activity measurements and micro- and macro- characterization technologies such as BET, XRD, SEM-EDX, FT-IR, DTG and so on. By thorough investigation, it is found that 1%V_2O_5-10%WO3/ TiO_2 catalyst powder based on nanometer anatase TiO_2 form TiOSO4, which includs 8-10% sulfate (cal. SO_3 ) in the mass, is suitable for the preparation of monolithic SCR catalyst for coal-fired flue gas denitrification by mixing of proper kind and content of water, organic binder, extruding-aid addictive, pore-enlarging addictive, lubricating oil and fiber-glass in the sequences of mixing, kneading, extruding, drying and calcination under suitable conditions. Kinetic parameter of selected SCR catalyst powder was obtained, and then a global mathematical model including kinetics and intra-phase and intra-particle transfer was developed, which can be used for the design and performance of SCR catalyst.
1. Among commercial anantase TiO_2, anatase and rutile nanometer TiO_2 from TiOSO4 ,TiCl4 and mixture of anatase and rutile nanometer TiO_2, anatase nanometer TiO_2 including 8-10% sulfate form TiOSO4, are proper as SCR catalyst support while anatase nanometer TiO_2 form TiCl4 are not suitable due to its reaction with V_2O_5 to form V_3Ti_6O_(17).
2. Ingredient optimization study of SCR catalyst by DeNOx activity and characterization technologies shows 1%V_2O_5-10%WO3/TiO_2-9.2%SO_3 catalyst, whose nano-grade support is made from TiOSO4, has large BET area and textile construction, high DeNOx efficiency, broad window temperature and good selectivity, whose performance is even superior to commercial catalyst in some areas.
3. Kinetic parameter of selected SCR catalyst powder was obtained, and then a global mathematical model including kinetics and intra-phase and intra-particle transfer was developed, which can be used for the design and performance of SCR catalyst.
引文
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[1] 孙锦宜,林西平编著,环保催化材料与应用[M],化学工业出版社材料科学与工程出版中心,2002
[2] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NO_x by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[3] Pio Forzatti, Present status and perspectives in de-NO_x SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[4] Went,Gregory Thomas, Studies of supported vanadium oxide catalysts for the selective catalytic reduction of nitrogen oxides[D]: Ph. D. dissertation, University of California, Berkeley, 1991
[5] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[6] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NO_x SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[7] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NO_x catalysts[J], Journal of Catalysis, 1995, 155:117-130
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[10] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
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[12] Michael D. Amiridis, Robert V. Duevel and Israel E. Wachs, The effect of metal oxide addictive on the activity of V_2O_5/TiO_2 catalysts for the selective catalytic reduction of nitric oxide by ammonia[J], Applied catalysis B: Environmental, 1999, 20: 111-122
[13] L. Lisi, G. Lasorella, S. Malloggi and G, . Russo, Single and combined deactivation effect of alkali metals and HCl on commercial SCR catalysts[J], Applied catalysis B: Environmental, 2004, 50: 251-258
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[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NO_x by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[2] Pio Forzatti, Present Status and perspectives in de-NO_x SCR catalysis[J], Applied Catalysis A: General 222 (2001) :221-236
[3] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[4] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NO_x SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[5] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NO_x catalysts[J], Journal of Catalysis, 1995, 155:117-130
[6] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
[7] 山中龙雄,催化剂的有效实际应用[M],化学工业出版社,1988
[8] 罗永刚,易再生高比表面积脱硫脱硝剂的设计及其机理性研究[D]:博士学位论文,东南大学,2004
[9] 孙锦宜,林西平编著,环保催化材料与应用[M],化学工业出版社材料科学与工程出版中心,2002
[10] 一种用于还原法去除氮的氧化物的催化剂的制备工艺[P],宇都兴产株式会社,申请日:85.9.29,申请号:CN85 1 07366,A
[11] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[12] 高濂,纳米氧化钛光催化材料及应用[M],化学工业出版社,2005
