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

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  • Zongyuan Liu
    Department of Chemistry State University of New York at Stony Brook Stony Brook NY 11794 USA
  • David C. Grinter
    Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  • Pablo G. Lustemberg
    Instituto de Fisica Rosario (IFIR) CONICET—Universidad Nacional de Rosario Argentina
  • Thuy‐Duong Nguyen‐Phan
    Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  • Yinghui Zhou
    Department of Chemistry University of Wyoming Laramie WY 82071 USA
  • Si Luo
    Department of Chemistry State University of New York at Stony Brook Stony Brook NY 11794 USA
  • Iradwikanari Waluyo
    Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  • Ethan J. Crumlin
    Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
  • Dario J. Stacchiola
    Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  • Jing Zhou
    Department of Chemistry University of Wyoming Laramie WY 82071 USA
  • Javier Carrasco
    CIC Energigune Albert Einstein 48 01510 Miñano, Álava Spain
  • H. Fabio Busnengo
    Instituto de Fisica Rosario (IFIR) CONICET—Universidad Nacional de Rosario Argentina
  • M. Verónica Ganduglia‐Pirovano
    Instituto de Catálisis y Petroleoquímica CSIC C/Marie Curie 2 28049 Madrid Spain
  • Sanjaya D. Senanayake
    Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  • José A. Rodriguez
    Department of Chemistry State University of New York at Stony Brook Stony Brook NY 11794 USA

書誌事項

公開日
2016-05-04
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#am
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/ange.201602489
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Ni‐CeO<jats:sub>2</jats:sub> 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<jats:sub>2</jats:sub> at temperatures as low as 300 K, generating CH<jats:sub><jats:italic>x</jats:italic></jats:sub> and CO<jats:sub><jats:italic>x</jats:italic></jats:sub> 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<jats:sub>2−<jats:italic>x</jats:italic></jats:sub>(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH<jats:sub><jats:italic>x</jats:italic></jats:sub> or C species are detected in the C 1s XPS region. The reforming of methane proceeds in a clean and efficient way.</jats:p>

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