Balanced Fast-SpaciMS capillary configurations provide practically noninvasive channel-average measurements in catalytic monoliths

Tomáš Hlavatý; Petr Kočí; Martin Isoz; Dhruba Deka; William Partridge

doi:10.1016/j.ces.2023.119272

Balanced Fast-SpaciMS capillary configurations provide practically noninvasive channel-average measurements in catalytic monoliths

Tomáš Hlavatý, Petr Kočí, Martin Isoz, Dhruba Deka, William Partridge

Applied Catalysis&Emissions Res. Group

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

4 Scopus citations

Abstract

Spatially resolved capillary-inlet mass spectrometry (SpaciMS) provides a detailed picture of the spatiotemporal evolution of reaction network in catalytic monoliths. In the present work, we combine the SpaciMS experiments with a newly developed non-isothermal 3D CFD model for heterogeneously catalyzed reactive flows, including diffusion and permeation through the coated catalyst and channel wall. We explore how the capillary size and sampling rate can be balanced to minimize the impact on probed-channel conversions and provide species concentration measurements representative of the free channel average. In all studied configurations, the balanced sampling-rate fraction is noticeably higher than the corresponding capillary occlusion fraction. For a typical 350-micron capillary that occupies 11% of the channel cross- section, the balanced sampling rate represents 43% of the channel flow. The present work shows that together, a balanced SpaciMS configuration and numerical simulation provide accurate channel-averaged information of a monolithic catalyst under realistic operation conditions.

Original language	English
Article number	119272
Journal	Chemical Engineering Science
Volume	282
DOIs	https://doi.org/10.1016/j.ces.2023.119272
State	Published - Dec 5 2023

Funding

The work was financially supported by the Czech Science Foundation (GA 22-12227S). T.H. and M.I. acknowledge the institutional support RVO:61388998 (Czech Academy of Sciences). The contributions of D.D. and W.P. were supported by the US DOE Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. This manuscript has been co-authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). The work was financially supported by the Czech Science Foundation (GA 22-12227S ). T.H. and M.I. acknowledge the institutional support RVO:61388998 ( Czech Academy of Sciences ). The contributions of D.D. and W.P. were supported by the US DOE Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office . This manuscript has been co-authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

CFD
CO oxidation
SpaciFTIR
SpaciMS
Three-way catalyst

Access to Document

10.1016/j.ces.2023.119272

Cite this

@article{f69c09adf5e94df58ee537dd1142f3cd,

title = "Balanced Fast-SpaciMS capillary configurations provide practically noninvasive channel-average measurements in catalytic monoliths",

abstract = "Spatially resolved capillary-inlet mass spectrometry (SpaciMS) provides a detailed picture of the spatiotemporal evolution of reaction network in catalytic monoliths. In the present work, we combine the SpaciMS experiments with a newly developed non-isothermal 3D CFD model for heterogeneously catalyzed reactive flows, including diffusion and permeation through the coated catalyst and channel wall. We explore how the capillary size and sampling rate can be balanced to minimize the impact on probed-channel conversions and provide species concentration measurements representative of the free channel average. In all studied configurations, the balanced sampling-rate fraction is noticeably higher than the corresponding capillary occlusion fraction. For a typical 350-micron capillary that occupies 11% of the channel cross- section, the balanced sampling rate represents 43% of the channel flow. The present work shows that together, a balanced SpaciMS configuration and numerical simulation provide accurate channel-averaged information of a monolithic catalyst under realistic operation conditions.",

keywords = "CFD, CO oxidation, SpaciFTIR, SpaciMS, Three-way catalyst",

author = "Tom{\'a}{\v s} Hlavat{\'y} and Petr Ko{\v c}{\'i} and Martin Isoz and Dhruba Deka and William Partridge",

note = "Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

year = "2023",

month = dec,

day = "5",

doi = "10.1016/j.ces.2023.119272",

language = "English",

volume = "282",

journal = "Chemical Engineering Science",

issn = "0009-2509",

publisher = "Elsevier",

}

TY - JOUR

T1 - Balanced Fast-SpaciMS capillary configurations provide practically noninvasive channel-average measurements in catalytic monoliths

AU - Hlavatý, Tomáš

AU - Kočí, Petr

AU - Isoz, Martin

AU - Deka, Dhruba

AU - Partridge, William

PY - 2023/12/5

Y1 - 2023/12/5

N2 - Spatially resolved capillary-inlet mass spectrometry (SpaciMS) provides a detailed picture of the spatiotemporal evolution of reaction network in catalytic monoliths. In the present work, we combine the SpaciMS experiments with a newly developed non-isothermal 3D CFD model for heterogeneously catalyzed reactive flows, including diffusion and permeation through the coated catalyst and channel wall. We explore how the capillary size and sampling rate can be balanced to minimize the impact on probed-channel conversions and provide species concentration measurements representative of the free channel average. In all studied configurations, the balanced sampling-rate fraction is noticeably higher than the corresponding capillary occlusion fraction. For a typical 350-micron capillary that occupies 11% of the channel cross- section, the balanced sampling rate represents 43% of the channel flow. The present work shows that together, a balanced SpaciMS configuration and numerical simulation provide accurate channel-averaged information of a monolithic catalyst under realistic operation conditions.

AB - Spatially resolved capillary-inlet mass spectrometry (SpaciMS) provides a detailed picture of the spatiotemporal evolution of reaction network in catalytic monoliths. In the present work, we combine the SpaciMS experiments with a newly developed non-isothermal 3D CFD model for heterogeneously catalyzed reactive flows, including diffusion and permeation through the coated catalyst and channel wall. We explore how the capillary size and sampling rate can be balanced to minimize the impact on probed-channel conversions and provide species concentration measurements representative of the free channel average. In all studied configurations, the balanced sampling-rate fraction is noticeably higher than the corresponding capillary occlusion fraction. For a typical 350-micron capillary that occupies 11% of the channel cross- section, the balanced sampling rate represents 43% of the channel flow. The present work shows that together, a balanced SpaciMS configuration and numerical simulation provide accurate channel-averaged information of a monolithic catalyst under realistic operation conditions.

KW - CFD

KW - CO oxidation

KW - SpaciFTIR

KW - SpaciMS

KW - Three-way catalyst

UR - http://www.scopus.com/inward/record.url?scp=85171981936&partnerID=8YFLogxK

U2 - 10.1016/j.ces.2023.119272

DO - 10.1016/j.ces.2023.119272

M3 - Article

AN - SCOPUS:85171981936

SN - 0009-2509

VL - 282

JO - Chemical Engineering Science

JF - Chemical Engineering Science

M1 - 119272

ER -

Balanced Fast-SpaciMS capillary configurations provide practically noninvasive channel-average measurements in catalytic monoliths

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this