Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2013, Vol. 34 ›› Issue (5): 1002-1012.DOI: 10.1016/S1872-2067(12)60537-3

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Density functional theory study of direct synthesis of H2O2 from H2 and O2 on Pd(111), Pd(100), and Pd(110) surfaces

TIAN Pengfei, OUYANG Like, XU Xinchao, XU Jing, HAN Yi-Fan   

  1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2012-12-30 Revised:2013-05-20 Online:2013-05-06 Published:2013-05-06
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21176071, 21106041).

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Abstract:

The direct synthesis of hydrogen peroxide (H2O2) from hydrogen (H2) and oxygen (O2) on Pd(111), Pd(100), and Pd(110) surfaces was investigated using periodic density functional theory (DFT) calculations. Several elementary steps making up this reaction were postulated and calculated. The Pd(111) surface shows the highest catalytic selectivity for H2O2 among the three surfaces. Open surfaces such as Pd(100) and Pd(110) are not favorable for this reaction because O-O-containing species on these surfaces dissociate easily. The O-O bond energy and the binding energy of O-O-containing surface species are responsible for catalytic selectivity. The higher binding energy of O-O-containing surface species is not favorable for the direct synthesis of H2O2 because the higher binding energy results in lower dissociation barriers.

Key words: Palladium, Hydrogen peroxide, Hydrogen, Oxygen, Direct synthesis, Density functional theory