Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation

Andreas M. Gänzler; Maria Casapu; Alexey Boubnov; Oliver Müller; Sabrina Conrad; Henning Lichtenberg; Ronald Frahm; Jan Dierk Grunwaldt

doi:10.1016/j.jcat.2015.01.002

Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation

Andreas M. Gänzler, Maria Casapu, Alexey Boubnov, Oliver Müller, Sabrina Conrad, Henning Lichtenberg, Ronald Frahm, Jan Dierk Grunwaldt

Chemical Engineering and Materials Science

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

85 Scopus citations

Abstract

A comprehensive approach was applied to investigate oscillatory CO oxidation over a Pt/Al₂O₃-based diesel oxidation catalyst with small Pt particles (about 1.5 nm diameter) in a fixed-bed microreactor under relevant reaction conditions by combining spatially and time-resolved operando X-ray absorption spectroscopy, infrared thermography, and online mass spectrometry. The catalyst-bed zone responsible for the oscillatory behavior and the emerging hot spot was identified by means of IR thermography. Oscillations of the Pt oxidation state and the hot spot region evolved simultaneously and moved from the end toward the beginning of the catalyst bed with increasing reaction temperature. The changes in CO oxidation activity during oscillations can be unambiguously correlated with dynamic structural changes of the Pt particles. The applied operando approach is complementary to surface science studies and also studies on model Pt particles. Surface oxidation of small Pt nanoparticles leads to a fast deactivation of the catalyst, which is regenerated in a slow reduction step. The presence of metallic Pt is required for high activity of the catalyst.

Original language	English (US)
Pages (from-to)	216-224
Number of pages	9
Journal	Journal of Catalysis
Volume	328
DOIs	https://doi.org/10.1016/j.jcat.2015.01.002
State	Published - Jul 28 2015

Bibliographical note

Funding Information:
KIT and the BMBF projects ‘MatAkt’ and ‘ZeitKatMat’ are gratefully acknowledged for financial support, and SLS (SuperXAS beamline) and ANKA (XAS beamline) for providing beam time. Dr. M. Nachtegaal, Dr. O. Safonova (SLS), and Dr. S. Mangold (ANKA) are gratefully acknowledged for their help and technical support during XAS experiments. FLIR is acknowledged for providing the IR thermography camera and technical assistance. Jan-Dierk Grunwaldt and Ronald Frahm are finally grateful on the fruitful discussions on in situ and operando studies with people at Haldor Topsøe A/S which started with Bjerne Clausen, Alfons Molenbroek, Henrik and Nan Topsøe, Jens Rostrup-Nielsen, and especially inspiring conversations with Haldor Topsøe, who also gave an inspiring talk at HASYLAB.

Publisher Copyright:
© 2015 Elsevier Inc. All rights reserved.

Keywords

CO oxidation
Heterogeneous catalysis
Oscillations
Platinum
Structure-activity relationships

Access

10.1016/j.jcat.2015.01.002

OpenUrl availability

Full text

Cite this

@article{5d1162a27bcf44fa8fa28d529f7bfd57,

title = "Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation",

abstract = "A comprehensive approach was applied to investigate oscillatory CO oxidation over a Pt/Al2O3-based diesel oxidation catalyst with small Pt particles (about 1.5 nm diameter) in a fixed-bed microreactor under relevant reaction conditions by combining spatially and time-resolved operando X-ray absorption spectroscopy, infrared thermography, and online mass spectrometry. The catalyst-bed zone responsible for the oscillatory behavior and the emerging hot spot was identified by means of IR thermography. Oscillations of the Pt oxidation state and the hot spot region evolved simultaneously and moved from the end toward the beginning of the catalyst bed with increasing reaction temperature. The changes in CO oxidation activity during oscillations can be unambiguously correlated with dynamic structural changes of the Pt particles. The applied operando approach is complementary to surface science studies and also studies on model Pt particles. Surface oxidation of small Pt nanoparticles leads to a fast deactivation of the catalyst, which is regenerated in a slow reduction step. The presence of metallic Pt is required for high activity of the catalyst.",

keywords = "CO oxidation, Heterogeneous catalysis, Oscillations, Platinum, Structure-activity relationships",

author = "G{\"a}nzler, {Andreas M.} and Maria Casapu and Alexey Boubnov and Oliver M{\"u}ller and Sabrina Conrad and Henning Lichtenberg and Ronald Frahm and Grunwaldt, {Jan Dierk}",

