Effect of composition and promoters in Au/TS-1 catalysts for direct propylene epoxidation using H2 and O2
2008; Elsevier BV; Volume: 147; Issue: 3-4 Linguagem: Inglês
10.1016/j.cattod.2008.09.005
ISSN1873-4308
AutoresJi-Qing Lu, Xiaoming Zhang, Juan J. Bravo-Suárez, Tadahiro Fujitani, S. Ted Oyama,
Tópico(s)Catalysis and Hydrodesulfurization Studies
ResumoA series of Au/titanium silicalite-1 (TS-1) catalysts with different Si/Ti ratios and promoted with alkali and alkaline earth cations were prepared by deposition–precipitation (DP) and tested for direct propylene epoxidation. It was found that the gold loading and catalytic activity was highly dependent on the pH of the DP synthesis solution and the final composition of the catalyst. Addition of Group 1 metals such as K or Cs had little effect on the gold content, but increased activity, while Group 2 metals such as Mg, Ca, Sr, and Ba increased both the gold content and the catalytic activity. The highest improvement was provided by a Mg promoted catalyst, which at 443 K and 0.1 MPa with a H2/O2/C3H6/Ar = 1/1/1/7 feed mixture gave a propylene oxide (PO) formation rate of 88 gPO h−1 kgcat−1, compared to 57 gPO h−1 kgcat−1 for an unpromoted catalyst, corresponding to a 50% enhancement of activity. Ammonia temperature-programmed desorption (NH3-TPD) measurements indicated little change in adsorption amount with promotion indicating that the yield increase was not due to the elimination of acidic sites on the catalyst. Instead, the improved catalytic performance was ascribed to increased Au capture efficiency and dispersion by the catalyst. The effect of Si/Ti ratio, pH of synthesis, and the promoter ions on the gold content could be understood from their effect on the surface charge of the support.
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