Drifts and TPD analyses of ethanol on Pt catalysts over Al2O3 and ZrO2—partial oxidation of ethanol

Schmal, Martín; César, Deborah Vargas; Souza, Mariana M.V.M.; Guarido, Carlos E.

doi:10.1002/cjce.20597

Cited by 29 publications

(7 citation statements)

References 36 publications

(48 reference statements)

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“…2-butanone, cyclopentanone) or from partial oxidation products (e.g. aldehydes) of alcohols during the storage experiment [42,48]. Partial oxidation of alcohols also results in the observed absorption bands at about 1590 and 1475 cm −1 in blend 1 that have previously been attributed to the asymmetric and symmetric stretching of acetate species, respectively, in the case of ethanol [49,50].…”

Section: Tp-driftsmentioning

confidence: 75%

Sorption and Reaction of Biomass Derived HC Blends and Their Constituents on a Commercial Pt–Pd/Al2O3 Oxidation Catalyst

et al. 2021

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Within the Research Cluster of Excellence “The Fuel Science Center” at RWTH Aachen University, the production and application of new fuels from bio-based carbon feedstocks and CO2 with hydrogen from renewable electricity generation is being investigated. In this study, the storage and oxidation of ethanol, 1-butanol, 2-butanone, cyclopentanone, and cyclopentane as well as two blends thereof on a series production Pt–Pd/Al2O3 oxidation catalyst were investigated. Hydrocarbon (HC) storage and temperature-programmed surface reaction (TPSR) experiments were carried out to analyze their adsorption and desorption behavior. In addition, the individual HCs and both blends were investigated using Diffuse Reflectance Infrared Fourier Transform Spectroscopy (TP-DRIFTS). In general, all oxygenated HCs are adsorbed more strongly than cyclopentane due to their higher polarity. Interestingly, it could be observed that the two different blends [blend 1: ethanol (50 mol %), 2-butanone (21 mol %), cyclopentanone (14 mol %) and cyclopentane (15 mol %); blend 2: 1-butanol (45 mol %), ethanol (29 mol %) and cyclopentane (27 mol %)] exhibit a different storage behavior compared to the single hydrocarbons. It was shown that the presence of 1-butanol and cyclopentane in blend 2 strongly inhibits the oxidation of ethanol. As a result, the ethanol light-off temperature was increased by at least 100 K. A difference was also found in the storage behavior of cyclopentane. While no significant storage could be detected in the pure compound experiment, the experiments with both mixtures showed a larger amount stored. The presence of adsorbed species of the hydrocarbons and their corresponding reaction products has been demonstrated and gives an insight into the storage mechanism of blends. Graphic Abstract

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Section: Tp-driftsmentioning

confidence: 75%

Sorption and Reaction of Biomass Derived HC Blends and Their Constituents on a Commercial Pt–Pd/Al2O3 Oxidation Catalyst

et al. 2021

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“…We first performed series of ethanol TPD experiments over γ-Al temperature [43,45]. After 700 o C activation, the desorption peak shifted to ~ 230 o C which is slightly higher than that on alumina after activated at 500 o C and, at the same time, the desorption peak intensity decreased significantly.…”

Section: Resultsmentioning

confidence: 99%

Modification of the acid/base properties of γ-Al2O3 by oxide additives: An ethanol TPD investigation

et al. 2016

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The electronic properties of oxide-modified γ-Al 2 O 3 surfaces were investigated by using ethanol TPD. Ethanol TPD showed remarkable sensitivity toward the surface structures and electronic properties of the aluminas modified by various transition metal oxides. Maximum desorption rates for the primary product of ethanol adsorption, ethylene, were observed at 225 °C on non-modified γ-Al 2 O 3. Desorption temperature of ethanol over a γ-Al 2 O 3 samples with different amounts of BaO linearly increased with increasing loading. On the contrary, ethanol desorption temperature on Pt modified γ-Al 2 O 3 after calcined at 500 o C linearly decreased with increasing Pt loading. These results clearly suggested that the acid/base properties of the γ-Al 2 O 3 surface can be strongly affected by ad-atoms. For confirming these arguments, we performed ethanol TPD experiments on various oxide modified γ-Al 2 O 3 and normalized the maximum desorption temperatures based on the same number of oxide dopants. These normalized ethanol desorption temperatures linearly correlate with the electronegativity of the metal atom in the oxide. This linear relationship clearly demonstrates that the acidic properties of alumina surfaces can be systematically changed by ad-atoms.

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“…Ethanol reforming processes, such as steam reforming, partial oxidation, and dry reforming, have been studied experimentally on various transition metal catalysts such as Pt [18][19][20][21][22], Rh [22][23][24][25][26][27], Ru [28], Co [29][30][31], and Ni [32], as well as bimetallics such as RhRu [22] and Rh-Pt [23]. Noble metals are well studied as they are not as susceptible to [37,39], dissociative adsorption of ethanol to acetaldehyde [26], or ethanol dehydration to ethylene [18,40].…”

Section: Experimental Studiesmentioning

confidence: 99%

“…Noble metals are well studied as they are not as susceptible to [37,39], dissociative adsorption of ethanol to acetaldehyde [26], or ethanol dehydration to ethylene [18,40]. These findings were taken into account when developing the elementary reaction pathways in the microkinetic model for ethanol partial oxidation and reforming on Pt.…”

Section: Experimental Studiesmentioning

confidence: 99%

Microkinetic modeling and analysis of ethanol partial oxidation and reforming reaction pathways on platinum at short contact times

Koehle

Mhadeshwar

2012

Chemical Engineering Science

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2013iii ACKNOWLDGEMENTSThere are many people without whom this thesis would not have been possible. I must thank Ashish Mhadeshwar for the incredible amount of knowledge he imparted and the guidance he provided in order for this research to be conducted, shared at conferences and published. Many thanks to Doug Cooper, Bill Mustain and Ranjan Srivastava for standing in as advisors and providing support that was above and beyond expectations. I want to thank everyone that has become part of my UConn family, without whom this project would have been possible but much less fun:

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Drifts and TPD analyses of ethanol on Pt catalysts over Al₂O₃ and ZrO₂—partial oxidation of ethanol

Cited by 29 publications

References 36 publications

Sorption and Reaction of Biomass Derived HC Blends and Their Constituents on a Commercial Pt–Pd/Al2O3 Oxidation Catalyst

Sorption and Reaction of Biomass Derived HC Blends and Their Constituents on a Commercial Pt–Pd/Al2O3 Oxidation Catalyst

Modification of the acid/base properties of γ-Al2O3 by oxide additives: An ethanol TPD investigation

Microkinetic modeling and analysis of ethanol partial oxidation and reforming reaction pathways on platinum at short contact times

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