note = "Funding Information: KIT and the BMBF projects {\textquoteleft}MatAkt{\textquoteright} and {\textquoteleft}ZeitKatMat{\textquoteright} are gratefully acknowledged for financial support, and SLS (SuperXAS beamline) and ANKA (XAS beamline) for providing beam time. Dr. M. Nachtegaal, Dr. O. Safonova (SLS), and Dr. S. Mangold (ANKA) are gratefully acknowledged for their help and technical support during XAS experiments. FLIR is acknowledged for providing the IR thermography camera and technical assistance. Jan-Dierk Grunwaldt and Ronald Frahm are finally grateful on the fruitful discussions on in situ and operando studies with people at Haldor Tops{\o}e A/S which started with Bjerne Clausen, Alfons Molenbroek, Henrik and Nan Tops{\o}e, Jens Rostrup-Nielsen, and especially inspiring conversations with Haldor Tops{\o}e, who also gave an inspiring talk at HASYLAB. Publisher Copyright: {\textcopyright} 2015 Elsevier Inc. All rights reserved.",

year = "2015",

month = jul,

day = "28",

doi = "10.1016/j.jcat.2015.01.002",

language = "English (US)",

volume = "328",

pages = "216--224",

journal = "Journal of Catalysis",

issn = "0021-9517",

publisher = "Academic Press Inc.",

}

TY - JOUR

T1 - Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation

AU - Gänzler, Andreas M.

AU - Casapu, Maria

AU - Boubnov, Alexey

AU - Müller, Oliver

AU - Conrad, Sabrina

AU - Lichtenberg, Henning

AU - Frahm, Ronald

AU - Grunwaldt, Jan Dierk

N1 - Funding Information: KIT and the BMBF projects ‘MatAkt’ and ‘ZeitKatMat’ are gratefully acknowledged for financial support, and SLS (SuperXAS beamline) and ANKA (XAS beamline) for providing beam time. Dr. M. Nachtegaal, Dr. O. Safonova (SLS), and Dr. S. Mangold (ANKA) are gratefully acknowledged for their help and technical support during XAS experiments. FLIR is acknowledged for providing the IR thermography camera and technical assistance. Jan-Dierk Grunwaldt and Ronald Frahm are finally grateful on the fruitful discussions on in situ and operando studies with people at Haldor Topsøe A/S which started with Bjerne Clausen, Alfons Molenbroek, Henrik and Nan Topsøe, Jens Rostrup-Nielsen, and especially inspiring conversations with Haldor Topsøe, who also gave an inspiring talk at HASYLAB. Publisher Copyright: © 2015 Elsevier Inc. All rights reserved.

PY - 2015/7/28

Y1 - 2015/7/28

N2 - A comprehensive approach was applied to investigate oscillatory CO oxidation over a Pt/Al2O3-based diesel oxidation catalyst with small Pt particles (about 1.5 nm diameter) in a fixed-bed microreactor under relevant reaction conditions by combining spatially and time-resolved operando X-ray absorption spectroscopy, infrared thermography, and online mass spectrometry. The catalyst-bed zone responsible for the oscillatory behavior and the emerging hot spot was identified by means of IR thermography. Oscillations of the Pt oxidation state and the hot spot region evolved simultaneously and moved from the end toward the beginning of the catalyst bed with increasing reaction temperature. The changes in CO oxidation activity during oscillations can be unambiguously correlated with dynamic structural changes of the Pt particles. The applied operando approach is complementary to surface science studies and also studies on model Pt particles. Surface oxidation of small Pt nanoparticles leads to a fast deactivation of the catalyst, which is regenerated in a slow reduction step. The presence of metallic Pt is required for high activity of the catalyst.

AB - A comprehensive approach was applied to investigate oscillatory CO oxidation over a Pt/Al2O3-based diesel oxidation catalyst with small Pt particles (about 1.5 nm diameter) in a fixed-bed microreactor under relevant reaction conditions by combining spatially and time-resolved operando X-ray absorption spectroscopy, infrared thermography, and online mass spectrometry. The catalyst-bed zone responsible for the oscillatory behavior and the emerging hot spot was identified by means of IR thermography. Oscillations of the Pt oxidation state and the hot spot region evolved simultaneously and moved from the end toward the beginning of the catalyst bed with increasing reaction temperature. The changes in CO oxidation activity during oscillations can be unambiguously correlated with dynamic structural changes of the Pt particles. The applied operando approach is complementary to surface science studies and also studies on model Pt particles. Surface oxidation of small Pt nanoparticles leads to a fast deactivation of the catalyst, which is regenerated in a slow reduction step. The presence of metallic Pt is required for high activity of the catalyst.

KW - CO oxidation

KW - Heterogeneous catalysis

KW - Oscillations

KW - Platinum

KW - Structure-activity relationships

UR - http://www.scopus.com/inward/record.url?scp=84937909436&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84937909436&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2015.01.002

DO - 10.1016/j.jcat.2015.01.002

M3 - Article

AN - SCOPUS:84937909436

SN - 0021-9517

VL - 328

SP - 216

EP - 224

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation

Abstract

Bibliographical note

Keywords

Access

OpenUrl availability

Other files and links

Fingerprint

Cite this