Skip to main content
Log in

Mesoporous SiO2–Al2O3 supported chromium sesquioxide catalyst for cyclohexane nitrosation to ε-caprolactam with high selectivity

  • Published:
Reaction Kinetics, Mechanisms and Catalysis Aims and scope Submit manuscript

Abstract

Mesoporous SiO2–Al2O3 supported Cr2O3 catalysts were prepared by the sol–gel and impregnation methods. These catalysts were characterized and applied in cyclohexane nitrosation reaction. The effects of the preparation conditions and the catalyst deactivation were studied. The results show that 20% Cr2O3/SiO2–Al2O3 catalyst calcined at 400 °C exhibits not only the larger surface area, smaller particle size, but also the larger amount of Cr2+ and Brønsted acid sites. These catalysts show good catalytic performances in the cyclohexane nitrosation to ε-caprolactam and could be recycled for several times in this reaction system for the first time. The catalyst of Cr2O3/SiO2–Al2O3 calcined at 400 °C gives 10.8% conversion with 79.9% selectivity to ε-caprolactam.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  1. Yamamoto S, Sakaguchi S, Ishii Y (2003) Green Chem 5:300–302

    Article  CAS  Google Scholar 

  2. Ichihashi H, Sato H (2001) Appl Catal A Gen 221:359–366

    Article  CAS  Google Scholar 

  3. Brand U, Schmitz R, Deuker E, Fuchs H (1989) US Patent 4 806 638

  4. Yuan HX, Xia QH, Zhan HJ, Lu XH, Su KX (2006) Appl Catal A Gen 304:178–184

    Article  CAS  Google Scholar 

  5. Anilkumar M, Hoelderich WF (2012) J Catal 293:76–84

    Article  CAS  Google Scholar 

  6. Anilkumar M, Hoelderich WF (2011) Catal Today 98:289–294

    Google Scholar 

  7. Opanasenko M, Shamzhy M, Lamač M, Čejka J (2013) Catal Today 204:94–100

    Article  CAS  Google Scholar 

  8. Zhang D, Wang R, Wang L, Yang X (2013) J Mol Catal A Chem 366:179–185

    Article  CAS  Google Scholar 

  9. Vaschetto EG, Casuscelli SG, Eimer GA (2016) Micropor Mesopor Mater 221:175–185

    Article  CAS  Google Scholar 

  10. Bordoloi A, Halligudi SB (2010) Appl Catal A Gen 379:141–147

    Article  CAS  Google Scholar 

  11. Cesana A, Palmery S, Buzzoni R, Spanò G, Rivetti F, Carnelli L (2010) Catal Today 154:264–270

    Article  CAS  Google Scholar 

  12. Zhang D, Wang R, Yang X, Yao W (2010) React Kinet Catal Lett 101:455

    Article  CAS  Google Scholar 

  13. Zhao W, Salame P, Herledan V, Launay F, Gédéon A, Qi T (2010) J Porous Mater 17:335–340

    Article  Google Scholar 

  14. Anilkumar M, Hoelderich WF (2015) Appl Catal B Environ 165:87–93

    Article  CAS  Google Scholar 

  15. Li L, Liu B, Wu Z, Yuan X, Luo H (2015) Chem Eng J 280:670–676

    Article  CAS  Google Scholar 

  16. Xue X, Song F, Ma B, Yu Y, Li C, Ding Y (2013) Catal Commun 33:61–65

    Article  CAS  Google Scholar 

  17. Lin J, Xin F, Yang L, Zhuang Z (2014) Catal Commun 45:104–108

    Article  CAS  Google Scholar 

  18. Dong C, Wang K, Zhang JS, Luo GS (2015) Chem Eng Sci 126:633–640

    Article  CAS  Google Scholar 

  19. Raja R, Sankar G, Thomas JM (2001) J Am Chem Soc 123:8153–8154

    Article  CAS  PubMed  Google Scholar 

  20. Thomas JM, Raja R (2005) Proc Natl Acad Sci USA 102:13732–13736

    Article  CAS  PubMed  Google Scholar 

  21. Naylor MA, Anderson AW (1953) J Org Chem 18:115–119

    Article  CAS  Google Scholar 

  22. Wang H, Hu R, Yang Y, Gao M, Wang Y (2015) Catal Commun 70:6–11

    Article  CAS  Google Scholar 

