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Effect of iron loading on the performance and structure of Fe/ZSM-5 catalyst for the selective catalytic reduction of NO with NH3

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Abstract

A series of Fe/ZSM-5 catalysts with different Fe contents were prepared by impregnation method. The catalysts were characterized by TEM, XRD, H2 temperature-programed reduction (H2-TPR), temperature-programed desorption of ammonia (NH3-TPD), and in situ diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS), and the catalytic activity test was also carried out on selective catalytic reduction (SCR) denitration device. Results showed that the single metal iron-supported ZSM-5 catalyst has high deNOx activity in the medium–high temperature range, and the optimal loading of Fe active component is 10 wt%; the deNOx efficiency over 80% at the range of 350–450 °C and 431 °C reaches the maximum of 96.91%. Iron species can be finely dispersed on the surface of the carrier as amorphous oxides, and the crystalline structure of zeolite is retained. The significant redox performance, highly dispersed nanoparticles, and rich Lewis acid sites on the surface of catalyst are favorable for the SCR denitration reaction. Fe/ZSM-5 10 wt% catalyst has rich Lewis acid sites and less B acid sites and Lewis acidic sites play an important role during the reaction. Only Eley–Rideal (E-R) mechanism existed during the NH3-SCR reaction process, and there is no denitration reaction being accomplished by L-H mechanism at 150 °C.

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References

  • Acres GJK, Harrison B (2004) The development of catalysts for emission control from motor vehicles: early research at Johnson Matthey. Top Catal 28:3–11

    Article  CAS  Google Scholar 

  • Akah AC, Nkeng G, Garforth AA (2007) The role of Al and strong acidity in the selective catalytic oxidation of NH3 over Fe-ZSM-5. Appl Catal B Environ 74:34–39

    Article  CAS  Google Scholar 

  • And TGD, Kannan MP (2007) X-ray diffraction (XRD) studies on the chemical states of some metal species in cellulosic chars and the Ellingham diagrams. Energy Fuel 21:596–601

    Article  CAS  Google Scholar 

  • Auvray X, Partridge W, Choi J-S, Pihl J, Coehlo F, Yezerets A, Kamasamudram K, Currier N, Olsson L (2015) Kinetic modeling of NH3-SCR over a supported Cu zeolite catalyst using axial species distribution measurements. Appl Catal B Environ 163:393–403

    Article  CAS  Google Scholar 

  • Begum SH, Hung C-T, Chen Y-T, Huang S-J, Wu P-H, Han X, Liu S-B (2016) Acidity-activity correlation over bimetallic iron-based ZSM-5 catalysts during selective catalytic reduction of NO by NH3. J Mol Catal A Chem 423:423–432

    Article  CAS  Google Scholar 

  • Boroń P, Chmielarz L, Gurgul J, Łątka K, Gil B, Krafft J-M, Dzwigaj S (2014) The influence of the preparation procedures on the catalytic activity of Fe-BEA zeolites in SCR of NO with ammonia and N2O decomposition. Catal Today 235:210–225

    Article  CAS  Google Scholar 

  • Brandenberger S, Tissler A, Althoff R (2008) The state of the art in selective catalytic reduction of NO by ammonia using metal-exchanged zeolite catalysts. Catal Rev 50:492–531

    Article  CAS  Google Scholar 

  • Brandenberger S, Kröcher O, Wokaun A, Tissler A, Althoff R (2009) The role of Brønsted acidity in the selective catalytic reduction of NO with ammonia over Fe-ZSM-5. J Catal 268:297–306

    Article  CAS  Google Scholar 

  • Brandenberger S, Kröcher O, Tissler A, Althoff R (2010a) The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH3. Appl Catal B Environ 95:348–357

    Article  CAS  Google Scholar 

  • Brandenberger S, Kröcher O, Tissler A, Althoff R (2010b) The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH3. Appl Catal B Environ 95:348–357

    Article  CAS  Google Scholar 

  • Brandenberger S, Kröcher O, Casapu M, Tissler A, Althoff R (2011) Hydrothermal deactivation of Fe-ZSM-5 catalysts for the selective catalytic reduction of NO with NH3. Appl Catal B Environ 101:649–659

    Article  CAS  Google Scholar 

  • Chen L, Niu X, Li Z, Dong Y, Zhang Z, Yuan F, Zhu Y (2016a) Promoting catalytic performances of Ni-Mn spinel for NH3 -SCR by treatment with SO2 and H2O. Catal Commun 85:48–51

