Stability and mobility of supported Ni_n (n = 1–10) clusters on ZrO₂(111) and YSZ(111) surfaces: a density functional theory study

Abstract

The performance of supported metal catalysts, such as nickel nanoparticles decorating yttria-stabilized zirconia (YSZ), depends on their microstructure and the metal-support interface. Here, we have used spin polarized density functional theory (DFT) to evaluate different Ni cluster geometries and determined the electronic structure of the most stable configurations. We have described the interaction of Nin (n = 1-10) clusters supported on the cubic ZrO2(111) and YSZ(111) surfaces, which show a preference for pyramidal shapes rather than flat structures wetting the surface. The interfacial interaction is characterized by charge transfer from the cluster to the surface. We also show how yttrium, present in YSZ, affects the Ni-Ni interaction. Through analysing the difference between the cohesive energy and the clustering energy, we show the preference of Ni-Ni bond formation over Ni-surface interaction; this energy difference decreases with the increase of the Nin cluster size. From the evaluation of the Ni atomic hopping rates on YSZ, we have demonstrated that under different temperature conditions, Ni atoms aggregate with other atoms and clusters, which affects the cluster size stability.

Cation-doping strategies for tuning of zirconia acid–base properties

“…Moreover, it was observed that one of these cations will be located at the (111) surface and the oxygen vacancy at the subsurface. Similar results were later obtained by Cadi-Essadek et al [ 28 , 30 , 47 ] and Ricca et al [ 48 ] using DFT approaches (generalized gradient approximation (GGA) and hybrid functionals). It is worth noticing that alternative configurations have also been identified by Chaopradith et al [ 49 ], which may be appropriate for higher dopant concentrations.…”

Advancing the multiscale understanding on solid oxide electrolysis cells via modelling approaches: A review

“…Density functional theory (DFT) [28,29,31,42,43] Molecular dynamics (MD) [32,[37][38][39] Kinetic Monte Carlo The above five scales and the corresponding modelling approaches are reviewed in the following sections. Microscale models are employed to study the detailed electronic structure of materials as well as the atomic/molecular interactions.…”

“…Cadi-Essadek et al [29] conducted DFT modelling to assess the stability of various Ni cluster configurations on the ZrO2 and YSZ using clustering energy as an index. Besides, the cohesive energy and the interaction energy was calculated to understand the interaction among Ni atoms, and the interaction between the electrolyte surface and the DFT was also used to evaluate the catalytic/electrocatalytic reactions of gaseous reactants in porous materials [30].…”

Defect-induced efficient dry reforming of methane over two-dimensional Ni/h-boron nitride nanosheet catalysts

“…Here, we chose Ni dimer to clarify the interaction between Ni clusters and h-BNNS [48][49][50][51]. As shown in Fig.…”