  23. Yan Y, Liu S, Hao F, Liu P, Luo H (2014) Catal Commun 50:9–12

    Article  CAS  Google Scholar 

  24. Liu S, Hao F, Liu P, Luo H (2015) RSC Adv 5:22863–22868

    Article  CAS  Google Scholar 

  25. You KY, Wu BH, Mao LQ, Yin DL, Liu PL, Luo HA (2007) Catal Lett 118:129–133

    Article  CAS  Google Scholar 

  26. You KY, Mao LQ, Chen L, Yin DL, Liu PL, Luo HA (2008) Catal Commun 9:2136–2139

    Article  CAS  Google Scholar 

  27. Mao LQ, Chen L, Wu BH, Yin DL, You KY, Liu PL, Luo HA (2008) Chem Res Chin Univ 24:246–248

    Article  CAS  Google Scholar 

  28. Liu PL, Xie H, You KY, Hao F, Li XF, Luo HA (2010) Catal Lett 136:150–154

    Article  CAS  Google Scholar 

  29. Hao F, Zhong J, Liu PL, You KY, Wei C, Liu HJ, Luo HA (2011) J Mol Catal A Chem 351:210–216

    Article  CAS  Google Scholar 

  30. Hao F, Zhong J, Liu PL, You KY, Luo HA (2012) J Mol Catal A Chem 363–364:41–48

    Article  CAS  Google Scholar 

  31. Hao F, Liu PL, You KY, Luo HA (2014) Mater Res Innov 18:321–325

    Article  CAS  Google Scholar 

  32. Li Z, Meng F, Ren J, Zheng H, Xie K (2008) Chin J Catal 29:643–648

    Article  CAS  Google Scholar 

  33. Cao J, Xu Y, Sui L, Zhang X, Gao S, Cheng X, Zhao H, Huo L (2015) Sensor Actuat B 220:910–918

    Article  CAS  Google Scholar 

  34. Chen D, Huang A, Gu H, Zhang M, Shao Z (2015) Ceram Int 41:14748–14753

    Article  CAS  Google Scholar 

  35. Gibot P, Schnell F, Spitzer D (2015) Mater Lett 161:172–174

    Article  CAS  Google Scholar 

  36. Dolle P, Alnot M, Ehrhardt JJ, Cassuto A (1979) J Electron Spectrosc Relat Phenom 17:299–321

    Article  CAS  Google Scholar 

  37. Kumar GM, Ilanchezhiyan P, Kawakita J, Subramanianc M, Jayavel R (2010) Cryst Eng Commun 12:1887–1892

    Article  CAS  Google Scholar 

  38. Mischle S, Mathieu HJ, Landolt D (1988) Surf Interface Anal 11:182–188

    Article  Google Scholar 

  39. Jacobs PA, Beyer HK (1979) J Phys Chem 83:1174–1177

    Article  CAS  Google Scholar 

  40. Fritz PO, Lunsford JH (1989) J Catal 118:85–98

    Article  CAS  Google Scholar 

  41. Lónyi F, Lunsford JH (1992) J Catal 136:566–577

    Article  Google Scholar 

  42. Makarova MA, Garforth A, Zholobenko VL, Dwyer J, Earl GJ, Rawlence D (1994) Stud Surf Sci Catal 84:365–372

    Article  CAS  Google Scholar 

  43. Lischke G, Parlitz B, Schreier UL, Fricke R (1998) Appl Catal A Gen 166:351–361

    Article  CAS  Google Scholar 

  44. Bertoluzza A, Fagbabo C, Morelli MA, Gottadri V, Guglielmi M (1982) J Non-Cryst Solids 48:117–128

    Article  CAS  Google Scholar 

  45. Barrett PA, Sankar G, Catlow CRA, Thomas JM (1996) J Phys Chem 100:8977–8985

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by NSFC (U1662127, 21306160), Project of Hunan Provincial Natural Science Foundation of China (2016JJ2123, 2018JJ3497), Project of Hunan provincial Education Department (17C1525), and Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Wei Xiong.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (PDF 723 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Hao, F., Yang, Y., Xiong, W. et al. Mesoporous SiO2–Al2O3 supported chromium sesquioxide catalyst for cyclohexane nitrosation to ε-caprolactam with high selectivity. Reac Kinet Mech Cat 125, 199–211 (2018). https://doi.org/10.1007/s11144-018-1397-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11144-018-1397-x

Keywords

Navigation