A Comparative Study of Hydrogen Spillover on Pd and Pt Decorated MoO₃(010) Surfaces from First Principles

Abstract

Hydrogen chemisorption and diffusion on Pt and Pd decorated MoO3(010) surfaces were examined using periodic density functional methods. The deposition of Pt and Pd on MoO3 was first carefully investigated. The strong metal−support interactions were found to greatly reduce the catalytic activity of Pt and Pd atoms anchored at their most favorable binding sites. On the other hand, the energies and activation barriers along selected diffusion pathways indicate that hydrogen dissociation and diffusion on the supported Pt5 and Pd5 clusters are feasible, whereas Pt clusters exhibit better catalytic activity than Pd clusters. Subsequently, the dissociated hydrogen atoms tend to directly diffuse onto the sublayer oxygen atoms instead of the surface oxygen atoms.

H2 INTERACTION WITH BIMETALLIC DIMERS SUPPORTED ON THE MgO(100) SURFACE: A DFT CLUSTER MODEL STUDY

“…Our observation is consistent with that made by Li et al, 23 who have reported that single Pd and Pt atoms lose their catalytic activity toward hydrogen dissociative adsorption when deposited on the MoO 3 (010) surface. However, the deactivation triggered by MoO 3 is considerably greater than in our case.…”

“…For instance, the E values for the H 2 capture on AgPd/C and PdAg/C vary by 7.84 kcal/ mol. 30 Furthermore, small exoenergetic e®ects of H 2 molecular adsorption have been predicted even for single Pd and Pt atoms on the MoO 3 support 23 : the E values are merely equal to À6.92 and À9.69 kcal/mol, respectively.…”

“…Periodic PerdewÀWang (PW91) DFT calculations performed recently by Li et al 23 have revealed that the MoO 3 support greatly reduces the ability of Pd or Pt to dissociate H 2 molecules. The deactivation can be seen for single atoms and small clusters of Pd and Pt deposited on the MoO 3 (010) surface.…”

Density functional study of hydrogen adsorption and diffusion on Ni‐loaded graphene and graphene oxide

“…In previous studies, Chen and coworkers reported that oxygen atoms in metal oxides can greatly facilitate the hydrogen spillover due to the abundant hydrogen‐bonding networks. Herein, we investigated if hydrogen can spillover onto the GO in the presence of oxygen groups.…”

Electrochemical Conversion of Dichloroacetic Acid to Chloroacetic Acid in a Microfluidic Stack and in a Series of Microfluidic Reactors

“…On the basis of first‐principles calculations, Li et al. suggested that dissociated H atoms directly diffuse into sublayer oxygen atoms rather than into surface oxygen atoms 10. Chen et al.…”