Advertisement

Key role of NO + C3H8 reaction for the elimination of NO in automobile exhaust by three-way catalyst

  • Yusheng Chen
  • Jie Deng
  • Jun Fan
  • Yi Jiao
  • Jianli WangEmail author
  • Yaoqiang ChenEmail author
Research Article
  • 34 Downloads

Abstract

Pd-only three-way catalysts with improved catalytic activity for NO elimination were prepared. In order to explore the catalytic reaction rules of NO reduction under a three-way catalytic system, a series of single reactions related to NO reduction were evaluated. It was found that the reaction temperatures of NO + H2 or NO + CO or NO + C3H6 reactions were below 250 °C, while that of NO + C3H8 was up to 350 °C. Thus, the reaction NO + C3H8 served as the key reaction in determining the purification efficiency of NO at the high-temperature stage. By in situ FTIR, we proposed that three possible steps were involved in NO + C3H8 reaction. The first step was the oxidation of C3H8 and NO to acetone and nitrate species by active oxygen species, respectively (C3H8 + O* → C3H6O, NO + O* → NO3). XPS results revealed that the amount of active oxygen species in Pd/CeO2-ZrO2-Al2O3 (Pd/CZA, 73.7%) was much higher than that in Pd/CexZr1−xO2+Al2O3 (Pd/CZ+A, 64.1%). This was in line with the higher reaction efficiency of the first step over Pd/CZA. Then the NO + C3H8 reaction was accelerated by the first step, which consequently contributed to the higher NO elimination efficiency of Pd/CZA.

Keywords

Three-way catalyst NO elimination Single reaction Reaction steps Active oxygen species 

Notes

Funding information

We gratefully acknowledge the National Key Research and Development Program of China (2016YFC0204903) for their generous financial support to our research.

Supplementary material

11356_2019_5834_MOESM1_ESM.docx (234 kb)
ESM 1 (DOCX 234 kb)

