Operando Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of the NO Reduction Reaction over Rhodium-Based Catalysts

Fabiane C. Ballotin; Thomas Hartman; Joris Koek; Robin G. Geitenbeek; Bert M. Weckhuysen

doi:10.1002/cphc.202100375

Operando Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of the NO Reduction Reaction over Rhodium-Based Catalysts

Fabiane C. Ballotin, Thomas Hartman, Joris Koek, Robin G. Geitenbeek, Bert M. Weckhuysen^*

^*Corresponding author for this work

Utrecht University

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

Abstract

Operando shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) with on-line mass spectrometry (MS) has been used to investigate the surface species, such as NO, NOH, NO₂, N₂O, and reaction products of the NO reduction reaction with CO and H₂ over supported Rh-based catalysts in the form of catalyst extrudates. By correlating surface intermediates and reaction products, new insights in the reaction mechanism could be obtained. Upon applying different reaction conditions (i. e., H₂ or CO), the selectivity of the catalytic reaction could be tuned towards the formation of N₂. Furthermore, in the absence of Rh, no reaction products were detected. The importance of the operando SHINERS as a surface-sensitive characterization technique in the field of heterogeneous catalysis provides routes towards a better understanding of catalytic performance.

Original language	English
Pages (from-to)	1595-1602
Number of pages	8
Journal	ChemPhysChem
Volume	22
Issue number	15
DOIs	https://doi.org/10.1002/cphc.202100375
Publication status	Published - 4 Aug 2021

Bibliographical note

Funding Information:
This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. We acknowledge Utrecht University (UU) and Nienke Visser (UU) for performing the TEM-EDX measurements.

Funding Information:
This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. We acknowledge Utrecht University (UU) and Nienke Visser (UU) for performing the TEM‐EDX measurements.

Publisher Copyright:
© 2021 The Authors. ChemPhysChem published by Wiley-VCH GmbH.

Funding

This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. We acknowledge Utrecht University (UU) and Nienke Visser (UU) for performing the TEM‐EDX measurements.

Keywords

NO reduction
operando spectroscopy
Raman Spectroscopy
rhodium
SHINERS

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ChemPhysChem - 2021 - Ballotin - Operando Shell‐Isolated Nanoparticle‐Enhanced Raman Spectroscopy of the NO ReductionFinal published version, 0.98 MBLicence: CC BY

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title = "Operando Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of the NO Reduction Reaction over Rhodium-Based Catalysts",

abstract = "Operando shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) with on-line mass spectrometry (MS) has been used to investigate the surface species, such as NO, NOH, NO2, N2O, and reaction products of the NO reduction reaction with CO and H2 over supported Rh-based catalysts in the form of catalyst extrudates. By correlating surface intermediates and reaction products, new insights in the reaction mechanism could be obtained. Upon applying different reaction conditions (i. e., H2 or CO), the selectivity of the catalytic reaction could be tuned towards the formation of N2. Furthermore, in the absence of Rh, no reaction products were detected. The importance of the operando SHINERS as a surface-sensitive characterization technique in the field of heterogeneous catalysis provides routes towards a better understanding of catalytic performance.",

keywords = "NO reduction, operando spectroscopy, Raman Spectroscopy, rhodium, SHINERS",

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note = "Funding Information: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. We acknowledge Utrecht University (UU) and Nienke Visser (UU) for performing the TEM-EDX measurements. Funding Information: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. We acknowledge Utrecht University (UU) and Nienke Visser (UU) for performing the TEM‐EDX measurements. Publisher Copyright: {\textcopyright} 2021 The Authors. ChemPhysChem published by Wiley-VCH GmbH.",

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Operando Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of the NO Reduction Reaction over Rhodium-Based Catalysts

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