Modeling and Simulation of Transient Adsorption and Reaction in Vacuum Using the Temporal Analysis of Products Reactor

Rothaemel, M.; Baerns, M.

doi:10.1021/ie950379b

Cited by 50 publications

(12 citation statements)

References 25 publications

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“…However, this enhanced HCN production rate decreases rapidly after the introduction of methane. This is due to a limited number of active sites that is available for the methane decomposition [19]. Thus, the hydrogen cyanide production rate seems to correlate with the availability of hydrogen as hydrogen is slowly released from adsorbed ammonia species but rapidly from methane.…”

Section: Discussionmentioning

confidence: 99%

HCN synthesis from methane and ammonia over platinum

Delagrange

Schuurman

2007

Catalysis Today

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The mechanism of the HCN formation from ammonia and methane over Pt black was investigated using a temporal analysis of products (TAPs) reactor system. At 1173 K the hydrogen cyanide production rate depends on the order of introducing the reactants. HCN is formed rapidly on the methane pulse just after introducing ammonia. However, a slow formation of HCN is observed on the ammonia pulse that follows a methane pulse. Moreover the form of the HCN response resembles closely that of the nitrogen and hydrogen also released during the ammonia pulse. Thus, the rate-determining step for the formation of HCN is the decomposition rate of ammonia. A reaction sequence based on elementary steps is proposed for the HCN synthesis. The formation of HCN after pulsing H 2 points to a pool of surface intermediate species that are hydrogenated to HCN. #

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Section: Discussionmentioning

confidence: 99%

HCN synthesis from methane and ammonia over platinum

Delagrange

Schuurman

2007

Catalysis Today

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“…31,148,149 Analytical advances specific to the TAP methodology have also been reported. 146,[150][151][152][153][154] Since 2001 a step-by-step advancement of the mathematical theory of the TAP "reaction-diffusion" systems has been constructed, including:…”

Section: Discussionmentioning

confidence: 99%

Forty years of temporal analysis of products

Morgan

Maguire

Fushimi

et al. 2017

Catal. Sci. Technol.

131

101

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A detailed understanding of reaction mechanisms and kinetics is required in order to develop and optimize catalysts and catalytic processes. While steady-state investigations are known to give a global view of the catalytic system, transient studies are invaluable since they can provide more comprehensive insight into elementary steps. For almost forty years temporal analysis of products (TAP) has been successfully utilized for transient studies of gas phase heterogeneous reactions, and there have been a number of advances in instrumentation and numerical modeling methods in that time. Since TAP is a complex methodology it is often viewed as a niche specialty. With the purpose to make TAP more relevant and approachable to a wider segment of the catalytic research community, part of the intention of this work is to highlight the significant contributions TAP has made to elucidating mechanistic and kinetic aspects of complex, multistep heterogeneous reactions. With this in mind, an outlook is also disclosed for the technique in terms of what is needed to revitalize the field and make it more applicable to the recent advances in catalyst characterization (e.g. operando modes).

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“…[48] Pressure conditions for TAP pulse experiments have been investigated in detail by Rothaemel and Baerns. [50] b) Irreversible and reversible adsorption phenomena on SZs in TAP Pulse experiments with n-butane on SZs were carried out with both powder catalysts. The time-dependent pulse responses of the main fragment (m/z 43) at various temperatures are shown www.chemcatchem.org in Figure 6 as both measured intensities and height-normalized intensities.…”

Section: Transient Experiments With Tap A) Tap Working Conditions Formentioning

confidence: 99%

An Integrated Catalytic and Transient Study of Sulfated Zirconias: Investigation of the Reaction Mechanism and the Role of Acidic Sites in n‐Butane Isomerization

Breitkopf¹

2009

ChemCatChem

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The transient temporal analysis of products (TAP) pulse method has been applied to investigate the isomerization of n‐butane on sulfated zirconias at very low pressure. By combining these results with findings from XRD, XPS, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), temperature‐programmed desorption (TPD), and catalytic studies at atmospheric pressure, a wide range of pressure conditions can be accessed to study the influence of surface sulfate groups on the isomerization activity and the mechanism of this reaction. The catalytic activity of powder catalysts has been correlated to the surface site density of sulfates, with pyrosulfate structures playing a major role in the initiation of the reaction. The complex interplay between sulfate‐free and sulfate‐covered zirconia surfaces for the adsorption of alkanes has been investigated in detail, with TAP pulse experiments showing a monomolecular reaction pathway at low n‐butane partial pressures. Moreover, TAP pulse experiments have allowed detection of the reaction products of this initiation process, including butene and water, and have shown their influence on the deactivation of sulfated zirconias. Heats of adsorption have been calculated from the TAP pulse experiments.

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Modeling and Simulation of Transient Adsorption and Reaction in Vacuum Using the Temporal Analysis of Products Reactor

Cited by 50 publications

References 25 publications

HCN synthesis from methane and ammonia over platinum

HCN synthesis from methane and ammonia over platinum

Forty years of temporal analysis of products

An Integrated Catalytic and Transient Study of Sulfated Zirconias: Investigation of the Reaction Mechanism and the Role of Acidic Sites in n‐Butane Isomerization

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