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[14] 张继光主编,催化剂制备过程技术[M],中国石化出版社,2004
[15] Carlo Orsenigo, Luca Lietti, Enrico Tronconi, et. al., Dynamic investigation of the role of the surface sulfates in NO_x reduction and SO2 oxidation over V_2O_5-WO3/TiO_2 catalysts[J], Ind. Eng. Chem. Res., 1998,37(6):2350-2359
[16] P. Ciambelli, M. E. Fortuna, D. Sannino and A. Baldacci, The influence of sulphate on the catalytic properties of V_2O_5-TiO_2 and WO3-TiO_2 in the reduction of nitric oxide with ammonia[J], Catalysis Today, 1996, 29: 161-164
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[2] 刘清雅,蜂窝状堇青石基 CuO/A12O3 催化剂的制备及其烟气脱硫脱硝的研究[D]:博士学位论文,太原:中科院山西煤化所,2004
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[5] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[6] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
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[9] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[10] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155: 117-130
[11] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
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[15] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[16] Akira Miyamoto, Kan Kobayashi, Mokoto Inomata, et. al., Nitrogen-15 tracer investigation of the mechanism of the reduction of NO with NH3 on vanadium oxide catalysts[J], J. Phys. Chem., 1982, 86(15): 2945-2950
[17] Carlo Orsenigo, Luca Lietti, Enrico Tronconi, et. al., Dynamic investigation of the role of the surface sulfates in NOx reduction and SO2 oxidation over V_2O_5-WO3/TiO_2 catalysts[J], Ind. Eng. Chem. Res., 1998,37(6): 2350-2359
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[1] Guido Busca, Luca Lietti, Gianguido Ramis and Francesco Berti, chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: a review[J], Applied catalysis B: Environmental, 1998, 18: 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Miroslav Radojevic, Reduction of nitrogen oxides in flue gas[J], Environmental pollution, 1998, 102(S1): 685-689
[4] Michael D. Amiridis, Robert V. Duevel and Israel E. Wachs, The effect of metal oxide addictive on the activity of V_2O_5/TiO_2 catalysts for the selective catalytic reduction of nitric oxide by ammonia[J], Applied catalysis B: Environmental, 1999, 20: 111-122
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[8] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[9] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
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[12] L. Lisi, G. Lasorella, S. Malloggi and G, . Russo, Single and combined deactivation effect of alkali metals and HCl on commercial SCR catalysts[J], Applied catalysis B: Environmental, 2004, 50: 251-258
[13] Hiroyuki Kamata, Katsumi Takahashi and C. U. Ingemar Odenbrand, The role of K2O in the selective reduction of NO with NH3 over a V_2O_5(WO3)/TiO_2 commercial selective catalytic reduction catalyst[J], Journal of Molecular Catalysis A: General, 1999, 139: 189-198
[14] Chen, Jianping, Preparation, Characterization and deactivation of the catalysts for the selective catalytic reduction of NO with NH3[D]: Ph. D. dissertation, State University of New York at Baffalo, 1993
[15] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[16] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], Catalysis today, 1996, 29: 143-148
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[18] Went, Gregory Thomas, Study of supported vanadium oxide catalysts for the selective catalytic reduction of nitrogen oxides[D]: Ph. D. dissertation, University of Califonia, Berkeley, 1991
[1] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[2] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[3] G. Ramis, G. Busca, C. Cristiani, et. al., Characterization of tungsta-titania catalysts[J], Langmuir, 1992, 8 (7): 1744-1749
[4] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155: 117-130
[5] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
[6] M. A. Reiche, T. Bürgi, A. Baiker, et. al., Vanadia and tungsta grafted on TiO_2: influence of the grafting sequence on structural and chemicperties[J], Applied catalysis A: general, 2000, 198: 155-169
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[11] E. Tronconi, L. Lietti, P. Forzatti, et. al., Experimental and theoretical investigation of the dynamicsof the SCR-DeNOx reaction[J], Chemical Engineering Science, 1996, 51(11): 2965-2970