References

  1. Andonova S, Marchionni V, Lietti L, Olsson L (2017) Micro-calorimetric studies of NO2 adsorption on Pt/BaO-supported on γ-Al2O3 NOx storage and reduction (NSR) catalysts—Impact of CO2. Mol Catal 436:43–52CrossRefGoogle Scholar
  2. Burch R, Coleman MD (1999) An investigation of the NO/H2/O2 reaction on noble-metal catalysts at low temperatures under lean-burn conditions. Appl Catal B 23:115–121CrossRefGoogle Scholar
  3. Burch R, Watling TC (1998) The effect of sulphur on the reduction of NO by C3H6 and C3H8 over Pt/Al2O3 under lean-burn conditions. Appl Catal B 17:131–139CrossRefGoogle Scholar
  4. Chajar Z, Primet M, Praliaud H (1998) Comparison of the C3H8 oxidation by NO or by O2 on copper-based catalysts. J Catal 180:279–283CrossRefGoogle Scholar
  5. Cheng X, Zhu A, Zhang Y, Wang Y, Au CT, Shi C (2009) A combined DRIFTS and MS study on reaction mechanism of NO reduction by CO over NiO/CeO2 catalyst. Appl Catal B 90:395–404CrossRefGoogle Scholar
  6. Ciambelli P, Corbo P, Migliardini F (2000) Potentialities and limitations of lean de-NOx catalysts in reducing automotive exhaust emissions. Catal Today 59:279–286CrossRefGoogle Scholar
  7. Dasireddy VDBC, Likozar B (2017) Selective catalytic reduction of NOx by CO over bimetallic transition metals supported by multi-walled carbon nanotubes (MWCNT). Chem Eng J 326:886–900CrossRefGoogle Scholar
  8. Epling WS, Campbell LE, Yezerets A, Currier NW, Parks JE (2004) Overview of the fundamental reactions and degradation mechanisms of NOx storage/reduction catalysts. Catal Rev 46:163–245CrossRefGoogle Scholar
  9. Fan J, Wu X, Yang L, Weng D (2007) The SMSI between supported platinum and CeO2–ZrO2–La2O3 mixed oxides in oxidative atmosphere. Catal Today 126:303–312CrossRefGoogle Scholar
  10. Finocchio E, Busca G, Lorenzelli V (1994) FTIR studies on the selective oxidation and combustion of light hydrocarbons at metal oxide surfaces. J Chem Soc Faraday Trans 90:3347–3356CrossRefGoogle Scholar
  11. Gandhi HS, Graham GW, McCabe RW (2003) Automotive exhaust catalysis. J Catal 216:433–442CrossRefGoogle Scholar
  12. Hadjiivanov K, Knözinger H (2000) Species formed after NO adsorption and NO + O2 co-adsorption on TiO2: an FTIR spectroscopic study. Phys Chem Chem Phys 2:2803–2806CrossRefGoogle Scholar
  13. Hadjiivanov K, Knözinger H, Tsyntsarski B, Dimitrov L (1999) Effect of water on the reduction of NOx with propane on Fe-ZSM-5. An FTIR mechanistic study. Catal Lett 62:35–40CrossRefGoogle Scholar
  14. Haneda M, Shinoda K, Nagane A, Houshito O, Takagi H, Nakahara Y, Hiroe K, Fujitani T, Hamada H (2008) Catalytic performance of rhodium supported on ceria–zirconia mixed oxides for reduction of NO by propene. J Catal 259:223–231CrossRefGoogle Scholar
  15. Haneda M, Tomida Y, Takahashi T, Azuma Y, Fujimoto T (2017) Three-way catalytic performance and change in the valence state of Rh in Y- and Pr-doped Rh/ZrO2 under lean/rich perturbation conditions. Catal Commun 90:1–4CrossRefGoogle Scholar
  16. Hosokawa S, Matsuki K, Tamaru K, Oshino Y, Aritani H, Asakura H, Teramura K, Tanaka T (2017) Selective reduction of NO over Cu/Al2O3: enhanced catalytic activity by infinitesimal loading of Rh on Cu/Al2O3. Mol Catal 442:74–82CrossRefGoogle Scholar
  17. Jirátová K, Mikulová J, Klempa J, Grygar T, Bastl Z, Kovanda F (2009) Modification of Co–Mn–Al mixed oxide with potassium and its effect on deep oxidation of VOC. Appl Catal A 361:106–116CrossRefGoogle Scholar
  18. Kang SB, Nam I-S, Cho BK, Kim CH, Oh SH (2015) Universal activity function for predicting performance of Pd-based TWC as function of Pd loading and catalyst mileage. Chem Eng J 259:519–533CrossRefGoogle Scholar
  19. Kašpar J, Fornasiero P, Hickey N (2003) Automotive catalytic converters: current status and some perspectives. Catal Today 77:419–449CrossRefGoogle Scholar
  20. Kobayashi T, Yamada T, Kayano K (2001) Effect of basic metal additives on NOx reduction property of Pd-based three-way catalyst. Appl Catal B 30:287–292CrossRefGoogle Scholar
  21. Li X, Chen J, Lin P, Meng M, Fu Y, Tu J, Li Q (2004) A study of the NOx storage catalyst of Ba–Fe–O complex oxide. Catal Commun 5:25–28CrossRefGoogle Scholar
  22. Li L, Shen Q, Cheng J, Hao Z (2010) Catalytic oxidation of NO over TiO2 supported platinum clusters. II: mechanism study by in situ FTIR spectra. Catal Today 158:361–369CrossRefGoogle Scholar
  23. Lin S, Yang L, Yang X, Zhou R (2014) Redox behavior of active PdOx species on (Ce,Zr)xO2–Al2O3 mixed oxides and its influence on the three-way catalytic performance. Chem Eng J 247:42–49CrossRefGoogle Scholar
