Dry Reforming of Methane on a Highly‐Active Ni‐CeO2 Catalyst: Effects of Metal‐Support Interactions on C−H Bond Breaking

• DOI: 10.1002/anie.201602489
• Publication Date: 2016-05-04T17:55:38Z
• Authors: Zongyuan Liu; David C. Grinter; Pablo G. Lustemberg; Thuy‐Duong Nguyen...; Yinghui Zhou; Si Luo; Iradwikanari Waluyo; Ethan J. Crumlin; Dario J. Stacchiola; Jing Zhou; Javier Carrasco; H. Fabio Busnengo; M. Verónica Gandu...; Sanjaya D. Senana...; José A. Rodriguez
• Keywords: X-ray photoelectron spectroscopy; NICKEL; 02 engineering and technology; Physical Chemistry; 7. Clean energy; 01 natural sciences; nickel; https://purl.org/becyt/ford/1.4; methane dissociation; DENSITY FUNCTIONAL THEORY; https://purl.org/becyt/ford/1; density functional theory; CERIA; Organic Chemistry; 540; ceria; 0104 chemical sciences; Chemical sciences; 13. Climate action; Chemical Sciences; METHANE DISSOCIATION; X-RAY PHOTOELECTRON SPECTROSCOPY; 0210 nano-technology

AbstractNi‐CeO2 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/CeO2 at temperatures as low as 300 K, generating CHx and COx 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/CeO2−x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CHx or C species are detected in the C 1s XPS region. The reforming of methane proceeds in a clean and efficient way.