Effect of reduction temperature on the CO₂-reforming of methane over TiO₂-supported Ni catalyst

Abstract

On the basis of the rate constant per active site determined by pulse surface reaction rate analysis (PSRA), the effect of reduction temperature on the CO₂-reforming of methane has been studied for TiO₂-supported Ni catalyst. Reduction at 773 K resulted in a larger rate constant for the CH₄–CO₂ reaction than that at 673 K. Since the amount of CO adsorbed on the catalyst decreased with an increase in the reduction temperature, the phenomenon could be understood as a result of the strong metal–support interaction (SMSI). The ability of the catalyst to dissociate CO₂ was not affected by the reduction temperature, while that for the dissociation of CH₄ was enhanced by increasing the reduction temperature on a per active site of catalyst basis. A higher specific activity was obtained also for the steady-state CH₄–CO₂ reaction by reducing the catalyst at a higher temperature, suggesting that the activation of CH₄ rather than of CO₂ is primarily responsible for the higher activity in the SMSI state.

References

1. S. J. Tauster, S. C. Fung and R. T. Garten, J. Am. Chem. Soc., 1978, 100, 170.
2. S. J. Tauster, S. C. Fung, R. T. K. Baker and J. A. Horsley, Science, 1981, 211, 4487.
3. M. A. Vannice and R. L. Garten, J. Catal., 1979, 56, 236.
4. M. A. Vannice, J. Catal., 1982, 74, 199.
5. P. Meriaudeau, O. H. Ellestad, M. Defaux and C. Naccache, J. Catal., 1982, 75, 243.
6. K. Foger, J. Catal., 1982, 78, 406.
7. P. Turlier and G. A. Martin, React. Kinet. Catal. Lett., 1982, 21, 387.
8. R. Burch and A. R. Flambard, J. Catal., 1982, 78, 389.
9. A. Erdohelyi, J. Cserenyi, E. Papp and F. Solymosi, Appl. Catal. A: General, 1994, 108, 205.
10. T. Osaki, H. Masuda and T. Mori, Catal. Lett., 1994, 29, 33.
11. T. Osaki, T. Horiuchi, K. Suzuki and T. Mori, J. Chem. Soc., Faraday Trans., 1996, 92, 1627.
12. T. Osaki, H. Masuda, T. Horiuchi and K. Suzuki, Catal. Lett., 1995, 34, 59.
13. T. Mori, K. Suzuki, M. Saito, T. Hattori and Y. Murakami, Bull. Chem. Soc. Jpn., 1989, 62, 3001.
14. K. Kunimori, S. Matsui and T. Uchijima, Chem. Lett., 1985, 359.
15. J. B. F. Anderson and R. Burch, Appl. Catal., 1986, 21, 179.
16. T. Mori, H. Masuda and Y. Murakami, J. Chem. Soc. Jpn., 1977, 315.
17. A. Tomita and Y. Tamai, J. Catal., 1972, 27, 293.
18. J. G. McCarty and H. Wise, J. Catal., 1979, 57, 406.
19. F. Solymosi, Catal. Rev., 1967, 1, 233.