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Dry Reforming of Methane on a Highly‐Active Ni‐CeO 2 Catalyst: Effects of Metal‐Support Interactions on C−H Bond Breaking

2016; Wiley; Volume: 55; Issue: 26 Linguagem: Inglês

10.1002/anie.201602489

1521-3773

Zongyuan Liu, David C. Grinter, Pablo G. Lustemberg, Thuy‐Duong Nguyen‐Phan, Yinghui Zhou, Si Luo, Iradwikanari Waluyo, Ethan J. Crumlin, Darı́o Stacchiola, Jing Zhou, Javier Carrasco, H. F. Busnengo, M. V. Ganduglia-Pirovano, Sanjaya D. Senanayake, José A. Rodríguez,

Catalysis and Oxidation Reactions

Abstract Ni‐CeO 2 is a highly efficient, stable and non‐expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density‐functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO 2− x (111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C 1s XPS region. The reforming of methane proceeds in a clean and efficient way.