A first-principle calculation of sulfur oxidation on metallic Ni(111) and Pt(111), and bimetallic Ni@Pt(111) and Pt@Ni(111) surfaces

Chen Hao Yeh, Jia Jen Ho*

*此作品的通信作者

研究成果: 雜誌貢獻期刊論文同行評審

11 引文 斯高帕斯(Scopus)

摘要

Sulfur, a pollutant known to poison fuel-cell electrodes, generally comes from S-containing species such as hydrogen sulfide (H2S). The S-containing species become adsorbed on a metal electrode and leave atomic S strongly bound to the metal surface. This surface sulfur is completely removed typically by oxidation with O2 into gaseous SO2. According to our DFT calculations, the oxidation of sulfur at 0.25 ML surface sulfur coverage on pure Pt(111) and Ni(111) metal surfaces is exothermic. The barriers to the formation of SO2 are 0.41 and 1.07 eV, respectively. Various metals combined to form bimetallic surfaces are reported to tune the catalytic capabilities toward some reactions. Our results show that it is more difficult to remove surface sulfur from a Ni@Pt(111) surface with reaction barrier 1.86 eV for SO2 formation than from a Pt@Ni(111) surface (0.13 eV). This result is in good agreement with the statement that bimetallic surfaces could demonstrate more or less activity than to pure metal surfaces by comparing electronic and structural effects. Furthermore, by calculating the reaction free energies we found that the sulfur oxidation reaction on the Pt@Ni(111) surface exhibits the best spontaneity of SO2 desorption at either room temperature or high temperatures.

原文英語
頁(從 - 到)3194-3203
頁數10
期刊ChemPhysChem
13
發行號13
DOIs
出版狀態已發佈 - 2012 九月 17

ASJC Scopus subject areas

  • 原子與分子物理與光學
  • 物理與理論化學

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