    Article  CAS  Google Scholar 

  • Chen Y, Zhang Z, Liu L, Mi L, Wang X (2016b) In situ DRIFTS studies on MnOx nanowires supported by activated semi-coke for low temperature selective catalytic reduction of NOx with NH3. Appl Surf Sci 366:139–147

    Article  CAS  Google Scholar 

  • Du T, Qu H, Liu Q, Zhong Q, Ma W (2015) Synthesis, activity and hydrophobicity of Fe-ZSM-5@silicalite-1 for NH3-SCR. Chem Eng J 262:1199–1207

    Article  CAS  Google Scholar 

  • Eigenmann F, Maciejewski M, Baiker A (2006) Selective reduction of NO by NH3 over manganese–cerium mixed oxides: relation between adsorption, redox and catalytic behavior. Appl Catal B Environ 62:311–318

    Article  CAS  Google Scholar 

  • Feng B, Wang Z, Sun Y, Zhang C, Tang S, Li X, Huang X (2016) Size controlled ZSM-5 on the structure and performance of Fe catalyst in the selective catalytic reduction of NOx with NH3. Catal Commun 80:20–23

    Article  CAS  Google Scholar 

  • Fierro G, Moretti G, Ferraris G, Andreozzi GB (2011) A Mössbauer and structural investigation of Fe-ZSM-5 catalysts: influence of Fe oxide nanoparticles size on the catalytic behaviour for the NO-SCR by C3H8. Appl Catal B Environ 102:215–223

    Article  CAS  Google Scholar 

  • Gao G, Shi J-W, Liu C, Gao C, Fan Z, Niu C (2017) Mn/CeO2 catalysts for SCR of NOx with NH3 : comparative study on the effect of supports on low-temperature catalytic activity. Appl Surf Sci 411:338–346

    Article  CAS  Google Scholar 

  • Hadjiivanov KI (2000) Identification of neutral and charged NxOy surface species by IR spectroscopy. Catal Rev 42:71–144

    Article  CAS  Google Scholar 

  • Hidalgo CV, Itoh H, Hattori T, Niwa M, Murakami Y (1984) Measurement of the acidity of various zeolites by temperature-programmed desorption of ammonia. J Catal 85:362–369

    Article  CAS  Google Scholar 

  • Hoost TE, Laframboise KA, Otto K (1996) Infrared study of acetone and nitrogen oxides on Cu-ZSM-5. Catal Lett 37:153–156

    Article  CAS  Google Scholar 

  • Iwasaki M, Yamazaki K, Banno K, Shinjoh H (2008) Characterization of Fe/ZSM-5 DeNOx catalysts prepared by different methods: relationships between active Fe sites and NH3-SCR performance. J Catal 260:205–216

    Article  CAS  Google Scholar 

  • Jaan L, Ohlsen JR (2007) Characterization of nitrogen oxides by vibrational spectroscopy. Prog Inorg Chem 27:465–513

    Google Scholar 

  • Jung SM, Demoulin O, Grange P (2005) The study of a synergetic effect over a H-ZSM-5/V2O5 hybrid catalyst on SCR reaction. J Mol Catal A Chem 236:94–98

    Article  CAS  Google Scholar 

  • Krishna K, Makkee M (2006) Preparation of Fe-ZSM-5 with enhanced activity and stability for SCR of NOx. Catal Today 114:23–30

    Article  CAS  Google Scholar 

  • Kumar MS, Schwidder M, Grünert W, Bentrup U, Brückner A (2006) Selective reduction of NO with Fe-ZSM-5 catalysts of low Fe content: part II. Assessing the function of different Fe sites by spectroscopic in situ studies. J Catal 239:173–186

    Article  CAS  Google Scholar 

  • Lai S, She Y, Zhan W, Guo Y, Guo Y, Wang L, Lu G (2016) Performance of Fe-ZSM-5 for selective catalytic reduction of NOx with NH3 : effect of the atmosphere during the preparation of catalysts. J Mol Catal A Chem 424:232–240

    Article  CAS  Google Scholar 

  • Liu F, He H (2010) Structure−activity relationship of iron titanate catalysts in the selective catalytic reduction of NOx with NH3. J Phys Chem C 114:16929–16936

    Article  CAS  Google Scholar 

  • Liu X, Li J, Li X, Peng Y, Wang H, Jiang X, Wang L (2016) NH3 selective catalytic reduction of NO: a large surface TiO2 support and its promotion of V2O5 dispersion on the prepared catalyst. Chin J Catal 37:878–887

