Temporal Analysis of Product (TAP)

Fushimi, Rebecca

doi:10.1007/978-3-031-07125-6_40

Cited by 5 publications

(5 citation statements)

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“…Quantifying active species using MZTRT and DRIFTS. Due to its well-defined nature, it is possible to precisely resolve the intrinsic kinetics of catalytic processes using the TAP experiment 40,42 . For linear (first order or pseudo first order) reactions Multi-Zone TAP Reactor Theory 43,44 (MZTRT) is a powerful and efficient tool for simulating TAP exit flux responses.…”

Section: Resultsmentioning

confidence: 99%

“…Temporal Analysis of Products experiments. The TAP technique has been described extensively in the literature 41,42,77 , but it is summarised here. During the TAP experiment a nanomole pulse of gas (~10 15 molecules, 108 μs pulse width) is sent into a packed bed microreactor that is held at ultra-high vacuum (< 10 -9 torr).…”

Section: Measuring the Intrinsic Kinetics Of Co Oxidation On Uc And W...mentioning

confidence: 99%

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Interrogating Site Dependent Kinetics over SiO2-Supported Pt Nanoparticles

Reece,

Kim,

O'Connor

2023

Preprint

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A detailed knowledge of reaction kinetics is key to the development of new more efficient heterogeneous catalytic processes. However, the ability to resolve site dependent kinetics has been largely limited to surface science experiments on model systems. Herein, we can bypass the pressure, materials, and temperature gaps, resolving and quantifying two distinct pathways for CO oxidation over SiO2-supported 2 nm Pt nanoparticles under operando conditions. We find that the pathway distribution directly correlates with the distribution of well-coordinated (e.g., terrace) and under-coordinated (e.g., edge, vertex) CO adsorption sites on the 2 nm Pt nanoparticles as measured by in situ DRIFTS. We conclude that well-coordinated sites follow classic Langmuir-Hinshelwood kinetics, but under-coordinated sites follow non-standard kinetics with CO oxidation being barrierless but conversely also slow. This fundamental method of kinetic site deconvolution is broadly applicable to other catalytic systems, affording bridging of the complexity gap in heterogeneous catalysis.

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Section: Resultsmentioning

confidence: 99%

Section: Measuring the Intrinsic Kinetics Of Co Oxidation On Uc And W...mentioning

confidence: 99%

Interrogating Site Dependent Kinetics over SiO2-Supported Pt Nanoparticles

Reece,

Kim,

O'Connor

2023

Preprint

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“…This makes it possible to "switch on" gas phase collisions, potentially allowing deconvolution of gas phase and surface reactions [23,24]. The examples referenced here are only a small sample of the applications of the TAP technique, with extensive reviews published elsewhere [11,15,16,25]. Figure 2.…”

Section: Overview Of the Tap Experiments Figure 1 (A) Schematic Overv...mentioning

confidence: 99%

“…The TAP systems developed by Gleaves have been described extensively in the previous literature [8,15,25] but the core components are highlighted here. The TAP-2 (and TAP-3) systems consists of an oil diffusion pump (e.g., Varian VHS-10) that is mounted to a large liquid nitrogen cooled chamber that can be isolated from the rest of the system using a gate valve.…”

Section: The Gleaves Tap System Designmentioning

confidence: 99%

“…First, the computer sets the RGA (Stanford Research Systems RGA200) to the desired M/Z value to be recorded during the pulse. The selection of RGA is highly important, and two systems were tested as part of this work: a Hiden 3F PIC and the Stanford Research Systems (SRS) RGA200 both of which have been used in TAP systems developed by Gleaves [25]. It was found that the radial asymmetry that is present in the Hiden 3F PIC ioniser caused the signal response to be modified as a function of RGA orientation, whereas the SRS RGA200 is radially symmetric, and orientation had no effect on the signal.…”

Section: The Pulsing Systemmentioning

confidence: 99%

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Simplifying the Temporal Analysis of Products Reactor

Brandão,

High,

Kim

et al. 2023

Preprint

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The Temporal Analysis of Products (TAP) experiment provides an unparalleled level of kinetic insight into heterogenous catalytic materials, but due to the complex and expensive instrumentation required, its application has been limited to a small group of dedicated researchers. Herein we demonstrate through a series of designs that precisely defined TAP experiments can be performed on systems far smaller and simpler than previously imagined. The pulse reactors described in this work utilise readily available components and so can be assembled, operated, and maintained with minimal training. Using the case study of CO oxidation over a Pt/SiO2 catalyst we show that precise kinetic, mechanistic, and surface composition information is feasible using our single-valve design. With the developments outlined in this work we aim to decrease the activation barrier to TAP and open up the technique to a new generation of researchers.

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