  24. Papavasiliou A, Tsetsekou A, Matsouka V, Konsolakis M, Yentekakis IV, Boukos N (2009) Development of a Ce–Zr–La modified Pt/γ-Al2O3 TWCs’ washcoat: effect of synthesis procedure on catalytic behaviour and thermal durability. Appl Catal B 90:162–174CrossRefGoogle Scholar
  25. Roy S, Hegde MS, Madras G (2009) Catalysis for NOx abatement. Appl Energy 86:2283–2297CrossRefGoogle Scholar
  26. Ryou Y, Lee J, Lee H, Kim CH, Kim DH (2018) Low temperature NO adsorption over hydrothermally aged Pd/CeO2 for cold start application. Catal Today 307:93–101CrossRefGoogle Scholar
  27. Salem I, Courtois X, Corbos EC, Marecot P, Duprez D (2008) NO conversion in presence of O2, H2O and SO2: improvement of a Pt/Al2O3 catalyst by Zr and Sn, and influence of the reducer C3H6 or C3H8. Catal Commun 9:664–669CrossRefGoogle Scholar
  28. Shen M, Yang M, Wang J, Wen J, Zhao M, Wang W (2009) Pd/support interface-promoted Pd-Ce0.7Zr0.3O2-Al2O3 automobile three-way catalysts: studying the dynamic oxygen storage capacity and CO, C3H8, and NO conversion. J Phys Chem C 113:3212–3221CrossRefGoogle Scholar
  29. Shimizu KI, Kawabata H, Satsuma A, Hattori T (1999) Role of acetate and nitrates in the selective catalytic reduction of NO by propene over alumina catalyst as investigated by FTIR. J Phys Chem B 103:5240–5245CrossRefGoogle Scholar
  30. Shimizu K, Shibata J, Yoshida H, Satsuma A, Hattori T (2001) Silver-alumina catalysts for selective reduction of NO by higher hydrocarbons: structure of active sites and reaction mechanism. Appl Catal B 30:151–162CrossRefGoogle Scholar
  31. Shimizu K, Sugino K, Kato K, Yokota S, Okumura K, Satsuma A (2007) Reaction mechanism of H2-promoted selective catalytic reduction of NO with C3H8 over Ag-MFI zeolite. J Phys Chem C 111:6481–6487CrossRefGoogle Scholar
  32. Toyao T, Jing Y, Kon K, Hayama T, Nagaoka S, Shimizu K (2018) Catalytic NO-CO reactions over La-Al2O3 supported Pd: promotion effect of La. Chem Lett 47:1036–1039CrossRefGoogle Scholar
  33. Twigg MV (2007) Progress and future challenges in controlling automotive exhaust gas emissions. Appl Catal B 70:2–15CrossRefGoogle Scholar
  34. Twigg MV (2011) Catalytic control of emissions from cars. Catal Today 163:33–41CrossRefGoogle Scholar
  35. Ueda K, Ohyama J, Satsuma A (2017) Investigation of reaction mechanism of NO–C3H6–CO–O2 reaction over NiFe2O4 catalyst. ACS Omega 2:3135–3143CrossRefGoogle Scholar
  36. Wang X, Yu Y, He H (2011) Effects of temperature and reductant type on the process of NOx storage reduction over Pt/Ba/CeO2 catalysts. Appl Catal B 104:151–160CrossRefGoogle Scholar
  37. Wang Y, Ge C, Zhan L, Li C, Qiao W, Ling L (2012) MnOx–CeO2/activated carbon honeycomb catalyst for selective catalytic reduction of NO with NH3 at low temperatures. Ind Eng Chem Res 51:11667–11673CrossRefGoogle Scholar
  38. Wang J, Chen H, Hu Z, Yao M, Li Y (2014) A review on the Pd-based three-way catalyst. Catal Rev 57:79–144CrossRefGoogle Scholar
  39. Wang S, Sun M, Huang M, Cheng T, Wang J, Yuan S, Chen Y (2017) Enhanced thermal stability of CeO2-ZrO2-Nd2O3 composite by adding surfactant and its supported Rh-only three-way catalyst. Mol Catal 433:162–169CrossRefGoogle Scholar
  40. Weng X, Zhang J, Wu Z, Liu Y, Wang H, Darr JA (2011) Continuous syntheses of highly dispersed composite nanocatalysts via simultaneous co-precipitation in supercritical water. Appl Catal B 103:453–461CrossRefGoogle Scholar
  41. Wang X, Kang Q, Li D (2009) Catalytic combustion of chlorobenzene over MnOx–CeO2 mixed oxide catalysts. Appl Catal B 86:166–175Google Scholar
  42. Yang L, Lin S, Yang X, Fang W, Zhou R (2014) Promoting effect of alkaline earth metal doping on catalytic activity of HC and NOx conversion over Pd-only three-way catalyst. J Hazard Mater 279:226–235CrossRefGoogle Scholar
  43. Yang L, Yang X, Zhou R (2016) Probing BaO doping effect on the structure and catalytic performance of Pd/CexZr1–xO2 (x=0.2–0.8) catalysts for automobile emission control. J Phys Chem C 120:2712–2723CrossRefGoogle Scholar
  44. Yoon DY, Kim YJ, Lim JH, Cho BK, Hong SB, Nam I-S, Choung JW (2015) Thermal stability of Pd-containing LaAlO3 perovskite as a modern TWC. J Catal 330:71–83CrossRefGoogle Scholar
  45. Zhang Z, Fan Y, Xin Y, Li Q, Li R, Anderson JA, Zhang Z (2015) Improvement of air/fuel ratio operating window and hydrothermal stability for Pd-only three-way catalysts through a Pd-Ce2Zr2O8 superstructure interaction. Environ Sci Technol 49:7989–7995CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.College of ChemistrySichuan UniversityChengduChina
  2. 2.Institute of New Energy and Low-Carbon TechnologySichuan UniversityChengduChina
  3. 3.National Engineering Research Center for Flue Gas DesulfurizationSichuan UniversityChengduChina

Personalised recommendations