Skip to main content
Log in

The nitriding of titanium silicate-1 and its effect on gas-phase epoxidation of propylene

  • Chemical routes to materials
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

The nitrogen-containing titanium silicate-1 (N-TS-1) was synthesized to improve the catalytic performance of Au/N-TS-1 in gas-phase epoxidation of propylene. The nitrogen content has an important influence on the activity of the catalyst and can be controlled by adjusting the nitriding temperature and the nitriding time. The propylene oxide (PO) formation rate was promoted from 78.7 gPO/h/kgCat of Au/TS-1 to 138.7 gPO/h/kgCat of Au/N-TS-1 (nitrided at the optimal condition). It was found that the ligand effect of terminal-NH2 caused by nitrogen enrichment increased the Au capture efficiency and the gold loading. And the reduction in the acid amount on the surface of the molecular sieve caused by nitridation reduced the adsorption of PO on the surface of the support.

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.

Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7
Figure 8
Figure 9
Figure 10
Figure 11
Figure 12

Similar content being viewed by others

References

  1. Haruta M (2010) Gold as a low-temperature oxidation catalyst: factors controlling activity and selectivity. Cheminform 29(17):43–47

    Google Scholar 

  2. Russo V, Tesser R, Santacesaria E, Di Serio M (2013) Chemical and technical aspects of propene oxide production via hydrogen peroxide (HPPO Process). Ind Eng Chem Res 52(3):1168–1178

    CAS  Google Scholar 

  3. Lin M, Xia C, Zhu B, Li H, Shu X (2016) Green and efficient epoxidation of propylene with hydrogen peroxide (HPPO process) catalyzed by hollow TS-1 zeolite: a 1.0 kt/a pilot-scale study. Chem Eng J 295:370–375

    CAS  Google Scholar 

  4. Hayashi T, Tanaka K, Haruta M (1998) Selective vapor-phase epoxidation of propylene over Au/TiO2 catalysts in the presence of oxygen and hydrogen. J Catal 178(2):566–575

    CAS  Google Scholar 

  5. Nijhuis TA, Huizinga BJ, Makkee M, Moulijn JA (1999) Direct epoxidation of propene using gold dispersed on TS-1 and other titanium-containing supports. Ind Eng Chem Res 38(3):884–891

    CAS  Google Scholar 

  6. Haruta M (1997) Novel catalysis of gold deposited on metal oxides. Catal Surv Asia 1(1):61–73

    CAS  Google Scholar 

  7. Haruta M (1997) Size-and support-dependency in the catalysis of gold. Catal Today 36(1):153–166

    CAS  Google Scholar 

  8. Haruta M (1997) Gold as a low-temperature oxidation catalyst: factors controlling activity and selectivity. In: Grasselli RK, Oyama ST, Gaffney AM, Lyons JE (eds) Studies in surface science and catalysis. Elsevier, Osaka, pp 123–134

    Google Scholar 

  9. Qi C, Akita T, Okumura M, Haruta M (2001) Epoxidation of propylene over gold catalysts supported on non-porous silica. Appl Catal A Gen 218(1–2):81–89

    CAS  Google Scholar 

  10. Sinha AK, Seelan S, Okumura M, Akita T, Tsubota S, Haruta M (2005) Three-dimensional mesoporous titanosilicates prepared by modified sol–gel method: ideal gold catalyst supports for enhanced propene epoxidation. J Phys Chem B 109(9):3956–3965

    CAS  Google Scholar 

  11. Lu J, Zhang X, Bravo-Suárez JJ, Bando KK, Fujitani T, Oyama ST (2007) Direct propylene epoxidation over barium-promoted Au/Ti-TUD catalysts with H2 and O2: effect of Au particle size. J Catal 250(2):350–359

    CAS  Google Scholar 

  12. Yap N, Andres RP, Delgass WN (2004) Reactivity and stability of Au in and on TS-1 for epoxidation of propylene with H2 and O2. J Catal 226(1):156–170

    CAS  Google Scholar 

  13. Lu J, Zhang X, Bravo-Suárez JJ, Fujitani T, Oyama ST (2009) Effect of composition and promoters in Au/TS-1 catalysts for direct propylene epoxidation using H2 and O2. Catal Today 147(3–4):186–195

    CAS  Google Scholar 

  14. Haruta M, Uphade BS, Tsubota S, Miyamoto A (1998) Selective oxidation of propylene over gold deposited on titanium-based oxides. Res Chem Intermed 24(3):329–336

    CAS  Google Scholar 

  15. Uphade BS, Okumura M, Tsubota S, Haruta M (2000) Effect of physical mixing of CsCl with Au/Ti-MCM-41 on the gas-phase epoxidation of propene using H2 and O2: drastic depression of H2 consumption. Appl Catal A Gen 190(1–2):43–50

    CAS  Google Scholar 

  16. Sinha AK, Seelan S, Akita T, Tsubota S, Haruta M (2003) Vapor phase propylene epoxidation over Au/Ti-MCM-41 catalysts prepared by different Ti incorporation modes. Appl Catal A Gen 240(1–2):243–252

