Interplay of theoretical calculations and experiments for a study of catalysis by gold

Okumura, Mitsutaka; Haruta, Masatake

doi:10.1016/j.cattod.2015.05.006

Cited by 25 publications

(12 citation statements)

References 54 publications

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“…Stabilizing the nanoparticles against agglomeration during operation is a challenge . For some metals such as gold, nanocrystal faceting affects catalytic function . This motivates the use of seeds and ligands to improve shape uniformity, but ligands to synthesize and stabilize nanoparticles can inhibit catalysis.…”

Section: Commercial Applicationsmentioning

confidence: 99%

Nanoparticle Manufacturing – Heterogeneity through Processes to Products

Stavis¹,

Fagan²,

Stopa

et al. 2018

ACS Appl. Nano Mater.

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Commercial products are now making use of the unique properties of nanoscale particles. However, common challenges of making nanoparticles into products still limit their impact. In this article, we review recent advances in nanoparticle manufacturing in liquids, clarifying the similarities between different processes and products at a system level. Our integrative survey emphasizes the fundamental challenge of heterogeneity, which propagates through manufacturing processes and increases the cost of quality control. We also consider the central constraint of production scale, external costs of safety and sustainability, and technology transfer from the laboratory to the market. We review applications of nanoparticles in nanocomposite materials, healthcare and medicine, electronics and photonics, and energy and the environment, and conclude with a summary of the critical issues.

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Section: Commercial Applicationsmentioning

confidence: 99%

Nanoparticle Manufacturing – Heterogeneity through Processes to Products

Stavis¹,

Fagan²,

Stopa

et al. 2018

ACS Appl. Nano Mater.

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“…Few-atomg old clusters have been shown to be highly active for selected catalytic reactions, [1][2][3] such as CO oxidation, [4,5] the water-gas shift reaction, [6] O 2 activation, [7] propene epoxidation, [5,8,9] methanea ctivation, [10] and water splitting. [11,12] Gold clusters exhibit high reaction rates, with as trong dependence on the precise cluster size and charge state.…”

Section: Introductionmentioning

confidence: 99%

“…[21][22][23] The geometry of pure neutral gold clusters (clustersc onsisting only of gold atoms are referred to as pure clusters in this paper) is planar up to n = 10, [24] while yttriumdopedg old clusters are quasi-planar up to Au 8 Yf or mostc luster sizes. However,A u 4 Yh as a3 Ds hapea nd also Au nÀ1 Y( n = 6-9) clusters are slightly distorted from ap erfect planar shape. [23] Electronically,t he trivalenty ttrium dopant alters the electronic shell structure of the gold clusters, for example, Au 6 Y + and Au 16 Y + both have closed electronic structures with 8a nd 18 itinerant electrons,r espectively.T he enhanceds tabilities of these clusters explain their high relative abundance in photofragmentatione xperiments.…”

Section: Introductionmentioning

confidence: 99%

Non‐covalent Interactions and Charge Transfer between Propene and Neutral Yttrium‐Doped and Pure Gold Clusters

Barabás

Vanbuel

Ferrari

et al. 2019

Chemistry A European J

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The dopant and size‐dependent propene adsorption on neutral gold (Aun) and yttrium‐doped gold (Aun−1Y) clusters in the n=5–15 size range are investigated, combining mass spectrometry and gas phase reactions in a low‐pressure collision cell and density functional theory calculations. The adsorption energies, extracted from the experimental data using an RRKM analysis, show a similar size dependence as the quantum chemical results and are in the range of ≈0.6–1.2 eV. Yttrium doping significantly alters the propene adsorption energies for n=5, 12 and 13. Chemical bonding and energy decomposition analysis showed that there is no covalent bond between the cluster and propene, and that charge transfer and other non‐covalent interactions are dominant. The natural charges, Wiberg bond indices, and the importance of charge transfer all support an electron donation/back‐donation mechanism for the adsorption. Yttrium plays a significant role not only in the propene binding energy, but also in the chemical bonding in the cluster‐propene adduct. Propene preferentially binds to yttrium in small clusters (n<10), and to a gold atom at larger sizes. Besides charge transfer, relaxation also plays an important role, illustrating the non‐local effect of the yttrium dopant. It is shown that the frontier molecular orbitals of the clusters determine the chemical bonding, in line with the molecular‐like electronic structure of metal clusters.

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“…Gold has been enjoyed as the most inert metal for a very long time, until the pioneer of Haruta [1,2] found that the gold nanoparticles supported on some metal oxides showed surprisingly high catalytic activity for small molecule reaction at low temperature. , the Nano gold catalysis has picturesque growing in the field of heterogeneous catalysis [3][4][5]. Technologically, numerous potential industrialization applications of Nano gold catalysts were developed, such as synthesis of fine chemicals [6,7], selective hydrogenations [8,9], water gas shift reaction [10], carbon-carbon bond forming reaction [11], oxidation of organic compounds with molecular O 2 [12,13], pollution and emission control [14] and fuel cell applications [15,16] Scientifically, a huge number of theoretical and experimental studies have been devoted to understand the wide gap between the chemical inertness of bulk gold and high catalytic activity of Nano gold [17][18][19][20][21].…”

Section: Introductionmentioning

confidence: 99%

Kinetics Study The Catalyze Mode Of The Formamide Degradation Reaction By Aux Cluster (X=0, 1, 2, 3): Point, Line Or Surface?

Liu¹,

Liu²,

Teixeira

et al. 2018

BJSTR

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The related energy and multi-channel CHONH 2 degradation reaction potential energy surface under the catalysis of Aux (x=0, 1, 2, 3) cluster was studied, while its dynamic characterization has been investigated with density functional calculations. The geometries were fully optimized with the CCSD(T)//B3PW91 level. We can conclude two results: [1] The calculated results shown that the main pathway of the CHONH 2 degradation reaction under the catalysis of Aux (x=0, 1, 2, 3) cluster can give the main product P1 (CO+NH 3 ), while the minor product is P1(H 2 +HNCO) and P3 (H 2 O+HNC). We calculated the rate constant of the main reaction pathway, the calculated dynamic characterization indicating that the rate constants have the positive temperature dependence. According to the dynamic results and the energetically intermediates and transition states involved in the dominant paths, the reaction is expected to be occurred the most rapidly under the catalysis of Au 2 . [2] From the PESs, we can see the present invention, the singlet atom is the best catalysis and can catalyze the reaction better. The present invention studies may provide useful information on the issues of the reaction mechanism and product distributions.

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Interplay of theoretical calculations and experiments for a study of catalysis by gold

Cited by 25 publications

References 54 publications

Nanoparticle Manufacturing – Heterogeneity through Processes to Products

Nanoparticle Manufacturing – Heterogeneity through Processes to Products

Non‐covalent Interactions and Charge Transfer between Propene and Neutral Yttrium‐Doped and Pure Gold Clusters

Kinetics Study The Catalyze Mode Of The Formamide Degradation Reaction By Aux Cluster (X=0, 1, 2, 3): Point, Line Or Surface?

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