First-principles investigations of the structural, electronic, and magnetic properties of Pt13−nNin clusters

Zhao, Fangfang; Liu, Chuan; Wang, Peng; Huang, Shiping; Tian, Hui

doi:10.1016/j.jallcom.2013.06.175

Cited by 25 publications

(12 citation statements)

References 41 publications

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“…The geometry of the Pt 13 cluster is icosahedral with one atom in the center, this is the smallest core@shell nanoparticle possible, previous reports have used this small cluster to model core@shell catalysts. 50,51 On the other hand, in order to get the (100) and ( 111) facets of real nanoparticles, from Pt 38 to Pt 260 truncated cuboctahedra were constructed adding layer by layer to a 6 atom Pt cluster with O h symmetry. This structural evolution (from icosahedral to fcc-like clusters as the cluster size increases) has been suggested on the basis of DFT calculations 52 that examined three different growth pathways and the approximate sizes where transitions between these structures may occur.…”

Section: Resultsmentioning

confidence: 99%

Challenges of modelling real nanoparticles: Ni@Pt electrocatalysts for the oxygen reduction reaction

Ramos-Sánchez

Praserthdam

Godínez-Salomón

et al. 2015

Phys. Chem. Chem. Phys.

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Theoretical/computational methods have been extensively applied to screen possible nano-structures attempting to maximize catalytic and stability properties for applications in electrochemical devices. This work shows that the method used to model core@shell structures is of fundamental importance in order to truly represent the physicochemical changes arising from the formation of a core-shell structure. We demonstrate that using a slab approach for modelling nanoparticles the oxygen adsorption energies are qualitatively well represented. Although this is a good descriptor for the catalytic activity, huge differences are found for the calculated surface stability between the results of a nano-cluster and those of a slab approach. Moreover, for the slab method depending on the geometric properties of the core and their similarity to the elements of the core or shell, contradictory effects are obtained. In order to determine the changes occurring as the number of layers and nano particle size are increased, clusters of Ni@Pt from 13 to 260 atoms were constructed and analyzed in terms of geometric parameters, oxygen adsorption, and dissolution potential shift. It is shown that the results of modelling the Ni@Pt nanoparticles with a cluster approach are in good agreement with experimental geometrical parameters, catalytic activity, and stability of a carefully prepared series of Ni@Pt nanostructures where the shell thickness is systematically changed. The maximum catalytic activity and stability are found for a monolayer of Pt whereas adding a second and third layer the behavior is almost the same than that in pure Pt nanoparticles.

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Section: Resultsmentioning

confidence: 99%

Challenges of modelling real nanoparticles: Ni@Pt electrocatalysts for the oxygen reduction reaction

Ramos-Sánchez

Praserthdam

Godínez-Salomón

et al. 2015

Phys. Chem. Chem. Phys.

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“…N best solutions with lower energies are kept for further LM, and the solution s with the lowest energy will be selected as the final solution of this DL searching. (4) If E(s ) < E(s), s is selected as the starting cluster and return to step (2). Otherwise, solution s is the result of the BDLS run.…”

Section: Bdls Proceduresmentioning

confidence: 99%

“…The basic steps of ILS method include first improvement local search method and perturbation operator. If the energy of the obtained configuration is lower than that of the configuration s, then go to step (2). Otherwise, the best configuration is s .…”

Section: Description Of Bdls-ils Algorithmmentioning

confidence: 99%

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Fast optimization of binary clusters using a novel dynamic lattice searching method

Cheng

2014

The Journal of Chemical Physics

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Global optimization of binary clusters has been a difficult task despite of much effort and many efficient methods. Directing toward two types of elements (i.e., homotop problem) in binary clusters, two classes of virtual dynamic lattices are constructed and a modified dynamic lattice searching (DLS) method, i.e., binary DLS (BDLS) method, is developed. However, it was found that the BDLS can only be utilized for the optimization of binary clusters with small sizes because homotop problem is hard to be solved without atomic exchange operation. Therefore, the iterated local search (ILS) method is adopted to solve homotop problem and an efficient method based on the BDLS method and ILS, named as BDLS-ILS, is presented for global optimization of binary clusters. In order to assess the efficiency of the proposed method, binary Lennard-Jones clusters with up to 100 atoms are investigated. Results show that the method is proved to be efficient. Furthermore, the BDLS-ILS method is also adopted to study the geometrical structures of (AuPd)79 clusters with DFT-fit parameters of Gupta potential.

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“…Then, they are attractive from a fundamental perspective and often show distinct catalytic properties and stability as compared to individual metals, which is typically ascribed to the coupling effect and/or synergism in the electronic and/or geometric structures that occur when the metals are combined ( Ferrando et al, 2008 ; Tao, 2012 ; Yan et al, 2017 ; Ding et al, 2018 ; Añez et al, 2021 ; Reboul et al, 2021 ). Significant efforts have been put into the research field of nanocatalysis to explore the structure, surface composition, and atomic distribution for two metals systems, which are crucial for their properties and catalytic activities of bimetallic nanoalloys ( Ferrando et al, 2008 ; Jellinek, 2008 ; Piotrowski et al, 2012 ; Cui et al, 2013 ; Zhao et al, 2013 ; Guedes-Sobrinho et al, 2015 ; Gilroy et al, 2016 ; Wang et al, 2016 ; Wu et al, 2019 ). However, an in-depth understanding of the processes involved in forming these alloy materials is somewhat limited, especially at the atomic level.…”

Section: Introductionmentioning

confidence: 99%

A Theoretical Study on the Structural, Electronic, and Magnetic Properties of Bimetallic Pt13−nNin (N = 0, 3, 6, 9, 13) Nanoclusters to Unveil the Catalytic Mechanisms for the Water-Gas Shift Reaction

2022

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In this work, first-principles calculations by using density functional theory at the GFN-xTB level, are performed to investigate the relative stability and structural, electronic, and magnetic properties of bimetallic Pt13−nNin (n = 0, 3, 6, 9, 13) nanoclusters by using corrected Hammer and Nørskov model. In addition, by employing the reaction path and the energetic span models, the energy profile and the turnover frequency are calculated to disclose the corresponding reaction mechanism of the water-gas shift reaction catalyzed by these nanoclusters. Our findings render that Ni causes an overall shrinking of the nanocluster’s size and misalignment of the spin channels, increasing the magnetic nature of the nanoclusters. Pt7Ni6 nanocluster is the most stable as a result of the better coupling between the Pt and Ni d-states. Pt4Ni9 maintains its structure over the reaction cycle, with a larger turnover frequency value than Pt7Ni6. On the other hand, despite Pt10Ni3 presenting the highest value of turnover frequency, it suffers a strong structural deformation over the completion of a reaction cycle, indicating that the catalytic activity can be altered.

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First-principles investigations of the structural, electronic, and magnetic properties of Pt13−nNin clusters

Cited by 25 publications

References 41 publications

Challenges of modelling real nanoparticles: Ni@Pt electrocatalysts for the oxygen reduction reaction

Challenges of modelling real nanoparticles: Ni@Pt electrocatalysts for the oxygen reduction reaction

Fast optimization of binary clusters using a novel dynamic lattice searching method

A Theoretical Study on the Structural, Electronic, and Magnetic Properties of Bimetallic Pt13−nNin (N = 0, 3, 6, 9, 13) Nanoclusters to Unveil the Catalytic Mechanisms for the Water-Gas Shift Reaction

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