The generation of ground‐state structures and electronic properties of ternary AlkTilNim clusters (k + l + m = 4) from a two‐stage density functional theory global searching approach

Koh, Pin Wai; Yoon, Tiem Leong; Lim, Thong Leng; Chang, Yee Hui Robin

doi:10.1002/qua.25884

Cited by 3 publications

(7 citation statements)

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“…Complementing the work done by these authors, an unbiased search for the ground states structures of Al k Ti l Ni m clusters employing full DFT calculations has been carried out by the present authors recently . The present paper is a natural continuation of our work, which stops at the cluster size of four atoms.…”

Section: Introductionmentioning

confidence: 70%

“…Our previous work, as well as the present one, use a modified version of the original PTMBHGA code for generating and optimizing the configurations of Al‐Ti‐Ni multicomponent alloy clusters. The PTMBHGA code used in this work is interfaced with the first‐principles DFT package Gaussian 09 (G09) .…”

Section: Methodsmentioning

confidence: 99%

“…In the present work, the size of the Al‐Ti‐Ni clusters is larger than that in ref. . If we were to use exactly the same simulation parameters as in the case for the four‐atom clusters, the computation time would become unbearably lengthy (subjected to the constraint of our computational resource).…”

Section: Methodsmentioning

confidence: 99%

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Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Koh

Yoon

Lim

et al. 2019

Int J of Quantum Chemistry

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The structural and electronic properties of ternary Al x Ti y Ni z clusters, where x, y, and z are integers and x + y + z = 6, are investigated. Both Slater, Vosko, Wilks, and Nusair and B3LYP exchange-correlation (XC) functionals are employed in a two-stage density functional theory (DFT) calculations to generate these clusters. In the first stage, a minimum energy cluster structure is generated by an unbiased global search algorithm coupled with a DFT code using a light XC functional and small basis sets. In the second stage, the obtained cluster structure is further optimized by another round of global minimization search coupled with a DFT calculator using a heavier XC functional and more costly basis set. Electronic properties of the structures are illustrated in the form of a ternary diagram. Our DFT calculations find that the thermodynamic stability of the clusters increases with the increment in the number of constituent nickel atoms. These results provide a new insight to the structure, stability, chemical order, and electronic properties for the ternary alloy nanoclusters. K E Y W O R D SAl-Ti-Ni ternary alloy clusters, electronic structures, first-principles calculations, ground-state structures 1 | INTRODUCTION Atomic clusters are aggregates of atoms ranging from a few to thousands of atoms or molecules. Nanoclusters are atomic clusters with a diameter in the order of nanometers. They exhibit distinctly different electronic and structural behaviors compared with their larger size counterpart due to low dimensional and quantum confinement effects. [1] From the year 2000 onward, transition metal clusters had been intensively studied, both experimentally [2][3][4][5][6][7] and computationally. Nanoclusters, mainly binaries or ternaries, have attracted much attention due to their broad applications in catalysis, [32][33][34] magnetic-recording materials, [35] and biological applications, to name a few. For example, FeAlAu n (n = 1 − 6), [36] Fe-Co-Ni, [1,37,38] Fe-Co-Pd, [39] and Ag-Au-Pd [40] trimetallic clusters have been studied for their magnetic, electronic, and structural properties.In the search of the ground-state structures of ternary alloy clusters, one common practice is to generate them based on classical and semiclassical methods such as adoption of Gupta potential, Sutton-Chen potential, and others empirical potentials. These empirical or semiempirical results commonly show that the ground-state structures of the small clusters are in the shape of an icosahedron, whereas truncated octahedron and a truncated decahedral structure is favored by the large clusters. [2] Structural evolution of cluster can be explained and tackled by classical and semiclassical approaches, but these methods may fail if the electronic effects from valence electrons of the atoms have to be taken into account. [1,37,38] Using classical and semiclassical approaches in the search of ground-state configurations for transition metal clusters will produce unreliable results, due to the existence of localized d orbitals. ...