[12] C. U. Ingemar Odenbrand, Ana Bahamonde, Pedro Avila, et. al., Kinetic study of the selective reduction of nitric oxide over vanadia-tungsta-titania/sepiolite catalyst[J], Applied Catalysis B: Environmental, 1994, 5: 117-131
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[15] Carlo Orsenigo, Alessandra Beretta, Pio Forzatti, et. al., Theretical and experimental study of the interaction between NOx reduction and SO2 oxidation over DeNOx-SCR catalysts[J], Catalysis Today, 1996, 27: 15-21
[16] Jiri Svachula, Louis J. Alemany, Natale Ferlazzo, Pio Forzatti , et. al., Oxidation of SO2 to SO3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 32(5): 826-834
[17] Enrico Tronconi, Andra Cavanna, Carlo Orsenigo and Pio Forzatti, Transient kinetics of SO2 oxidation over SCR-DeNOx monolith catalysts[J], ind. Eng. Chem. Res., 1999, 28(7): 2593-2598
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[20] Akira Miyamoto, Kan Kobayashi, Mokoto Inomata, et. al., Nitrogen-15 tracer investigation of the mechanism of the reduction of NO with NH3 on vanadium oxide catalysts[J], J. Phys. Chem., 1982, 86(15): 2945-2950
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[24] C. U. Ingemar Odenbrand, Ana Bahamonde, Pedro Avila, et. al., Kinetic study of the selective reduction of nitric oxide over vanadia-tungsta-titania/sepiolite catalyst[J], Applied Catalysis B: Environmental, 1994, 5: 117-131
[25] Went, Gregory Thomas, Study of supported vanadium oxide catalysts for the selective catalytic reduction of nitrogen oxides[D], Ph. D, University of Califonia, Berkeley, 1991
[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[4] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[5] R. Q. Long, R. T. Yang, Selective catalytic reduction of NO with ammonia over V_2O_5 doped TiO_2 clay catalysts[J], Applied catalysis B: Environmental, 2000, 24:13-21
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[7] Enrico Tronconi, The role of inter- and intra-phase mass transfer in the SCR-DeNOx reaction over catalysts of different shapes[J], catalysis today, 1999, 52: 249-258
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[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Miroslav Radojevic, Reduction of nitrogen oxides in flue gas[J], Environmental pollution, 1998, 102(S1): 685-689
[4] Jiri Svachula, Natale Ferlazzo, Pio Forzatti, et. al., Selective reduction of NOx by NH_3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 12(6): 1053-1060
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[11] Jiri Svachula, Louis J. Alemany, Natale Ferlazzo, Pio Forzatti , et. al., Oxidation of SO2 to SO3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 32(5): 826-834
[12] Enrico Tronconi, Andra Cavanna, Carlo Orsenigo and Pio Forzatti, Transient kinetics of SO2 oxidation over SCR-DeNOx monolith catalysts[J], ind. Eng. Chem. Res., 1999, 28(7): 2593-2598
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[18] Enrico Tronconi, The role of inter- and intra-phase mass transfer in the SCR-DeNOx reaction over catalysts of different shapes[J], catalysis today, 1999, 52: 249-258
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[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NO_x by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
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[3] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
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[5] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NO_x catalysts[J], Journal of Catalysis, 1995, 155:117-130
[6] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
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[12] 高濂,纳米氧化钛光催化材料及应用[M],化学工业出版社,2005
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[14] 张继光主编,催化剂制备过程技术[M],中国石化出版社,2004
[15] Carlo Orsenigo, Luca Lietti, Enrico Tronconi, et. al., Dynamic investigation of the role of the surface sulfates in NO_x reduction and SO2 oxidation over V_2O_5-WO3/TiO_2 catalysts[J], Ind. Eng. Chem. Res., 1998,37(6):2350-2359
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[2] 刘清雅,蜂窝状堇青石基 CuO/A12O3 催化剂的制备及其烟气脱硫脱硝的研究[D]:博士学位论文,太原:中科院山西煤化所,2004
