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

Journal Article · Wed May 04 00:00:00 EDT 2016 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201602489· OSTI ID:1400757

Liu, Zongyuan ^[1]; Grinter, David C. ^[2]; Lustemberg, Pablo G. ^[3]; Nguyen‐Phan, Thuy‐Duong ^[2]; Zhou, Yinghui ^[4]; Luo, Si ^[1]; Waluyo, Iradwikanari ^[2]; Crumlin, Ethan J. ^[5]; Stacchiola, Dario J. ^[2]; Zhou, Jing ^[4]; Carrasco, Javier ^[6]; Busnengo, H. Fabio ^[3]; Ganduglia‐Pirovano, M. Verónica ^[7]; Senanayake, Sanjaya D. ^[2]; Rodriguez, José A. ^[8]

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1. Department of Chemistry State University of New York at Stony Brook Stony Brook NY 11794 USA
2. Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
3. Instituto de Fisica Rosario (IFIR) CONICET—Universidad Nacional de Rosario Argentina
4. Department of Chemistry University of Wyoming Laramie WY 82071 USA
5. Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
6. CIC Energigune Albert Einstein 48 01510 Miñano, Álava Spain
7. Instituto de Catálisis y Petroleoquímica CSIC C/Marie Curie 2 28049 Madrid Spain
8. Department of Chemistry State University of New York at Stony Brook Stony Brook NY 11794 USA, Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA

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.

• Sponsoring Organization: USDOE
• Grant/Contract Number: SC0012704
• OSTI ID: 1400757
• Journal Information: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 128 Journal Issue: 26; ISSN 0044-8249
• Publisher: Wiley Blackwell (John Wiley & Sons)
• Country of Publication: Germany
• Language: English