    Article  CAS  Google Scholar 

  • Liu J, Li X, Zhao Q, Ke J, Xiao H, Lv X, Liu S, Tadé M, Wang S (2017) Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: in situ FTIR analysis for structure-activity correlation. Appl Catal B Environ 200:297–308

    Article  CAS  Google Scholar 

  • Luo J, Gao F, Kamasamudram K, Currier N, Peden CHF, Yezerets A (2017) New insights into Cu/SSZ-13 SCR catalyst acidity. Part I: nature of acidic sites probed by NH3 titration. J Catal 348:291–299

    Article  CAS  Google Scholar 

  • Ma Z, Wu X, Härelind H, Weng D, Wang B, Si Z (2016) NH3-SCR reaction mechanisms of NbOx/Ce0.75Zr0.25O2 catalyst: DRIFTS and kinetics studies. J Mol Catal A Chem 423:172–180

    Article  CAS  Google Scholar 

  • Pérez Vélez R, Ellmers I, Huang H, Bentrup U, Schünemann V, Grünert W, Brückner A (2014) Identifying active sites for fast NH3-SCR of NO/NO2 mixtures over Fe-ZSM-5 by operando EPR and UV–vis spectroscopy. J Catal 316:103–111

    Article  CAS  Google Scholar 

  • Reddy BM, Khan A (2003) Structural characterization of CeO2−TiO2 and V2O5/CeO2−TiO2 catalysts by Raman and Xps techniques. J Phys Chem B 107:5162–5167

    Article  CAS  Google Scholar 

  • Schwidder M, Kumar MS, Klementiev K, Pohl MM, Brückner A, Grünert W (2005) Selective reduction of NO with Fe-ZSM-5 catalysts of low Fe content : I. relations between active site structure and catalytic performance. J Catal 231:314–330

    Article  CAS  Google Scholar 

  • Shakya BM, Harold MP, Balakotaiah V (2015) Simulations and optimization of combined Fe- and Cu-zeolite SCR monolith catalysts. Chem Eng J 278:374–384

    Article  CAS  Google Scholar 

  • Shi X, Liu F, Shan W, He H (2012a) Hydrothermal deactivation of Fe-ZSM-5 prepared by different methods for the selective catalytic reduction of NOx with NH3. Chin J Catal 33:454–464

    Article  CAS  Google Scholar 

  • Shi X, Liu F, Shan W, Hong HE (2012b) Hydrothermal deactivation of Fe-ZSM-5 prepared by different methods for the selective catalytic reduction of NOx with NH3. Chin J Catal 33:454–464

    Article  CAS  Google Scholar 

  • Shi X, Liu F, Xie L, Shan W, He H (2013) NH3-SCR performance of fresh and hydrothermally aged Fe-ZSM-5 in standard and fast selective catalytic reduction reactions. Environ Sci Technol 47:3293–3298

    Article  CAS  Google Scholar 

  • Shi X, He H, Xie L (2015) The effect of Fe species distribution and acidity of Fe-ZSM-5 on the hydrothermal stability and SO2 and hydrocarbons durability in NH3-SCR reaction. Chin J Catal 36:649–656

    Article  CAS  Google Scholar 

  • Shi Y, Wang X, Xia Y, Sun C, Zhao C, Li S, Li W (2017) Promotional effect of CeO2 on the propene poisoning resistance of HBEA zeolite catalyst for NH3-SCR of NOx. Mol Catal 433:265–273

    Article  CAS  Google Scholar 

  • Usberti N, Jablonska M, Blasi MD, Forzatti P, Lietti L, Beretta A (2015) Design of a “high-efficiency” NH3-SCR reactor for stationary applications. A kinetic study of NH3 oxidation and NH3-SCR over V-based catalysts. Appl Catal B Environ 179:185–195

    Article  CAS  Google Scholar 

  • Vogel W, Knözinger H, Carvill BT, Sachtler WMH, Zhang ZC (1998) Mass diffusion effect in large zeolite Y aggregates on Pd cluster size distribution: a combined in situ EXAFS/XRD study. J Phys Chem B 102:1750–1758

    Article  CAS  Google Scholar 

  • Wang L, Li W, Schmieg SJ, Weng D (2015) Role of Brønsted acidity in NH3 selective catalytic reduction reaction on Cu/SAPO-34 catalysts. J Catal 324:98–106

    Article  CAS  Google Scholar 

  • Weng X, Dai X, Zeng Q, Liu Y, Wu Z (2016) DRIFT studies on promotion mechanism of H3PW12O40 in selective catalytic reduction of NO with NH3. J Colloid Interface Sci 461:9–14

