Towards rigorous multiscale flow models of nanoparticle reactivity in chemical looping applications

Stefan Andersson, Stefan Radl, Ingeborg-Helene Svenum, Stephen A. Shevlin, Z. Xiao Guo, Shahriar Amini

Research output: Contribution to journalArticleResearchpeer-review

Abstract

A multiscale modeling framework is described and applied to the reactivity of iron oxide nanoparticles in a chemical looping reforming (CLR) reactor. At the atomic scale/nanoscale, we have performed kinetic Monte Carlo modeling, guided by Density Functional Theory calculations, on the detailed kinetics of the CH4 conversion to products as a function of temperature. These results have been post-processed for use in macroscopic models with the goal to integrate process information with materials information. Two levels of macroscopic models have been used to evaluate the performance of the nanoparticles in their final application: (1) a pore-unresolved intra-particle transport model that accounts for limitations via an effective diffusivity and an effectiveness factor, and (2) a fluid-particle multiphase flow model that allows the study of the consequences of clustering and intra-particle transport on overall reactor performance. This modeling approach ultimately leads to better descriptors of material performance that can be used in future materials screening activities.
Original languageEnglish
JournalCatalysis Today
DOIs
Publication statusE-pub ahead of print - 10 Jun 2019

Fingerprint

Nanoparticles
Kinetics
Multiphase flow
Reforming reactions
Iron oxides
Density functional theory
Screening
Fluids
Temperature
ferric oxide

Keywords

  • Chemical looping
  • nanoparticles
  • iron oxide
  • multiscale modeling
  • kinetic Monte Carlo
  • flow modeling
  • Nanoparticles
  • Flow modeling
  • Iron oxide
  • Kinetic Monte Carlo
  • Multiscale modeling

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Chemistry(all)
  • Catalysis

Fields of Expertise

  • Mobility & Production

Cite this

Towards rigorous multiscale flow models of nanoparticle reactivity in chemical looping applications. / Andersson, Stefan; Radl, Stefan; Svenum, Ingeborg-Helene; Shevlin, Stephen A.; Guo, Z. Xiao; Amini, Shahriar.

In: Catalysis Today, 10.06.2019.

Research output: Contribution to journalArticleResearchpeer-review

Andersson, Stefan ; Radl, Stefan ; Svenum, Ingeborg-Helene ; Shevlin, Stephen A. ; Guo, Z. Xiao ; Amini, Shahriar. / Towards rigorous multiscale flow models of nanoparticle reactivity in chemical looping applications. In: Catalysis Today. 2019.
@article{0852bbb66e03401b82e3c6e632a6a761,
title = "Towards rigorous multiscale flow models of nanoparticle reactivity in chemical looping applications",
abstract = "A multiscale modeling framework is described and applied to the reactivity of iron oxide nanoparticles in a chemical looping reforming (CLR) reactor. At the atomic scale/nanoscale, we have performed kinetic Monte Carlo modeling, guided by Density Functional Theory calculations, on the detailed kinetics of the CH4 conversion to products as a function of temperature. These results have been post-processed for use in macroscopic models with the goal to integrate process information with materials information. Two levels of macroscopic models have been used to evaluate the performance of the nanoparticles in their final application: (1) a pore-unresolved intra-particle transport model that accounts for limitations via an effective diffusivity and an effectiveness factor, and (2) a fluid-particle multiphase flow model that allows the study of the consequences of clustering and intra-particle transport on overall reactor performance. This modeling approach ultimately leads to better descriptors of material performance that can be used in future materials screening activities.",
keywords = "Chemical looping, nanoparticles, iron oxide, multiscale modeling, kinetic Monte Carlo, flow modeling, Nanoparticles, Flow modeling, Iron oxide, Kinetic Monte Carlo, Multiscale modeling",
author = "Stefan Andersson and Stefan Radl and Ingeborg-Helene Svenum and Shevlin, {Stephen A.} and Guo, {Z. Xiao} and Shahriar Amini",
year = "2019",
month = "6",
day = "10",
doi = "10.1016/j.cattod.2019.06.024",
language = "English",
journal = "Catalysis Today",
issn = "0920-5861",
publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Towards rigorous multiscale flow models of nanoparticle reactivity in chemical looping applications

AU - Andersson, Stefan

AU - Radl, Stefan

AU - Svenum, Ingeborg-Helene

AU - Shevlin, Stephen A.

AU - Guo, Z. Xiao

AU - Amini, Shahriar

PY - 2019/6/10

Y1 - 2019/6/10

N2 - A multiscale modeling framework is described and applied to the reactivity of iron oxide nanoparticles in a chemical looping reforming (CLR) reactor. At the atomic scale/nanoscale, we have performed kinetic Monte Carlo modeling, guided by Density Functional Theory calculations, on the detailed kinetics of the CH4 conversion to products as a function of temperature. These results have been post-processed for use in macroscopic models with the goal to integrate process information with materials information. Two levels of macroscopic models have been used to evaluate the performance of the nanoparticles in their final application: (1) a pore-unresolved intra-particle transport model that accounts for limitations via an effective diffusivity and an effectiveness factor, and (2) a fluid-particle multiphase flow model that allows the study of the consequences of clustering and intra-particle transport on overall reactor performance. This modeling approach ultimately leads to better descriptors of material performance that can be used in future materials screening activities.

AB - A multiscale modeling framework is described and applied to the reactivity of iron oxide nanoparticles in a chemical looping reforming (CLR) reactor. At the atomic scale/nanoscale, we have performed kinetic Monte Carlo modeling, guided by Density Functional Theory calculations, on the detailed kinetics of the CH4 conversion to products as a function of temperature. These results have been post-processed for use in macroscopic models with the goal to integrate process information with materials information. Two levels of macroscopic models have been used to evaluate the performance of the nanoparticles in their final application: (1) a pore-unresolved intra-particle transport model that accounts for limitations via an effective diffusivity and an effectiveness factor, and (2) a fluid-particle multiphase flow model that allows the study of the consequences of clustering and intra-particle transport on overall reactor performance. This modeling approach ultimately leads to better descriptors of material performance that can be used in future materials screening activities.

KW - Chemical looping

KW - nanoparticles

KW - iron oxide

KW - multiscale modeling

KW - kinetic Monte Carlo

KW - flow modeling

KW - Nanoparticles

KW - Flow modeling

KW - Iron oxide

KW - Kinetic Monte Carlo

KW - Multiscale modeling

UR - http://www.scopus.com/inward/record.url?scp=85067228999&partnerID=8YFLogxK

U2 - 10.1016/j.cattod.2019.06.024

DO - 10.1016/j.cattod.2019.06.024

M3 - Article

JO - Catalysis Today

JF - Catalysis Today

SN - 0920-5861

ER -