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[5] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[6] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
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[9] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[10] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155: 117-130
[11] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
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[16] Akira Miyamoto, Kan Kobayashi, Mokoto Inomata, et. al., Nitrogen-15 tracer investigation of the mechanism of the reduction of NO with NH3 on vanadium oxide catalysts[J], J. Phys. Chem., 1982, 86(15): 2945-2950
[17] Carlo Orsenigo, Luca Lietti, Enrico Tronconi, et. al., Dynamic investigation of the role of the surface sulfates in NOx reduction and SO2 oxidation over V_2O_5-WO3/TiO_2 catalysts[J], Ind. Eng. Chem. Res., 1998,37(6): 2350-2359
[18] Carlo Orsenigo, Alessandra Beretta, Pio Forzatti, et. al., Theretical and experimental study of the interaction between NOx reduction and SO2 oxidation over DeNOx-SCR catalysts[J], Catalysis Today, 1996, 27: 15-21
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[1] Guido Busca, Luca Lietti, Gianguido Ramis and Francesco Berti, chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: a review[J], Applied catalysis B: Environmental, 1998, 18: 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Miroslav Radojevic, Reduction of nitrogen oxides in flue gas[J], Environmental pollution, 1998, 102(S1): 685-689
[4] Michael D. Amiridis, Robert V. Duevel and Israel E. Wachs, The effect of metal oxide addictive on the activity of V_2O_5/TiO_2 catalysts for the selective catalytic reduction of nitric oxide by ammonia[J], Applied catalysis B: Environmental, 1999, 20: 111-122
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[6] G. Ramis, G. Busca, C. Cristiani, et. al., Characterization of tungsta-titania catalysts[J], Langmuir, 1992, 8 (7): 1744-1749
[7] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155, 117-130
[8] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[9] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[10] Erich Hums and Herbert E. Gobel, Effects of As2O3 on the phase composition of V_2O_5-MoO3-TiO_2(anatase) DeNOx catalysts[J], Ind. Eng. Chem. Res., 1991,30(8): 1814-1818
[11] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
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[13] Hiroyuki Kamata, Katsumi Takahashi and C. U. Ingemar Odenbrand, The role of K2O in the selective reduction of NO with NH3 over a V_2O_5(WO3)/TiO_2 commercial selective catalytic reduction catalyst[J], Journal of Molecular Catalysis A: General, 1999, 139: 189-198
[14] Chen, Jianping, Preparation, Characterization and deactivation of the catalysts for the selective catalytic reduction of NO with NH3[D]: Ph. D. dissertation, State University of New York at Baffalo, 1993
[15] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[16] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], Catalysis today, 1996, 29: 143-148
[17] 向德辉,二氧化硫氧化用钒催化剂的进展[J],硫酸工业,1981 年 01 期
[18] Went, Gregory Thomas, Study of supported vanadium oxide catalysts for the selective catalytic reduction of nitrogen oxides[D]: Ph. D. dissertation, University of Califonia, Berkeley, 1991
[1] L. Lietti, J. L. Alemany, P. Forzatti, et. al., Reactivity of V_2O_5-WO_3/TiO_2 catalysts in the selective catalytic reduction of nitric oxide by ammonia[J], catalysis today, 1996, 29: 143-148
[2] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[3] G. Ramis, G. Busca, C. Cristiani, et. al., Characterization of tungsta-titania catalysts[J], Langmuir, 1992, 8 (7): 1744-1749
[4] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155: 117-130
[5] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
[6] M. A. Reiche, T. Bürgi, A. Baiker, et. al., Vanadia and tungsta grafted on TiO_2: influence of the grafting sequence on structural and chemicperties[J], Applied catalysis A: general, 2000, 198: 155-169
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[11] E. Tronconi, L. Lietti, P. Forzatti, et. al., Experimental and theoretical investigation of the dynamicsof the SCR-DeNOx reaction[J], Chemical Engineering Science, 1996, 51(11): 2965-2970
