Facile Ester Synthesis on Ag-Modified Nanoporous Au: Oxidative Coupling of Ethanol and 1-Butanol Under UHV Conditions

Stowers, Kara J.; Madix, Robert J.; Biener, Monika M.; Biener, Juergen; Friend, Cynthia M.

doi:10.1007/s10562-015-1525-4

Cited by 15 publications

(33 citation statements)

References 31 publications

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“…These single-crystal alloy studies in turn provide a bridge to understanding O 2 dissociation on AgAu alloy materials with a greater degree of structural complexity, such as npAu, under well-controlled low-pressure conditions [30]. The recombination of O atoms to form molecular oxygen is the microscopic reverse of O 2 dissociation, and the peak temperatures for O recombination are diagnostic of the different O 2 dissociation sites on the crystal surface [22].…”

Section: Correlating Across Pressures and Compositions: The Role Of Omentioning

confidence: 99%

“…Through judicious control of the oxygen dosing temperature in surface science studies on npAg 0.03 Au 0.97 , atomic O was identified as the oxygen species which is responsible for the oxidative reactivity of npAg 0.03 Au 0.97 [30]. Intact molecular oxygen desorbs from npAg 0.03 Au 0.97 below 300 K under well-controlled low-pressure conditions and therefore dosing O 2 at 300 K leaves only adsorbed atomic O on the surface.…”

Section: Correlating Across Pressures and Compositions: The Role Of Omentioning

confidence: 99%

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Catalyst design for enhanced sustainability through fundamental surface chemistry

Personick

Montemore

Kaxiras

et al. 2016

Phil. Trans. R. Soc. A.

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Decreasing energy consumption in the production of platform chemicals is necessary to improve the sustainability of the chemical industry, which is the largest consumer of delivered energy. The majority of industrial chemical transformations rely on catalysts, and therefore designing new materials that catalyse the production of important chemicals via more selective and energy-efficient processes is a promising pathway to reducing energy use by the chemical industry. Efficiently designing new catalysts benefits from an integrated approach involving fundamental experimental studies and theoretical modelling in addition to evaluation of materials under working catalytic conditions. In this review, we outline this approach in the context of a particular catalyst-nanoporous gold (npAu)-which is an unsupported, dilute AgAu alloy catalyst that is highly active for the selective oxidative transformation of alcohols. Fundamental surface science studies on Au single crystals and AgAu thin-film alloys in combination with theoretical modelling were used to identify the principles which define the reactivity of npAu and subsequently enabled prediction of new reactive pathways on this material. Specifically, weak van der Waals interactions are key to the selectivity of Au materials, including npAu. We also briefly describe other systems in which this integrated approach was applied.

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Section: Correlating Across Pressures and Compositions: The Role Of Omentioning

confidence: 99%

Section: Correlating Across Pressures and Compositions: The Role Of Omentioning

confidence: 99%

Catalyst design for enhanced sustainability through fundamental surface chemistry

Personick

Montemore

Kaxiras

et al. 2016

Phil. Trans. R. Soc. A.

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“…This difference could present an advantage for the ozone-activated materials for selective oxidation in the presence of CO.Further, previous studies with npAu ingots activated solely with the flowing reactant stream reported only the formation of butyraldehyde from the oxidation of 1-butanol, with no evidence of the coupling product, butyl butyrate,34 but the ozone-activated materials readily self-couple butanol. This reaction was revisited under catalytic conditions after controlled studies in UHV showed that npAu can effectively catalyze the self-coupling of 1-butanol and ethanol (see below) 35. Under a flow of 5.36% 1-butanol and 20% O 2 in He (50 mL/min), butyl butyrate was…”

mentioning

confidence: 99%

Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation

Personick¹,

Zugic²,

Biener

et al. 2015

ACS Catal.

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131

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We report a new method for facile and reproducible activation of nanoporous gold (npAu) materials of different forms for the catalytic selective partial oxidation of alcohols under ambient pressure, steady flow conditions. This method, based on the surface cleaning of npAu ingots with ozone to remove carbon documented in ultrahigh vacuum conditions, produces active npAu catalysts from ingots, foils and shells by flowing an ozone/dioxygen mixture over the catalyst at 150 °C, followed by a temperature ramp from 50-150 °C in a flowing stream of 10% methanol and 20% oxygen. With this treatment all three materials (ingots, foils, and shells) can be reproducibly activated, despite potential carbonaceous poisons resulting from their synthesis, and are highly active for the selective oxidation of primary alcohols over prolonged periods of time.

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“…The current research in gold catalysis consists of the study of catalytic reactions on nanoporous catalysts [261][262][263][264][265]. The nanoporous Au, npAu, consists of a 3D structure of interconnected pores and ligaments with a ligament size in the 20-100 nm range.…”

Section: Processes On Self-supported Aumentioning

confidence: 99%

“…In this work, the authors focused on influence of ozone activation on the catalyst to improve the selectivity towards alcohol oxidation reactions. One of the key steps towards this goal is the dissociation of oxygen species at the surface of the catalyst, and Ag provides active sites for oxygen dissociation [261][262][263][264][265].…”

Section: Nanoporous Au As Catalyst For Selective Alcohol Oxidationmentioning

confidence: 99%

Dynamic Processes on Gold-Based Catalysts Followed by Environmental Microscopies

et al. 2017

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Abstract:Since the early discovery of the catalytic activity of gold at low temperature, there has been a growing interest in Au and Au-based catalysis for a new class of applications. The complexity of the catalysts currently used ranges from single crystal to 3D structured materials. To improve the efficiency of such catalysts, a better understanding of the catalytic process is required, from both the kinetic and material viewpoints. The understanding of such processes can be achieved using environmental imaging techniques allowing the observation of catalytic processes under reaction conditions, so as to study the systems in conditions as close as possible to industrial conditions. This review focuses on the description of catalytic processes occurring on Au-based catalysts with selected in situ imaging techniques, i.e., PEEM/LEEM, FIM/FEM and E-TEM, allowing a wide range of pressure and material complexity to be covered. These techniques, among others, are applied to unravel the presence of spatiotemporal behaviours, study mass transport and phase separation, determine activation energies of elementary steps, observe the morphological changes of supported nanoparticles, and finally correlate the surface composition with the catalytic reactivity.

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Facile Ester Synthesis on Ag-Modified Nanoporous Au: Oxidative Coupling of Ethanol and 1-Butanol Under UHV Conditions

Cited by 15 publications

References 31 publications

Catalyst design for enhanced sustainability through fundamental surface chemistry

Catalyst design for enhanced sustainability through fundamental surface chemistry

Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation

Dynamic Processes on Gold-Based Catalysts Followed by Environmental Microscopies

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