Operando Laboratory-based Multi-edge X-ray Absorption Near-Edge Spectroscopy of Solid Catalysts

Nina S Genz; Antti-Jussi Kallio; Ramon Oord; Frank Krumeich; Anuj Pokle; Øystein Prytz; Unni Olsbye; Florian Meirer; Simo Huotari; Bert Marc Weckhuysen

doi:10.1002/anie.202209334

Operando Laboratory-based Multi-edge X-ray Absorption Near-Edge Spectroscopy of Solid Catalysts

Nina S Genz, Antti-Jussi Kallio, Ramon Oord, Frank Krumeich, Anuj Pokle, Øystein Prytz, Unni Olsbye, Florian Meirer, Simo Huotari, Bert Marc Weckhuysen

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

Abstract

Laboratory-based X-ray absorption spectroscopy (XAS) and especially X-ray absorption near-edge structure (XANES) offers new opportunities in catalyst characterization and presents not only an alternative, but also a complementary approach to precious beamtime at synchrotron facilities. We successfully designed a laboratory-based setup for performing operando , quasi-simultaneous XANES analysis at multiple K edges, more specifically, operando XANES of mono-, bi-, and trimetallic CO 2 hydrogenation catalysts containing Ni, Fe, and Cu. Detailed operando XANES studies of the multi-element solid catalysts revealed metal-dependent differences in the reducibility and re-oxidation behavior and their influence on the catalytic performance in CO 2 hydrogenation. The applicability of operando laboratory-based XANES at multiple K edges paves the way for advanced multi-element catalyst characterization complementing detailed studies at synchrotron facilities.

Original language	English
Article number	e202209334
Pages (from-to)	1-8
Journal	Angewandte Chemie-International Edition
Volume	61
Issue number	48
Early online date	7 Oct 2022
DOIs	https://doi.org/10.1002/anie.202209334
Publication status	Published - 25 Nov 2022

Bibliographical note

Funding Information:
N.S.G. acknowledges the German Research Foundation (DFG) for funding (452243354). A.‐J.K. and S.H. were supported by the Academy of Finland (grant 295696) and A.‐J.K. additionally by the University of Helsinki Doctoral Programme for Materials Research and Nanoscience and the Jenny and Antti Wihuri foundation (00200134). We acknowledge the Helsinki Center for X‐ray Spectroscopy for providing experiment time and support with the HelXAS spectrometer (proposal 2020‐0005). The Research Council of Norway is acknowledged for support to the Norwegian Center for Transmission Electron Microscopy (NORTEM) national infrastructure (project number 197405). High‐resolution electron microscopy work was done at ScopeM (ETH Zurich), while general funding for this research work came from the Netherlands Research Council (NWO) in the form of a Gravitation Program “Multiscale Catalytic Energy Conversion” (MCEC).

Publisher Copyright:
© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Keywords

Alloys
CO Hydrogenation
Heterogeneous Catalysis
Multielement Catalysts
X-Ray Absorption Spectroscopy

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Angew Chem Int Ed - 2022 - Genz - Operando Laboratory‐Based Multi‐Edge X‐Ray Absorption Near‐Edge Spectroscopy of SolidFinal published version, 4.84 MBLicence: CC BY

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title = "Operando Laboratory-based Multi-edge X-ray Absorption Near-Edge Spectroscopy of Solid Catalysts",

abstract = "Laboratory-based X-ray absorption spectroscopy (XAS) and especially X-ray absorption near-edge structure (XANES) offers new opportunities in catalyst characterization and presents not only an alternative, but also a complementary approach to precious beamtime at synchrotron facilities. We successfully designed a laboratory-based setup for performing operando , quasi-simultaneous XANES analysis at multiple K edges, more specifically, operando XANES of mono-, bi-, and trimetallic CO 2 hydrogenation catalysts containing Ni, Fe, and Cu. Detailed operando XANES studies of the multi-element solid catalysts revealed metal-dependent differences in the reducibility and re-oxidation behavior and their influence on the catalytic performance in CO 2 hydrogenation. The applicability of operando laboratory-based XANES at multiple K edges paves the way for advanced multi-element catalyst characterization complementing detailed studies at synchrotron facilities.",

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note = "Funding Information: N.S.G. acknowledges the German Research Foundation (DFG) for funding (452243354). A.‐J.K. and S.H. were supported by the Academy of Finland (grant 295696) and A.‐J.K. additionally by the University of Helsinki Doctoral Programme for Materials Research and Nanoscience and the Jenny and Antti Wihuri foundation (00200134). We acknowledge the Helsinki Center for X‐ray Spectroscopy for providing experiment time and support with the HelXAS spectrometer (proposal 2020‐0005). The Research Council of Norway is acknowledged for support to the Norwegian Center for Transmission Electron Microscopy (NORTEM) national infrastructure (project number 197405). High‐resolution electron microscopy work was done at ScopeM (ETH Zurich), while general funding for this research work came from the Netherlands Research Council (NWO) in the form of a Gravitation Program “Multiscale Catalytic Energy Conversion” (MCEC). Publisher Copyright: {\textcopyright} 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

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AU - Genz, Nina S

AU - Kallio, Antti-Jussi

AU - Oord, Ramon

AU - Krumeich, Frank

AU - Pokle, Anuj

AU - Prytz, Øystein

AU - Olsbye, Unni

AU - Meirer, Florian

AU - Huotari, Simo

AU - Weckhuysen, Bert Marc

N1 - Funding Information: N.S.G. acknowledges the German Research Foundation (DFG) for funding (452243354). A.‐J.K. and S.H. were supported by the Academy of Finland (grant 295696) and A.‐J.K. additionally by the University of Helsinki Doctoral Programme for Materials Research and Nanoscience and the Jenny and Antti Wihuri foundation (00200134). We acknowledge the Helsinki Center for X‐ray Spectroscopy for providing experiment time and support with the HelXAS spectrometer (proposal 2020‐0005). The Research Council of Norway is acknowledged for support to the Norwegian Center for Transmission Electron Microscopy (NORTEM) national infrastructure (project number 197405). High‐resolution electron microscopy work was done at ScopeM (ETH Zurich), while general funding for this research work came from the Netherlands Research Council (NWO) in the form of a Gravitation Program “Multiscale Catalytic Energy Conversion” (MCEC). Publisher Copyright: © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

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N2 - Laboratory-based X-ray absorption spectroscopy (XAS) and especially X-ray absorption near-edge structure (XANES) offers new opportunities in catalyst characterization and presents not only an alternative, but also a complementary approach to precious beamtime at synchrotron facilities. We successfully designed a laboratory-based setup for performing operando , quasi-simultaneous XANES analysis at multiple K edges, more specifically, operando XANES of mono-, bi-, and trimetallic CO 2 hydrogenation catalysts containing Ni, Fe, and Cu. Detailed operando XANES studies of the multi-element solid catalysts revealed metal-dependent differences in the reducibility and re-oxidation behavior and their influence on the catalytic performance in CO 2 hydrogenation. The applicability of operando laboratory-based XANES at multiple K edges paves the way for advanced multi-element catalyst characterization complementing detailed studies at synchrotron facilities.

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Operando Laboratory-based Multi-edge X-ray Absorption Near-Edge Spectroscopy of Solid Catalysts

Abstract

Bibliographical note

Keywords

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