[12] C. U. Ingemar Odenbrand, Ana Bahamonde, Pedro Avila, et. al., Kinetic study of the selective reduction of nitric oxide over vanadia-tungsta-titania/sepiolite catalyst[J], Applied Catalysis B: Environmental, 1994, 5: 117-131
[13] 孙康编著,宏观反应动力学及其解析方法[M],冶金工业出版社,1998
[14] 郭汉贤著,应用化工动力学[M],化学工业出版社,2003
[15] Carlo Orsenigo, Alessandra Beretta, Pio Forzatti, et. al., Theretical and experimental study of the interaction between NOx reduction and SO2 oxidation over DeNOx-SCR catalysts[J], Catalysis Today, 1996, 27: 15-21
[16] Jiri Svachula, Louis J. Alemany, Natale Ferlazzo, Pio Forzatti , et. al., Oxidation of SO2 to SO3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 32(5): 826-834
[17] Enrico Tronconi, Andra Cavanna, Carlo Orsenigo and Pio Forzatti, Transient kinetics of SO2 oxidation over SCR-DeNOx monolith catalysts[J], ind. Eng. Chem. Res., 1999, 28(7): 2593-2598
[18] Shimpel Kurmura and Hiroshi Kuroda, Deposition of ammonium bisulfate in the selective catalytic reduction of nitrogen oxides with ammonia[J], Ind. Eng. Chem. Prod. Res. Dev., 1982, 21(1): 48-52
[19] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[20] Akira Miyamoto, Kan Kobayashi, Mokoto Inomata, et. al., Nitrogen-15 tracer investigation of the mechanism of the reduction of NO with NH3 on vanadium oxide catalysts[J], J. Phys. Chem., 1982, 86(15): 2945-2950
[21] J. A. Dumesic, N. Y. Topsoe, H. Topsoe, et. al., Kinetics of selective catalytic reduction of nitric oxide by ammonia over Vanadia/Titania[J], Journal of catalysis, 1996, 163: 409-417
[22] John Marangozis, Comparison and analysis of intrinsic kinetics and effectiveness factors for the catalytic reduction of NO with ammonia in the presence of oxygen[J], Ind. Eng. Chem. Res., 1992, 31(4): 987-994
[23] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[24] C. U. Ingemar Odenbrand, Ana Bahamonde, Pedro Avila, et. al., Kinetic study of the selective reduction of nitric oxide over vanadia-tungsta-titania/sepiolite catalyst[J], Applied Catalysis B: Environmental, 1994, 5: 117-131
[25] Went, Gregory Thomas, Study of supported vanadium oxide catalysts for the selective catalytic reduction of nitrogen oxides[D], Ph. D, University of Califonia, Berkeley, 1991
[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[4] Mokoto Inomata, Akira Miyamoto, Toshiaki Ul, et. al., Activities of V_2O_5/TiO_2 and V_2O_5/Al2O3 catalysts for the reduction of NO and NH3 in the presence of O2[J], Ind. Eng. Che. Prod. Res. Dev., 1982, 21(3): 424-428
[5] R. Q. Long, R. T. Yang, Selective catalytic reduction of NO with ammonia over V_2O_5 doped TiO_2 clay catalysts[J], Applied catalysis B: Environmental, 2000, 24:13-21
[6] Enrico Tronconi, Interaction between chemical kinetics and transport phenomena in monolithic catalysts[J], catalysis today, 1997, 34: 421-427
[7] Enrico Tronconi, The role of inter- and intra-phase mass transfer in the SCR-DeNOx reaction over catalysts of different shapes[J], catalysis today, 1999, 52: 249-258
[8] 山中龙雄,催化剂的有效实际应用[M],化学工业出版社,1988
[9] 朱丙辰编著,化学反应工程(第三版)[M],化学工业出版社教材出版中心,2001
[10] M. 贝伦斯等,化学反应工程(第二版)[M],中国石化出版社,1994
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[12] Ho Jeong Chae, Soo Tae Choo, Hoon Choi, et. al., Direct use of kinetic parameters for modeling and simulation of a selective catalytic reduction process[J], Ind. Eng. Chem. Res., 2000, 39(5): 1159-1170
[13] H. 斯科特·福格勒著,李术元 朱建华译,化学反应工程(原著第三版)(Elements of Chemical Reaction Engineering, Third Edition, H. Scott Gogler)[M],化学工业出版社工业装备与信息工程出版中心
[14] 孙康编著,宏观反应动力学及其解析方法[M],冶金工业出版社,1998
[15] 郭汉贤著,应用化工动力学[M],化学工业出版社,2003
[16] 宋占龙,加压煤气化钙基脱硫剂还原脱硫及硫化钙氧化的研究[D]:博士学位论文,东南大学,2006
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[20] Ana Bahamonde, Alessandra Beretta, Pedro Avila and Enrico Tronconi, An experimental and theoretical investigation of the behavior of a monolithic Ti-V-W-sepiolite catalyst in the reduction of NOx with NH3[J], Ind. Eng. Chem. Res., 196, 35(8): 2516-2521
[21] 许越主编,催化剂设计与制备工艺[M],化学工业出版社化学应用化学出版中心,2003
[1] Guido Busca, Luca Lietti, Gianguido Ramis, Francesco Berti, Chemical and Mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J], Applied Catalysis B: Environmental 18 (1998): 1-36
[2] Pio Forzatti, Present status and perspectives in de-NOx SCR catalysis[J], Applied catalysis A: general, 2001, 222: 221-236
[3] Miroslav Radojevic, Reduction of nitrogen oxides in flue gas[J], Environmental pollution, 1998, 102(S1): 685-689
