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Operando X-ray Spectroscopy

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Operando X-ray Spectroscopy

The Operando X-ray Spectroscopy belongs to the Bioenergy and Catalysis Laboratory (LBK) of the Energy and Environment Division (ENE) of PSI and is within a matrix organization responsible for the operation of the SuperXAS beamline to LSF.

Scientific Highlights

2 décembre 2020
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Key activity descriptors of nickel-iron oxygen evolution electrocatalysts in the presence of alkali metal cations

Ni-Fe oxyhydroxide is among the most active oxygen evolution electrocatalysts. Electrolyte alkali metal cations modify the activity and reaction intermediates, however, the exact mechanism is at question due to unexplained deviations from the cation size trend. Our X-ray absorption spectroelectrochemical results show that the OER activity follows the variations in .electrolyte pH rather than a specific cation. Our DFT-based reactivity descriptors confirm the conclusions of an indirect pH effect.

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31 août 2020
Smolentsev_2020

The structure of active sites of CoMo/Al2O3 catalysts determined by RIXS spectroscopy.

A fundamental understanding of the active sites in technical CoMo/ Al2O3 catalysts is crucial to improve the production of clean transportation fuels by hydrodesulfurization (HDS), which removes sulfur from fossil fuels. Sulfur dioxide, resulting from fossil fuel combustion, is one of the main causes for acid rain. In situ X-ray spectroscopic experiments at the SuperXAS beamline of the SLS provided insight in the structure and number of active sites (“Co−Mo−S”) in sulfided CoMo/ Al2O3 catalysts. When the Co to Mo ratio is less than 0.1, cobalt forms isolated sites on the MoS2 phase, where the cobalt promoter atoms are in centrosymmetric octahedral coordination with six-sulfur ligands.

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1 mai 2020
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Taking a snapshot of the triplet excited state of an OLED organometallic luminophore using X-rays

In this work, the complementarity of pump-probe experiments at SwissFEL (ALVRA endstation) and at synchrotrons (SuperXAS beamline of SLS and ID09 of ESRF) is used to investigate the triplet excited state of Cu OLED materials. Details about the charge transfer and structural rearrangements in the excited state of this material are revealed and obtained data can be used to verify computational methods for rational development of new OLED materials.

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25 mars 2020
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Elucidating the Oxygen Activation Mechanism on Ceria-Supported Copper-Oxo Species Using Time-Resolved X-ray Absorption Spectroscopy

We monitored the dynamic structure of the active sites in a catalyst containing highly dispersed copper-oxo species on ceria during low-temperature CO oxidation using time-resolved X-ray absorption spectroscopy. We quantitatively demonstrate that the CO oxidation mechanism below 90 °C involves an oxygen intermediate strongly bound to the active sites as well as the redox activity of Cu2+/Cu+ and Ce4+/Ce3+ couples.

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28 février 2020
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Elucidating the mechanism of heterogeneous Wacker oxidation over Pd-Cu/zeolite Y by transient XAS

Unlike the homogeneous Wacker process, the understanding of the mechanism of the heterogeneous system has long remained to be superficial. Here the authors investigated the mechanism of heterogeneous Wacker oxidation over Pd-Cu/zeolite Y through transient XAS coupled with kinetic studies and chemometric analysis.

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25 février 2020
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Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites

Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry. This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0.

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28 janvier 2019
wells 2019

Structural selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy

The link between Pd nanoparticle structure and surface reactivity for NH3 abatement was found using operando X-ray absorption fine structure spectroscopy, diffuse reflectance infrared Fourier-transformed spectroscopy and on-line mass spectrometry.

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14 janvier 2019
Ebner_2019_highlight

Fe-Based O2-Reduction Catalysts Synthesized Using Na2CO3 as a Pore-Inducing Agent

This work presents a new approach for synthesizing Fe-based oxygen reduction reaction (ORR) catalysts using sodium carbonate (Na2CO3) as an inexpensive but effective pore-inducing agent offering microporosity control.

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1 août 2018
Filez 2018 Angew.jpg

Kinetics of Lifetime Changes in Bimetallic Nanocatalysts Revealed by Quick X‐ray Absorption Spectroscopy

The different reaction steps involved in repeated Pt13In9 segregation‐alloying are identified by XAS and kinetically characterized at the single‐cycle level.

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Dr. Maarten Nachtegaal
Paul Scherrer Institut
5232 Villigen-PSI
Switzerland
Telephone: +41 56 310 3056
E-mail: maarten.nachtegaal@psi.ch

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Laboratory for Synchrotron Radiation and Femtochemistry

Swiss Light Source SLS

Synchrotron light large research facility.

SwissFEL

The new X-ray free electron laser facility.

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