Active Sites of Pd-Doped Flat and Stepped Cu(111) Surfaces for H-2 Dissociation in Heterogeneous Catalytic Hydrogenation

作者：Fu Qiang; Luo Yi^*

来源：ACS Catalysis, 2013, 3(6): 1245-1252.

DOI：10.1021/cs400267x

• hydrogenation
• active site
• density functional theory
• subsurface atom
• bimetallic alloy

It has been shown in recent experiments that the Cu(111) surface doped by a small amount of Pd atoms can exhibit excellent catalytic performance toward the dissociation of H-2 molecules. Here we performed systematic first-principles calculations to investigate the corresponding mechanism. Our results clearly demonstrate that a very small number of Pd atoms in the subsurface layer can effectively reduce the energy barrier of H-2 dissociation, making the ensembles composed of the surface and contiguous subsurface Pd atoms as the active sites. The catalytic activity can be further improved if the Pd atoms are doped in the stepped Cu surfaces. The impact of the subsurface Pd atoms comes from an enhanced surface-adsorbate interaction caused by adjusting the electronic structure of the substrate. The important role played by the subsurface atoms offers an efficient approach to finely tune the surface activity by a very limited number of atoms. Our findings should be very useful for understanding and improving the catalytic properties of alloy systems for the industrially important hydrogenation. reactions.

• 出版日期2013-6
• 单位中国科学技术大学