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Dry Reforming of Methane on a Highly‐Active Ni‐CeO2 Catalyst: Effects of Metal‐Support Interactions on C−H Bond Breaking |
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| Authors: | B?Sc Zongyuan Liu Dr David C Grinter Dr Pablo G Lustemberg Dr Thuy‐Duong Nguyen‐Phan Dr Yinghui Zhou B?Sc Si Luo Dr Iradwikanari Waluyo Dr Ethan J Crumlin Dr Dario J Stacchiola Prof Jing Zhou Dr Javier Carrasco Prof H Fabio Busnengo Dr M Verónica Ganduglia‐Pirovano Dr Sanjaya D Senanayake Prof José A Rodriguez |
| Institution: | 1. Department of Chemistry, State University of New York at Stony Brook, Stony Brook, NY, USA;2. Chemistry Department, Brookhaven National Laboratory, Upton, NY, USA;3. Instituto de Fisica Rosario (IFIR), CONICET—Universidad Nacional de Rosario, Argentina;4. Department of Chemistry, University of Wyoming, Laramie, WY, USA;5. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA;6. CIC Energigune, Mi?ano, álava, Spain;7. Instituto de Catálisis y Petroleoquímica, CSIC, Madrid, Spain |
| Abstract: | Ni‐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. |
| Keywords: | ceria density functional theory methane dissociation nickel X-ray photoelectron spectroscopy |