    Article  CAS  Google Scholar 

  • Wijayanti K, Xie K, Kumar A, Kamasamudram K, Olsson L (2017) Effect of gas compositions on SO2 poisoning over Cu/SSZ-13 used for NH3 -SCR. Appl Catal B Environ 219:142–154

    Article  CAS  Google Scholar 

  • Xu L, Li X-S, Crocker M, Zhang Z-S, Zhu A-M, Shi C (2013) A study of the mechanism of low-temperature SCR of NO with NH3 on MnOx/CeO2. J Mol Catal A Chem 378:82–90

    Article  CAS  Google Scholar 

  • Zhang J, Qu H (2014) Low-temperature selective catalytic reduction of NOx with NH3 over Fe–Cu mixed oxide/ZSM-5 catalysts containing Fe2CuO4 phase. Res Chem Intermed 41:4961–4975

    Article  CAS  Google Scholar 

  • Zhang L, Pierce J, Leung VL, Wang D, Epling WS (2013) Characterization of Ceria’s interaction with NOx and NH3. JPhysChemC 117:8282–8289

    CAS  Google Scholar 

  • Zhang B, Liu F, He H, Xue L (2014) Role of aggregated Fe oxo species in N2O decomposition over Fe/ZSM-5. Chin J Catal 35:1972–1981

    Article  CAS  Google Scholar 

  • Zhang T, Qiu F, Li J (2016) Design and synthesis of core-shell structured meso-Cu-SSZ-13@mesoporous aluminosilicate catalyst for SCR of NOx with NH3: enhancement of activity, hydrothermal stability and propene poisoning resistance. Appl Catal B Environ 195:48–58

    Article  CAS  Google Scholar 

  • Zhang L, Du T, Qu H, Chi B, Zhong Q (2017a) Synthesis of Fe-ZSM-5@Ce/mesoporous-silica and its enhanced activity by sequential reaction process for NH3-SCR. Chem Eng J 313:702–710

    Article  CAS  Google Scholar 

  • Zhang X, Ma C, Cheng X, Wang Z (2017b) Performance of Fe-Ba/ZSM-5 catalysts in NO + O2 adsorption and NO + CO reduction. Int J Hydrog Energy 42:7077–7088

    Article  CAS  Google Scholar 

  • Zhao X, Huang L, Li H, Hu H, Han J, Shi L, Zhang D (2015) Highly dispersed V2O5 /TiO2 modified with transition metals (Cu, Fe, Mn, Co) as efficient catalysts for the selective reduction of NO with NH3. Chin J Catal 36:1886–1899

    Article  CAS  Google Scholar 

  • Zhu L, Zhang L, Qu H, Zhong Q (2015) A study on chemisorbed oxygen and reaction process of Fe–CuOx/ZSM-5 via ultrasonic impregnation method for low-temperature NH3-SCR. J Mol Catal A Chem 409:207–215

    Article  CAS  Google Scholar 

  • Zhu L, Zeng Y, Zhang S, Deng J, Zhong Q (2017) Effects of synthesis methods on catalytic activities of CoO x –TiO2 for low-temperature NH3 -SCR of NO. J Environ Sci 54:277–287

    Article  Google Scholar 

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Funding

This work was supported by the National Natural Science Foundation of China (Nos. 50806020, 51506046), Excellent Youth Foundation of Henan Scientific Committee (No. 114100510010), and National Natural Science Foundation of Henan Province (No. 182300410256).

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Authors and Affiliations

  1. Department of Energy and Power Engineering, Henan University of Science and Technology, Luoyang, 471003, China

    Xue-tao Wang, Hai-peng Hu, Xiao-xin Su & Xiao-dong Yang

  2. National Engineering Lab of Coal-fired Pollution Emission Reduction, Shandong University, Jinan, 250061, China

    Xing-yu Zhang

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  1. Xue-tao Wang
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  2. Hai-peng Hu
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  3. Xing-yu Zhang
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  4. Xiao-xin Su
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Correspondence to Xue-tao Wang.

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Responsible editor: Philippe Garrigues

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Wang, Xt., Hu, Hp., Zhang, Xy. et al. Effect of iron loading on the performance and structure of Fe/ZSM-5 catalyst for the selective catalytic reduction of NO with NH3. Environ Sci Pollut Res 26, 1706–1715 (2019). https://doi.org/10.1007/s11356-018-3513-x

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