[4] Jiri Svachula, Natale Ferlazzo, Pio Forzatti, et. al., Selective reduction of NOx by NH_3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 12(6): 1053-1060
[5] Marek A. Buzzanowski and Ralph T. Yang, Simple Design of Monolith Reactor for selective reduction of NO for power plant emission control[J], Ind. Eng. Chem. Res., 1990, 29: 2074-2078
[6] Pio Forzatti, Daniele Ballardini and Lorenzo Sighicelli, Preparation and characterization of extruded monolithic ceramic catalysts[J], Catalysis Today, 1998, 41:87-94
[7] Jean W. Beeckman and L. Louis Hegedus, Design of monolith catalysts for power plant NOx emmision control[J], Ind. Eng. Chem. Res., 1991, 30: 969-978
[8] A. B. 司梯勒斯,催化剂生产-实验室与工业制备[M],华东化工学院出版社,1991
[9] 朱洪法编,催化剂成型[M],中国石化出版社,1992 年 1 月第一版
[10] G. 庞斯莱特等编[比],催化剂的制备 III 制备非均相催化剂的科学基础[M],化学工业出版社,1991
[11] 许越主编,催化剂设计与制备工艺[M],化学工业出版社化学应用化学出版中心,2003
[12] 张继光主编,催化剂制备过程技术[M],中国石化出版社,2004
[13] Michael D. Amiridis, Robert V. Duevel and Israel E. Wachs, The effect of metal oxide addictive on the activity of V_2O_5/TiO_2 catalysts for the selective catalytic reduction of nitric oxide by ammonia[J], Applied catalysis B: Environmental, 1999, 20: 111-122
[14] Hiroyuki Kamata, Katsumi Takahashi and C. U. Ingemar Odenbrand, The role of K_2O in the selective reduction of NO with NH3 over a V_2O_5(WO3)/TiO_2 commercial selective catalytic reduction catalyst[J], Journal of Molecular Catalysis A: General, 1999, 139: 189-198
[15] Ronald J. Willey, John W. Eldridge and J. R. Kittrell, Mechanistic model of the selective catalytic reduction of nitric oxide with ammonia[J], Ind. Eng. Chem. Prod. Res. Dev., 1985, 24(2): 226-233
[16] Ho Jeong Chae, Soo Tae Choo, Hoon Choi, et. al., Direct use of kinetic parameters for modeling and simulation of a selective catalytic reduction process[J], Ind. Eng. Chem. Res., 2000, 39(5): 1159-1170
[17] Luca Lietti, Isabella Nova, Gianguido Ramis, et. al., Characterization and reactivity of V_2O_5-MoO3/TiO_2 De-NOx SCR catalysts[J], Journal of catalysis, 1999, 187: 419-435
[18] G. Ramis, G. Busca, C. Cristiani, et. al., Characterization of tungsta-titania catalysts[J], Langmuir, 1992, 8 (7), 1744-1749
[19] Luis J. Alemany, Luca Lietti, Natale Ferlazzo, et. al., Reactivity and physicochemical characrerization of V_2O_5-WO3/TiO_2 De-NOx catalysts[J], Journal of Catalysis, 1995, 155: 117-130
[20] Luis J. Alemany, Francesco Berti, Guido Busca, et. al., characterization and composition V_2O_5-WO3-TiO_2 SCR catalysts[J], Applied catalysis B: Environmental, 1996, 10: 299-311
[21] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[22] John Marangozis, Comparison and analysis of intrinsic kinetics and effectiveness factors for the catalytic reduction of NO with ammonia in the presence of oxygen[J], Ind. Eng. Chem. Res., 1992, 31(4): 987-994
[23] J. A. Dumesic, N. Y. Topsoe, H. Topsoe, et. al., Kinetics of selective catalytic reduction of nitric oxide by ammonia over Vanadia/Titania[J], Journal of catalysis, 1996, 163: 409-417
[1] Guido Busca, Luca Lietti, Gianguido Ramis and Francesco Berti, chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: a review[J], Applied catalysis B: Environmental, 1998, 18: 1-36
[2] J. A. Dumesic, N. Y. Topsoe, H. Topsoe, et. al., Kinetics of selective catalytic reduction of nitric oxide by ammonia over Vanadia/Titania[J], Journal of catalysis, 1996, 163: 409-417
[3] John Marangozis, Comparison and analysis of intrinsic kinetics and effectiveness factors for the catalytic reduction of NO with ammonia in the presence of oxygen[J], Ind. Eng. Chem. Res., 1992, 31(4): 987-994
[4] Isabella Nova, Luca Lietti, Enrico Tronconi and Pio Forzatti, Dynamics of SCR reaction over TiO_2-supported vanadia-tungsta commercial catalyst[J], catalysis today, 2000, 60: 73-82
[5] Jiri Svachula, Natale Ferlazzo, Pio Forzatti, et. al., Selective reduction of NOx by NH3 over honeycomb DeNOxing catalysts[J], Ind. Eng. Chem. Res., 1993, 12(6): 1053-1060
[6] Ana Bahamonde, Alessandra Beretta, Pedro Avila and Enrico Tronconi, An experimental and theoretical investigation of the behavior of a monolithic Ti-V-W-sepiolite catalyst in the reduction of NOx with NH3[J], Ind. Eng. Chem. Res., 196, 35(8): 2516-2521
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