Near-Surface Accumulation of Hydrogen and CO Blocking Effects on a Pd–Au Alloy

Ogura, Shohei; Okada, Michio; Fukutani, Katsuyuki

doi:10.1021/jp402317h

Cited by 34 publications

(61 citation statements)

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“…17 The sample surface was first exposed to H 2 or D 2 at 140 K to populate the inside of the sample with H or D atoms, respectively. After that the sample was exposed to cis-2-or 1-butene around 100 K, and then TDS spectra of masses 2−4 and 56−68 were taken simultaneously.…”

Section: ■ Experimental Methodsmentioning

confidence: 99%

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

2015

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The H−D exchange reaction is one of the easiest ways to synthesize deuterium-labeled compounds. H−D exchange of olefins has been widely studied on metal surfaces such as Pd and Pt. However, H−D exchange of butene on these surfaces is hardly completed and always accompanied by hydrogenation or dehydrogenation, and its reaction mechanism is yet to be elucidated. In the present study, we investigated the reaction of cis-2-and 1-butenes with H and D atoms absorbed in the near-surface region of Pd 70 Au 30 (110) by using thermal desorption spectroscopy (TDS), reflection−absorption infrared spectroscopy (RAIRS), and TDS simulation. We show complete H−D exchange of both butene isomers without hydrogenation and dehydrogenation. Similar product yield distributions for both butene isomers indicate a fast di-σ bond migration on this surface, which is a key for the complete H−D exchange. Our results would lead to understanding and controlling the catalytic activity and selectivity of the Pd−Au alloy and Pd-related surfaces and would open up a new chemistry using absorbed hydrogen in combination with alloyed surfaces.

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Section: ■ Experimental Methodsmentioning

confidence: 99%

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

2015

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Section: Nuclear Surface Dynamics: Vibration Rotation and Nucleamentioning

confidence: 82%

“…As in case of pure Pd(110), the hydrogen absorption and desorption can also be controlled by CO adsorption on Pd 0.7 Au 0.3 (110) . Figure (a) demonstrates the changes in the hydrogen desorption temperature upon CO adsorption . As realized in Figure , hydrogen is initially charged into Pd 0.7 Au 0.3 (110) by dosing H 2 of 100 L at 140 K, after which the surface is exposed to various amounts of CO.…”

Section: Nuclear Surface Dynamics: Vibration Rotation and Nucleamentioning

confidence: 83%

“…After an ordinary sputtering and annealing process, its surface is dominantly covered by Au with a surface Pd concentration of < 10%. The TPD spectra taken for Pd 0.7 Au 0.3 (110) after dosage of 100 L H 2 at various exposure temperatures are shown in Figure (a) . While almost no H 2 desorption feature is observed at T e =105 K, a significant desorption signal appeared at T e =120 K. The peak area increased substantially with increasing sample temperature during H 2 exposure up to 200 K (inset in Figure (a)), which indicates that some kinetic process governs the hydrogen adsorption or absorption.…”

Section: Nuclear Surface Dynamics: Vibration Rotation and Nucleamentioning

confidence: 98%

“…When the dosing order of H 2 and CO is reversed, on the other hand, H 2 absorption from the gas phase into Pd 0.7 Au 0.3 (110) can be controlled, which is demonstrated in Figure (b) . Here, various amounts of CO are preadsorbed on the surface by annealing the CO‐saturated surface up to temperature TF , and then the surface is exposed to H 2 at 140 K. Figure (b) shows the corresponding TPD spectra .…”

Section: Nuclear Surface Dynamics: Vibration Rotation and Nucleamentioning

confidence: 99%

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Nuclear Dynamics and Electronic Eﬀects of Hydrogen on Solid Surfaces

Fukutani

Wilde

Ogura

2016

The Chemical Record

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Hydrogen is involved in a variety of chemical processes on surfaces. While hydrogen exhibits vibrational and rotational dynamics in its adsorption state, it in some cases undergoes diffusion into the substrate as well as on the surface, and participates in chemical reactions. Furthermore, hydrogen exchanges an electron with surfaces having a significant effect on the surface electronic structure. In this personal account, we review our recent studies on surface nuclear dynamics of hydrogen, hydrogen transport across surfaces, catalytic hydrogenation/isotope exchange reactions, and charge transfer between the surface and hydrogen by using a depth-resolved technique of nuclear reaction analysis and a quantum-state-selective detection of resonance enhanced multiphoton ionization in combination with surface science techniques. As a future prospect, we refer to ultraslow μ spin rotation spectroscopy for a direct probe of the hydrogen charge state at surfaces.

