Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths

Yuhan Wang; Ciaran Coney; Claire McAtee; Geoffrey McCullough; Alexandre Goguet

doi:10.1016/j.apcata.2022.118608

Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths

Yuhan Wang, Ciaran Coney, Claire McAtee, Geoffrey McCullough, Alexandre Goguet^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

2 Citations (Scopus)

26 Downloads (Pure)

Abstract

A spatially resolved technique was developed as a novel methodology to investigate the process of effective diffusions in monolith catalysts. The technique was then applied to the investigation of methane oxidation inside a commercial 3 wt% Pd/Al₂O₃ monolith catalyst. The mass transfer parameters of O₂ and CH₄ were measured, and their effective diffusivities were calculated by a modified Bosanquet approach, which confirmed that the dominant diffusion regime in the substrate and the washcoat were molecular and Knudsen respectively. The applicability of this new approach was assessed via a comparison between simulations of the water-inhibited CH₄ catalytic oxidation using either correlation or experimental-based mass transfer coefficients. This study demonstrates that careful measurement of diffusivity is essential to the accurate modelling of catalyst reaction rates.

Original language	English
Article number	118608
Journal	Applied Catalysis A: General
Volume	638
Early online date	02 May 2022
DOIs	https://doi.org/10.1016/j.apcata.2022.118608
Publication status	Published - 25 May 2022

Bibliographical note

Publisher Copyright:
© 2022 Elsevier B.V.

Keywords

Effective diffusion
Monolith catalysts
SpaciMS
Spatially resolved

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology

Access to Document

10.1016/j.apcata.2022.118608Licence: Unspecified

Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths
Copyright 2022 Elsevier. This manuscript is distributed under a Creative Commons Attribution-NonCommercial-NoDerivs License (https://creativecommons.org/licenses/by-nc-nd/4.0/), which permits distribution and reproduction for non-commercial purposes, provided the author and source are cited.
Accepted author manuscript, 1.12 MBLicence: CC BY-NC-ND

Shedding light on the mechanistic reaction pathways experienced by vehicular after-treatment catalysts : Spatiotemporal mapping and kinetic modelling of catalytic reactions occurring on wash coated monoliths
Coney, C. (Author), Dec 2019
Student thesis: Doctoral Thesis › Doctor of Philosophy

Cite this

@article{5fbf443ceb9b4eb99926713787de9a48,

title = "Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths",

abstract = "A spatially resolved technique was developed as a novel methodology to investigate the process of effective diffusions in monolith catalysts. The technique was then applied to the investigation of methane oxidation inside a commercial 3 wt% Pd/Al2O3 monolith catalyst. The mass transfer parameters of O2 and CH4 were measured, and their effective diffusivities were calculated by a modified Bosanquet approach, which confirmed that the dominant diffusion regime in the substrate and the washcoat were molecular and Knudsen respectively. The applicability of this new approach was assessed via a comparison between simulations of the water-inhibited CH4 catalytic oxidation using either correlation or experimental-based mass transfer coefficients. This study demonstrates that careful measurement of diffusivity is essential to the accurate modelling of catalyst reaction rates.",

keywords = "Effective diffusion, Monolith catalysts, SpaciMS, Spatially resolved",

author = "Yuhan Wang and Ciaran Coney and Claire McAtee and Geoffrey McCullough and Alexandre Goguet",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

month = may,

day = "25",

doi = "10.1016/j.apcata.2022.118608",

language = "English",

volume = "638",

journal = "Applied Catalysis A: General",

issn = "0926-860X",

publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths

AU - Wang, Yuhan

AU - Coney, Ciaran

AU - McAtee, Claire

AU - McCullough, Geoffrey

AU - Goguet, Alexandre

PY - 2022/5/25

Y1 - 2022/5/25

N2 - A spatially resolved technique was developed as a novel methodology to investigate the process of effective diffusions in monolith catalysts. The technique was then applied to the investigation of methane oxidation inside a commercial 3 wt% Pd/Al2O3 monolith catalyst. The mass transfer parameters of O2 and CH4 were measured, and their effective diffusivities were calculated by a modified Bosanquet approach, which confirmed that the dominant diffusion regime in the substrate and the washcoat were molecular and Knudsen respectively. The applicability of this new approach was assessed via a comparison between simulations of the water-inhibited CH4 catalytic oxidation using either correlation or experimental-based mass transfer coefficients. This study demonstrates that careful measurement of diffusivity is essential to the accurate modelling of catalyst reaction rates.

AB - A spatially resolved technique was developed as a novel methodology to investigate the process of effective diffusions in monolith catalysts. The technique was then applied to the investigation of methane oxidation inside a commercial 3 wt% Pd/Al2O3 monolith catalyst. The mass transfer parameters of O2 and CH4 were measured, and their effective diffusivities were calculated by a modified Bosanquet approach, which confirmed that the dominant diffusion regime in the substrate and the washcoat were molecular and Knudsen respectively. The applicability of this new approach was assessed via a comparison between simulations of the water-inhibited CH4 catalytic oxidation using either correlation or experimental-based mass transfer coefficients. This study demonstrates that careful measurement of diffusivity is essential to the accurate modelling of catalyst reaction rates.

KW - Effective diffusion

KW - Monolith catalysts

KW - SpaciMS

KW - Spatially resolved

U2 - 10.1016/j.apcata.2022.118608

DO - 10.1016/j.apcata.2022.118608

M3 - Article

AN - SCOPUS:85129569130

SN - 0926-860X

VL - 638

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

M1 - 118608

ER -

Development of a spatially resolved technique for the measurement of effective diffusions and its application to the modelling of washcoated catalytic monoliths

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

Access to Document

Fingerprint

Student theses

Shedding light on the mechanistic reaction pathways experienced by vehicular after-treatment catalysts : Spatiotemporal mapping and kinetic modelling of catalytic reactions occurring on wash coated monoliths

Cite this