4.6 Article

DFT Study on the Methane Synthesis from Syngas on a Cerium-Doped Ni(111) Surface

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 120, Issue 40, Pages 23030-23043

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b07400

Keywords

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Funding

  1. National Natural Science Foundation of China [21503210, 21521092]
  2. Jilin Province Youth Fund [20130522141JH]
  3. Jilin Province Natural Science Foundation [20150101012JC]
  4. Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)
  5. Department of Science and Technology of Sichuan Province [2011GZX0077, 2012JZ0007, 2014HH0049]
  6. Performance Computing Center of Jilin University
  7. Changchun Normal University

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The methanation of syngas (CO and H-2) on the Ce-doped Ni(111) surface (Ce-Ni(111)) has been investigated by using the density functional method. The doped Ce enhances the adsorption energy of the intermediates on the catalytic surface, except for H-2, particularly for O-containing species. On the Ce-Ni(111) surface, the reaction pathway CO + 3H(2) -> CHO + 5H -> CH + O + SH -> CH4 + H2O is the most favorite, in which the energy barrier is 1.18 eV for the rate-determining step. Compared with the pure Ni(111) surface, the doping of Ce improves the catalytic activity both thermodynamically and kinetically. The microkinetic analysis also supports that the methanation of syngas has high reaction rate on the Ce-Ni(111) compared with the pure Ni(111). The temperature has great influence on the reaction rate, while H-2/CO ratio shows only slightly impact. Our study also explains the experimental observation that the doped Ce can reduce the reaction temperature from similar to 500 degrees C on the pure Ni(111) to similar to 340 degrees C on the Ce-Ni(111) surface. The coverage of CHO is the largest on the Ce-Ni(111) surface. We expect that the obtained results could be useful for the future experimental study in searching the high efficient catalysts.

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