Citation: Ping Wang, Bo Yang. Influence of surface strain on activity and selectivity of Pd-based catalysts for the hydrogenation of acetylene: A DFT study[J]. Chinese Journal of Catalysis, ;2018, 39(9): 1493-1499. doi: 10.1016/S1872-2067(18)63081-5 shu

Influence of surface strain on activity and selectivity of Pd-based catalysts for the hydrogenation of acetylene: A DFT study

Ping Wang ,
Bo Yang

School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China

Received Date: 1 March 2018
Revised Date: 7 April 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (21603142), the Shanghai Pujiang Program (16PJ1406800) and the Shanghai Young Eastern Scholar Program (QD2016049).

The effects of surface strain and subsurface promoters, which are both important factors in heterogeneous catalysis, on catalytic selectivity and activity of Pd are examined in this study by considering the selective hydrogenation of acetylene as an example. Combined density functional theory calculations and microkinetic modeling reveal that the selectivity and activity of the Pd catalyst for acetylene hydrogenation can both be substantially influenced by the effects of Pd lattice strain variation and subsurface carbon species formation on the adsorption properties of the reactants and products. It is found that the adsorption energies of the reactants and products are, in general, linearly scaled with the lattice strain for both pristine and subsurface carbon atom-modified Pd(111) surfaces, except for the adsorption of C₂H₂ over Pd(111)-C. The activity for ethylene formation typically corresponds to the region of strong reactants adsorption in the volcano curve; such an effect of lattice strain and the presence of subsurface promoters can improve the activity of the catalyst through the weakening of the adsorption of reactants. The activity and selectivity for Pd(111)-C are always higher than those for the pristine Pd(111) surfaces with respect to ethylene formation. Based on the results obtained, Pd-based catalysts with shrinking lattice constants are suggested as good candidates for the selective hydrogenation of acetylene. A similar approach can be used to facilitate the future design of novel heterogeneous catalysts.
- Surface strain,
- Pd,
- Acetylene hydrogenation,
- Selectivity,
- Activity,
- Subsurface,
- Density functional theory,
- Microkinetic modelling
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