Growth and stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111)

Düll, Fabian; Meusel, Manuel; Späth, Florian; Schötz, Simon; Bauer, Udo; Bachmann, Philipp; Steinhauer, Johann; Steinrück, Hans‐Peter; Bayer, Andreas; Papp, Christian

doi:10.1039/c9cp04095a

Cited by 18 publications

(27 citation statements)

References 39 publications

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“…The same group used another template h-BN/Ir (111) allowing stabilization of Ir clusters containing 6 to 175 atoms up to 700K under UHV [24]. On h-BN/Rh(111) another group has prepared at RT, under UHV, Pt single atoms and Ptn clusters (n=2-50) [25]. Pt clusters containing around 12 atoms were stable up to 400 K [25].…”

Section: Introductionmentioning

confidence: 99%

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Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study

Sitja

Henry

2021

J. Phys. Chem. C

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Single atom catalyst (SAC) is a vivid new area of research in catalysis. However, the activity in CO oxidation of isolated Pt or Pd atoms, generally supported on an oxide powder, is still controversial. Furthermore, the steady state activity of few atoms clusters is still not yet quantitatively known. In this work we study, by molecular beam reactive scattering (MBRS), the activity of Pdn (n= 1-5) clusters, grown on a nanostructured alumina films on a Ni3Al(111) surface. It is shown that the single atoms are not active at 473 K but they diffuse and coalesce at 533K forming larger clusters. The activity of a cluster is proportional to the number of atoms it contains (n=2-5). At 533 K, the activity per (surface-) atom, which is the turnover frequency (TOF), is constant. Its value is close to those obtained for large clusters of 181±13 atoms and Pd (111) extended surfaces, in the same experimental conditions.

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Section: Introductionmentioning

confidence: 99%

“…On h-BN/Rh(111) another group has prepared at RT, under UHV, Pt single atoms and Ptn clusters (n=2-50) [25]. Pt clusters containing around 12 atoms were stable up to 400 K [25]. Another study with the same template has shown that Pd single atoms are mobile and coalesce at RT under UHV [26].…”

Section: Introductionmentioning

confidence: 99%

Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study

Sitja

Henry

2021

J. Phys. Chem. C

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“…However, if during the experiments, because of the temperature or the chemical environment, diffusion occurs, the initial wellcharacterized system disappears leadingand is replaced by a new and inoperable system. The experimental conditions can be sufficient to initiate the diffusion of monomers [8], dimers [13], but also larger clusters [9]. At present, the most common technique to determine the size statistics of very small clusters is to use an STM (Scanning Tunneling Microscope) which provides safely the ratio between occupied and unoccupied sites, i.e.…”

Section: Introductionmentioning

confidence: 99%

Modifications of statistics under dimer diffusion

Sitja¹

2021

Preprint

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The diffusion, "explosion" and "evaporation" of dimers and the subsequent coalescence are treated in a formal way by identifying and solving the differential equations deduced from the respective behaviors of dimers in the different cases. This study leads to analytic formulas allowing to calculate, in a simple and fast way, the size statistics obtained after the coalescence of the dimers or their constituents once the dimers have completely disappeared. These formulas are of capital interest to characterize systems in which the dimers initially present disappear. Study assumptions.Six assumptions will be made for this study: 1. Initial probabilities are known. G.S. -28-4-2021 -02:33 5 DIMER DIFFUSION 3 2. Only dimers disappear.3. The diffusion of dimers or constituents can be decomposed in two of tree steps according the scenario:(a) If the dimer diffuses: i. A dimer is removed from the set of dimers. ii. The taken dimer is then placed randomly at the surface (i.e. on a nucleation site) (b) If the dimer explode: i. A dimer is removed from the set of dimers ii. The first monomer is then placed randomly at the surface on a site holding a cluster. iii. The second single atom is then also placed randomly on a site holding a cluster.(c) If the dimer evaporates: i. A dimer is removed from the set of dimers and a monomer is added to the set of monomers. ii. A single atom is placed on a site on the surface.4. The number N of nucleation sites is very large : 1/N ≪ 1 5. The mean free path of a diffusing atom is large in comparison of the distance of nucleation centers.6. Finally, the size of a cluster is negligible in regard of the distance of nucleation center. This means that the capture probability for an atom does not depend of the size of the cluster already present on the nucleation center, and that condition 5 will be fulfilled. Dimer DiffusionWe will suppose here that the dimers leave their position and that, without breaking up, they diffuse until they reach a nucleation site (already occupied or not).Let us consider a starting situation in which we have the probability P 0 of having an empty site, the probability P 1 of having a site with a monomer, P 2 of having a site with a dimer... and P n of having a site with a cluster of n atoms. A priori, P 1 should be equal to 0, but, as said above, we are going to keep it, it won't make the calculations more complicated, and it could allow us to "solve" the improbable but not impossible problem where monomers, because of their enhanced interaction with the substrate, could be more efficiently trapped on the surface defects than the dimers.

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“…Deposited copper clusters rapidly and naturally coalesce into larger clusters [18] in a process known as Ostwald ripening, and it does not seem possible to study such small, size-selected clusters deposited on a support. This is a trend with many materials and obtaining small clusters is a challenge more often than not [254], exceptions being those cases in which the clusters can be trapped somehow [255,256], or when clusters are previously generated in vacuum where they can be size selected and then deposited on the target substrate [257,258].…”

Section: Motivationmentioning

confidence: 99%

“…This is of course also the case with most materials, and this effect is of theoretical and experimental interest in many fields such as the study of thin films [274][275][276][277] and epitaxial layer growth [278], of Moiré patterns on mismatched materials [279,280], 2D heterostructures [281][282][283], among many others. The effect of lattice mismatch is of more interest than just a technicality, since it can decide the electronic structure and stability of catalytic heterolayers [284,285], or form structures that can capture metallic clusters or other molecules, such as in graphene [255,286] which buckles under the induced mismatch strain, or hBN [256] which forms pores when deposited on certain metals. This mismatch has consequences for any interface between the two materials.…”

Section: Motivationmentioning

confidence: 99%

Neural Network Potential Simulations of Copper Supported on Zinc Oxide Surfaces

Leandro¹

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There are more things in Heaven and Earth, Horatio, Than are dreamt of in your Philosophy.(Hamlet, Shakespeare) They have a curse. They say: May you live in interesting times. (Apocryphal quote)Give me an algorithm and a point of fulcrum and I will move the world. (An Archimedes for the informatic age)The story so far: In the beginning the Universe was created. This has made a lot of people very angry and been widely regarded as a bad move.

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Growth and stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111)

Abstract: We investigated growth and temperature stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111) using high-resolution XPS and STM.

Cited by 18 publications

References 39 publications

Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study

Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study

Modifications of statistics under dimer diffusion

Neural Network Potential Simulations of Copper Supported on Zinc Oxide Surfaces

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Growth and stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111)

Abstract: We investigated growth and temperature stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111) using high-resolution XPS and STM.

Cited by 18 publications

References 39 publications

Activity of Pdn (n = 1–5) Clusters on Alumina Film on Ni3Al(111) for CO Oxidation: A Molecular Beam Study

Activity of Pdn (n = 1–5) Clusters on Alumina Film on Ni3Al(111) for CO Oxidation: A Molecular Beam Study

Modifications of statistics under dimer diffusion

Neural Network Potential Simulations of Copper Supported on Zinc Oxide Surfaces

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Product

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Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study

Activity of Pd_n (n = 1–5) Clusters on Alumina Film on Ni₃Al(111) for CO Oxidation: A Molecular Beam Study