    CAS  Google Scholar 

  17. Uphade BS, Akita T, Nakamura T, Haruta M (2002) Vapor-phase epoxidation of propene using H2 and O2 over Au/Ti–MCM-48. J Catal 209(2):331–340

    CAS  Google Scholar 

  18. Sacaliuc E, Beale AM, Weckhuysen BM, Nijhuis TA (2007) Propene epoxidation over Au/Ti-SBA-15 catalysts. J Catal 248(2):235–248

    CAS  Google Scholar 

  19. Stangland EE, Taylor B, Andres RP, Delgass WN (2005) Direct vapor phase propylene epoxidation over deposition-precipitation gold-titania catalysts in the presence of H2/O2: effects of support, neutralizing agent, and pretreatment. J Phys Chem B 109(6):2321–2330

    CAS  Google Scholar 

  20. Lee WS, Akatay MC, Stach EA, Ribeiro FH, Delgass WN (2014) Gas-phase epoxidation of propylene in the presence of H2 and O2 over small gold ensembles in uncalcined TS-1. J Catal 313:104–112

    CAS  Google Scholar 

  21. Rode CV, Nehete UN, Dongare MK (2003) Alkali promoted selective epoxidation of styrene to styrene oxide using TS-1 catalyst. Catal Commun 4(8):365–369

    CAS  Google Scholar 

  22. Shetti VN, Srinivas D, Ratnasamy P (2004) Enhancement of chemoselectivity in epoxidation reactions over TS-1 catalysts by alkali and alkaline metal ions. J Mol Catal A Chem 210(1–2):171–178

    CAS  Google Scholar 

  23. Lu JQ, Li N, Pan XR, Zhang C, Luo MF (2012) Direct propylene epoxidation with H2 and O2 over In modified Au/TS-1 catalysts. Catal Commun 28(2012):179–182

    CAS  Google Scholar 

  24. Wang XS, Guo XW, Li G (2002) Synthesis of titanium silicalite (TS-1) from the TPABr system and its catalytic properties for epoxidation of propylene. Catal Today 74(1–2):65–75

    CAS  Google Scholar 

  25. Chen X, Burda C (2004) Photoelectron spectroscopic investigation of nitrogen-doped titania nanoparticles. J Phys Chem B 108(40):15446–15449

    CAS  Google Scholar 

  26. Bertoti I, Mohai M, Sullivan JL, Saied SO (1995) Surface characterisation of plasma-nitrided titanium: an XPS study. Appl Surf Sci 84(4):357–371

    CAS  Google Scholar 

  27. Dogan F, Hammond KD, Tompsett GA, Huo H, Conner WC Jr, Auerbach SM, Grey CP (2009) Searching for microporous, strongly basic catalysts: experimental and calculated 29Si NMR spectra of heavily nitrogen-doped Y zeolites. J Am Chem Soc 131(31):11062–11079

    CAS  Google Scholar 

  28. Narasimharao K, Hartmann M, Thiel HH, Ernst S (2006) Novel solid basic catalysts by nitridation of zeolite beta at low temperature. Microporous Mesoporous Mater 90(1–3):377–383

    CAS  Google Scholar 

  29. Wang J, Liu Q (2005) Structural change and characterization in nitrogen-incorporated SBA15 oxynitride mesoporous materials via different thermal history. Microporous Mesoporous Mater 83(1–3):225–232

    CAS  Google Scholar 

  30. Singh UG, Williams RT, Hallam KR, Allen GC (2005) Synthesis and characterisation of titanium and titanium nitride-functionalised MCM 41 materials. Solid State Sci 7(9):1104–1112

    CAS  Google Scholar 

  31. Zhou J, Hua Z, Liu Z, Wu W, Zhu Y, Shi J (2011) Direct synthetic strategy of mesoporous ZSM-5 zeolites by using conventional block copolymer templates and the improved catalytic properties. ACS Catalysis 1(4):287–291

    CAS  Google Scholar 

  32. Schuster W, Niederer JP, Hoelderich WF (2001) The gas phase oxidative dehydrogenation of propane over TS-1. Appl Catal A Gen 209(1–2):131–143

    CAS  Google Scholar 

  33. Selli E, Forni L (1999) Comparison between the surface acidity of solid catalysts determined by TPD and FTIR analysis of pre-adsorbed pyridine. Microporous Mesoporous Mater 31(1–2):129–140

    CAS  Google Scholar 

  34. Cumaranatunge L, Delgass WN (2005) Enhancement of Au capture efficiency and activity of Au/TS-1 catalysts for propylene epoxidation. J Catal 232(1):38–42

    CAS  Google Scholar 

Download references

Acknowledgements

This work is supported by the National Natural Science Foundation of China (No. 21276127).

Author information

Authors and Affiliations

Authors

Contributions

The manuscript was prepared through contributions of all authors. All authors have given approval to the final version of the manuscript.

Corresponding author

Correspondence to Weihua Ma.

Ethics declarations

Conflict of interest

The authors declare that they have no competing financial interests.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Yuan, T., Zhu, Q., Gao, L. et al. The nitriding of titanium silicate-1 and its effect on gas-phase epoxidation of propylene. J Mater Sci 55, 3803–3811 (2020). https://doi.org/10.1007/s10853-019-04166-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-019-04166-4

Navigation