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Polyelemental Nanolithography via Plasma Ion Bombardment: From Fabrication to Superior H₂ Sensing Application

et al. 2018

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use of unique chemical, optical, and electrical properties of each metal component, one can obtain a homo-or heteromixture with unusual optical, electrical, chemical, and catalytic behaviors. On the basis of this knowledge, bi-, tri-, and even tetrametallic nanoscale structures have been synthesized by incorporating several metals into a single structure through various synthetic techniques. The controlled combination of multi-metals at the nanoscale offers an effective way of tuning the chemical and physical properties of nanostructures either by facilitating hybrid chemical, electronic, and magnetic interactions between metal components or by combining different properties associated with each pure component. These properties make multimetallic nanostructures a promising system for diverse applications. In particular, multimetallic nanostructures with spatial arrangement can advantageously be applied to electronics for sensing, charge transfer, and heat transfer behaviors.Controlled synthesis and positioning of multimetallic nanostructures have become increasingly important for systematic study. To date, several methods have been developed for ordered polyelemental nanostructures. For example, important advances have been made in ink-jet printing and blockcopolymer methods, in which two or three metal precursors are reduced in patterned polymer ink or a specific part of a block copolymer to produce bi-or tri-metallic nanospheres. [2] However, these approaches are considerably limited to the number of combinations of metals depending on the compatibility of elements and to the complex shape control of the nanostructures, which can change according to the demands of applications such as line shapes in electronics.In the present work, we developed a new method to fabricate a 3D polyelemental nanopattern with tunable combination, composition, shape, and array by using low-energy Ar + ion plasma. By using this approach, we achieved a 3D polyelemental nanopattern with high resolution (≈10 nm) and high aspect ratio (>20). Our system overcame limitations in terms of shape and arrangement and was adoptable to any metal combination. This method provides a simple and general approach for the fabrication of multimetallic nanopatterns regardless of the synthetic conditions of various metals. Furthermore, the structure formation during secondary sputtering was understood, andThe development of complex nanostructures containing a homo-and heteromixture of two or more metals is a considerable challenge in nanotechnology. However, previous approaches are considerably limited to the number of combinations of metals depending on the compatibility of elements, and to the complex shape control of the nanostructure. In this study, a significant step is taken toward resolving these limitations via the utilization of a low-energy argon-ion bombardment. The multilayer films are etched and re-sputtered on the sidewall of the pre-pattern, which is a secondary sputtering phenomenon. In contrast to the precursor mixing method, most metal...

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Near-Surface Accumulation of Hydrogen and CO Blocking Effects on a Pd–Au Alloy

Cited by 34 publications

References 35 publications

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

Nuclear Dynamics and Electronic Eﬀects of Hydrogen on Solid Surfaces

Polyelemental Nanolithography via Plasma Ion Bombardment: From Fabrication to Superior H₂ Sensing Application

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Near-Surface Accumulation of Hydrogen and CO Blocking Effects on a Pd–Au Alloy

Cited by 34 publications

References 35 publications

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

Complete H–D Exchange of Butene via D Absorbed in a Pd–Au Alloy

Nuclear Dynamics and Electronic Eﬀects of Hydrogen on Solid Surfaces

Polyelemental Nanolithography via Plasma Ion Bombardment: From Fabrication to Superior H2 Sensing Application

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Polyelemental Nanolithography via Plasma Ion Bombardment: From Fabrication to Superior H₂ Sensing Application