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Acta Physico-Chimica Sinica  2008, Vol. 24 Issue (09): 1662-1668    DOI: 10.3866/PKU.WHXB20080923
Article     
DFT Study on Hydrogen and Sulfur Adsorption on (111) Surface of Pd, Cu, Au, and PdAu, PdCu Alloys
HUANG Yong-Li; LIU Zhi-Ping
Division of Molecular and Materials Simulation, Key Laboratory for Nanomaterials, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029, P. R. China
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Abstract  The gradient corrected density functional theory (DFT) calculations were presented on the adsorption of both hydrogen and sulfur on pure Pd(111), Cu(111) and Au(111) surfaces, as well as on PdM3(111), Pd2M2(111), and Pd3M(111) surfaces. The most favorable adsorption sites, binding energies and the relaxation during adsorption were obtained with a coverage of 0.25. The Pd surface exhibited the strongest adsorption of both hydrogen and sulfur atoms. Cu was the next and Au had the weakest affinity with them. The binding energies of adsorption of hydrogen and sulfur on PdM alloys decreased with the increase of the concentration of metal M, except Pd3Au, in which case, the adsorption of hydrogen on Pd3Au (111) surface was even stronger than that on pure Pd, due to the larger lattice constant. According to the values of binding energy, it was found that the binding energies of both hydrogen and sulfur on PdAu decreased slower than that on PdCu, when the concentration of Au was lower than 25% (molar fraction). However, they decreased quickly when the concentration of Au exceeded 50%. PdAu alloy with 25%-50% Au was a promising candidate to resist sulfur and also with high performance in hydrogen permeation.

Key wordsDensity functional theory      Adsorption on surface of metal      Hydrogen atom      Sulfur atom      Palladiumalloy membrane      Sulfur tolerant     
Received: 10 March 2008      Published: 07 August 2008
MSC2000:  O641  
  TQ02  
Corresponding Authors: LIU Zhi-Ping     E-mail: liuzhp@mail.buct.edu.cn
Cite this article:

HUANG Yong-Li; LIU Zhi-Ping. DFT Study on Hydrogen and Sulfur Adsorption on (111) Surface of Pd, Cu, Au, and PdAu, PdCu Alloys. Acta Physico-Chimica Sinica, 2008, 24(09): 1662-1668.

URL:

http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/10.3866/PKU.WHXB20080923     OR     http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/Y2008/V24/I09/1662

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