Superior catalytic behavior of trace Pt-doped Ni/Mg(Al)O in methane reforming under daily start-up and shut-down operation

Li Dalin

Nishida Kazufumi

Zhan Yingying

Shishido Tetsuya

Oumi Yasunori

Sano Tsuneji

Takehira Katsuomi

Applied Catalysis A: General

Doping effects of Pt and Ru on Ni/Mg(Al)O catalysts were compared in daily start-up and shut-down operations of steam reforming of CH4. Trace Pt-doped catalyst showed better behavior than trace Ru-doped catalyst; the former was self-activated but the latter was not, although both exhibited self-regenerative activity. Moreover, the former exhibited sustainable activity, although the latter was quickly passivated, in the autothermal reforming of CH4. Formation of Pt-Ni alloy on the surface of fine Ni metal particles on the catalysts was suggested by EXAFS analyses. CH4 was dissociatively activated to form hydrogen on Pt, assisted by adsorbed O or OH species, leading to the self activation via Ni reduction by hydrogen spillover from Pt. The self-regeneration of the Pt-Ni/Mg(Al)O catalysts can be achieved by the continuous rebirth of active Ni metal species via reversible reduction-oxidation between Ni0 and Ni2+ in/on Mg(Ni,Al)O periclase assisted by the hydrogen spillover.

CH4 reforming

self activation

self-regeneration

Ni/Mg(Al)O catalyst

Pt doping

daily start-up and shut-down operation

Chemistry [ 430 ]

eng

Elsevier Science BV

Copyright (c) 2008 Published by Elsevier B.V.

[ISSN] 0926-860X

[DOI] 10.1016/j.apcata.2008.08.017

[NCID] AA10821202

[DOI] http://dx.doi.org/10.1016/j.apcata.2008.08.017