Electron Flow Generated by Gas Phase Exothermic Catalytic Reactions Using a Platinum−Gallium Nitride Nanodiode

Ji, Xiaozhong; Zuppero, Anthony; Gidwani, and Jawahar M.; Somorjai, Gábor A.

doi:10.1021/ja050945m

Cited by 49 publications

(61 citation statements)

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“…As the surface becomes less positively charged, the acetonitrile orientation flips 180° with the CH 3 group pointing toward the surface. We constructed a so called catalytic nanodiode (59)(60)(61), which is composed of a metal of thickness less than the mean free path of hot electrons, deposited on a semiconductor surface, as shown in Figure 8a. When exothermic catalytic chemical reactions occur, we find that the heat transferred is converted to a hot electron flow that can pass through the metal film into the semiconductor which has a Schottky barrier (62; 63), which allows the passing of energetic electrons in one direction but not in the other direction.…”

Section: Future Directions Of Molecular Surface Sciencementioning

confidence: 99%

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Somorjai

Park

2009

Surface Science

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Over the past forty years, surface science has evolved to become both an atomic scale and a molecular scale science. Gerhard Ertl's group has made major contributions in the field of molecular scale surface science, focusing on vacuum studies of adsorption chemistry on single crystal surfaces. In this review, we outline three important aspects that led to the recent advances of surface chemistry: the development of concepts, in situ instruments for molecular scale surface studies at buried interfaces (solid-gas and solidliquid), and new model nanoparticle surface systems in addition to single crystals.Combined molecular beam surface scattering and low energy electron diffraction (LEED)-surface structure studies on metal single crystal surfaces revealed new concepts, including adsorbate-induced surface restructuring and the unique activity of defects, atomic steps and kinks on metal surfaces. We have combined high pressure catalytic reaction studies with ultrahigh vacuum (UHV) surface characterization techniques using the UHV chamber equipped with a high-pressure reaction cell. New instruments, such as high pressure sum frequency generation (SFG) vibrational spectroscopy and scanning tunneling microscopy (STM) have been built that permit molecular-level surface studies performed at pressures. Tools that can access broad ranges of pressures can be used for both the in situ characterization of buried interfaces of solid-gas and solid-liquid and the study of catalytic reaction intermediates. The model systems for the study of molecular 2 surface chemistry have evolved from single crystals to nanoparticles in the 1-10 nm size range, which are the preferred media in catalytic reaction studies.

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Section: Future Directions Of Molecular Surface Sciencementioning

confidence: 99%

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Somorjai

Park

2009

Surface Science

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“…If the metal thickness is of the order of the electron mean free path, hot electrons can be collected during ballistic transport across the metal. Recent experimental 11-14 and theoretical 10,15 studies have demonstrated electronic excitations created during chemisorption and physisorption of gases at surfaces, and by chemical reactions at surfaces [16][17][18] .…”

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Probing Hot Electron Flow Generated on Pt Nanoparticles with Au/TiO₂Schottky Diodes during Catalytic CO Oxidation

et al. 2008

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Hot electron flow generated on colloid platinum nanoparticles during exothermic catalytic carbon monoxide oxidation was directly detected with Au/TiO 2 diodes.Although Au/TiO 2 diodes are not catalytically active, platinum nanoparticles on Au/TiO 2 exhibit both chemicurrent and catalytic turnover rate. Hot electrons are generated on the surface of the metal nanoparticles and go over the Schottky energy barrier between Au and TiO 2 . The continuous Au layer ensures that the metal nanoparticles are electrically connected to the device. The overall thickness of the metal assembly (nanoparticles and Au thin film) is comparable to the mean free path of hot electrons, resulting inballistic transport through the metal. The chemicurrent and chemical reactivity of nanoparticles with citrate, hexadecylamine, hexadecylthiol, and TTAB (Tetradecyltrimethylammonium Bromide) capping agents were measured during catalytic CO oxidation at pressures of 100 Torr O 2 and 40 Torr CO at 373~513 K. We found that chemicurrent yield varies with each capping agent, but always decreases with increasing temperature. We suggest that this inverse temperature dependence is associated with the influence of charging effects due to the organic capping layer during hot electron transport through the metal-oxide interface.

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“…[8,33,101] [40,41,107] Wir detektierten einen Strom "heißer" Elektronen mithilfe einer Schottky-Diode. [38,39,106,108] Werden Metallpartikel [59] oder ein Film [109] mit Durchmessern bzw. einer Dicke ähnlich der mittleren freien Weglänge für Elektronen (ca.…”

Section: Ladungstransportunclassified

Molekulare Faktoren der katalytischen Selektivität

Somorjai

Park

2008

Angewandte Chemie

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Abbildung 3. Entwicklung von Oberflächenmodellen: von der Einkristalloberfläche zu Nanopartikeln, Nanodrähten und Nanodioden. Abbildung 4. Einstufige Synthese monodisperser Rhodiumnanopartikel. acac: Acetylacetonat. Abbildung 5. Monodisperse Platinnanopartikel mit einheitlichen Größen von 1.7 bis 7.2 nm (a) und mit definierter Würfel-oder Kuboktaederform (b). Maßstab in (a): 10 nm; Maßstäbe in (b): 50 nm (links) und 5 nm (rechts). Die Prozentwerte in (b) beziehen sich auf den prozentualen Anteil der Nanopartikel mit der jeweiligen Form.

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Electron Flow Generated by Gas Phase Exothermic Catalytic Reactions Using a Platinum−Gallium Nitride Nanodiode

Cited by 49 publications

References 6 publications

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Probing Hot Electron Flow Generated on Pt Nanoparticles with Au/TiO₂Schottky Diodes during Catalytic CO Oxidation

Molekulare Faktoren der katalytischen Selektivität

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Electron Flow Generated by Gas Phase Exothermic Catalytic Reactions Using a Platinum−Gallium Nitride Nanodiode

Cited by 49 publications

References 6 publications

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Probing Hot Electron Flow Generated on Pt Nanoparticles with Au/TiO2Schottky Diodes during Catalytic CO Oxidation

Molekulare Faktoren der katalytischen Selektivität

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Probing Hot Electron Flow Generated on Pt Nanoparticles with Au/TiO₂Schottky Diodes during Catalytic CO Oxidation