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Section: Introductionmentioning

confidence: 70%

Section: Methodsmentioning

confidence: 99%

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Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Koh

Yoon

Lim

et al. 2019

Int J of Quantum Chemistry

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“…In some cases, subnano clusters have been considered, such as the four-atom AlTiNi clusters modeled by Koh et al , 100 where complex multiscale global optimization was applied. The interest in this system is motivated by the jellium behavior observed for small Al clusters; in this case, the stability of the clusters increases with the number of nickel atoms.…”

Section: Properties Of Trimetallic Nanoparticlesmentioning

confidence: 99%

“…Selectivity is also sensitive to the arrangement of atoms and exposed facets on the surface. 49 For example, the difference between the adsorption energies of the Pt (111) and Pt (100) surfaces can be traced to their intrinsic structural differences and the difference in binding energies, with density functional theory (DFT) studies showing that the binding energy of NH x species on the Pt (100) surface is greater than that on Pt (111) surface by ca. 0.7 eV.…”

Section: Key Properties Of Tmnps To Considermentioning

confidence: 99%

Heterogeneous Trimetallic Nanoparticles as Catalysts

et al. 2022

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The development and application of trimetallic nanoparticles continues to accelerate rapidly as a result of advances in materials design, synthetic control, and reaction characterization. Following the technological successes of multicomponent materials in automotive exhausts and photovoltaics, synergistic effects are now accessible through the careful preparation of multielement particles, presenting exciting opportunities in the field of catalysis. In this review, we explore the methods currently used in the design, synthesis, analysis, and application of trimetallic nanoparticles across both the experimental and computational realms and provide a critical perspective on the emergent field of trimetallic nanocatalysts. Trimetallic nanoparticles are typically supported on high-surface-area metal oxides for catalytic applications, synthesized via preparative conditions that are comparable to those applied for mono- and bimetallic nanoparticles. However, controlled elemental segregation and subsequent characterization remain challenging because of the heterogeneous nature of the systems. The multielement composition exhibits beneficial synergy for important oxidation, dehydrogenation, and hydrogenation reactions; in some cases, this is realized through higher selectivity, while activity improvements are also observed. However, challenges related to identifying and harnessing influential characteristics for maximum productivity remain. Computation provides support for the experimental endeavors, for example in electrocatalysis, and a clear need is identified for the marriage of simulation, with respect to both combinatorial element screening and optimal reaction design, to experiment in order to maximize productivity from this nascent field. Clear challenges remain with respect to identifying, making, and applying trimetallic catalysts efficiently, but the foundations are now visible, and the outlook is strong for this exciting chemical field.

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Electronic factors determining the methane bond breaking process on small aluminum clusters

Alexandrou

Groß

Bacalis

2019

Int J of Quantum Chemistry

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In order to understand the catalytic activity of small metal clusters as a function of their size, we have studied the interaction of CH4 with Al4 and Al5 neutral and charged clusters, as well as neutral thermally expanded clusters in the two lowest lying spin states, using density functional theory. These calculations, via extended search, are used to determine the stable positions of H and CH3 near the cluster, and the transition state to break the H─CH3 bond. In order to understand the factors underlying the reactivity of the clusters, we have analyzed the electronic structure at the transition state. By an analysis of the change of the electronic density of states close to the transition state, we identify the orbitals involved in the bond breaking process. In conjunction with our previous studies of Al2 and Al3 clusters, we find that the small Al clusters, except for Al5, lower the CH3─H dissociation barrier with respect to the gas‐phase value, although Al lacks occupied d‐orbitals. Still, Al5 does not catalyze methane bond breaking, which is attributed to the required interaction with low‐lying Al sp‐states. Furthermore, in all cases where stable methyl‐aluminum‐hydrides are possible, the recombinative desorption of methane is studied by vibrational analysis and application of transition state theory.

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The generation of ground‐state structures and electronic properties of ternary Al_kTi_lNi_m clusters (k + l + m = 4) from a two‐stage density functional theory global searching approach

Cited by 3 publications

References 91 publications

Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Heterogeneous Trimetallic Nanoparticles as Catalysts

Electronic factors determining the methane bond breaking process on small aluminum clusters

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The generation of ground‐state structures and electronic properties of ternary AlkTilNim clusters (k + l + m = 4) from a two‐stage density functional theory global searching approach

Cited by 3 publications

References 91 publications

Generation of ground‐state structures and electronic properties of ternary AlxTiyNiz clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Generation of ground‐state structures and electronic properties of ternary AlxTiyNiz clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Heterogeneous Trimetallic Nanoparticles as Catalysts

Electronic factors determining the methane bond breaking process on small aluminum clusters

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The generation of ground‐state structures and electronic properties of ternary Al_kTi_lNi_m clusters (k + l + m = 4) from a two‐stage density functional theory global searching approach

Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach

Generation of ground‐state structures and electronic properties of ternary Al_xTi_yNi_z clusters (x + y + z = 6) with a two‐stage density functional theory global search approach