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Reaction cell for in situ soft x-ray absorption spectroscopy and resonant inelastic x-ray scattering measurements of heterogeneous catalysis up to 1 atm and 250 °C
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
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2013 (English)In: Review of Scientific Instruments, ISSN 0034-6748, E-ISSN 1089-7623, Vol. 84, no 11, 113107- p.Article in journal (Refereed) Published
Abstract [en]

We present a novel in situ reaction cell for heterogeneous catalysis monitored in situ by x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS). The reaction can be carried out at a total pressure up to 1 atm, a regime that has not been accessible to comparable in situ techniques and thus closes the pressure gap to many industrial standard conditions. Two alternate catalyst geometries were tested: A) a thin film evaporated directly onto a x-ray transparent membrane with a flowing reaction gas mixture behind it or B) a powder placed behind both the membrane and a gap of flowing reaction gas mixture. To illustrate the working principle and feasibility of our reaction cell setup we have chosen ethylene epoxidation over a silver catalyst as a test case. The evolution of incorporated oxygen species was monitored by total electron/fluorescence yield O K-XAS as well as O K-RIXS, which is a powerful method to separate contributions from inequivalent sites. We find that our method can reliably detect transient species that exist during catalytic reaction conditions that are hardly accessible using other spectroscopic methods.

Place, publisher, year, edition, pages
2013. Vol. 84, no 11, 113107- p.
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:uu:diva-209192DOI: 10.1063/1.4829630ISI: 000329982000008OAI: oai:DiVA.org:uu-209192DiVA: diva2:656158
Available from: 2013-10-15 Created: 2013-10-15 Last updated: 2017-12-06Bibliographically approved
In thesis
1. In situ X-Ray Spectroscopy of Ethylene Epoxidation over Ag and studies of Li-ion batteries and Cu sulfidation
Open this publication in new window or tab >>In situ X-Ray Spectroscopy of Ethylene Epoxidation over Ag and studies of Li-ion batteries and Cu sulfidation
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is based on experiments applying synchrotron based X-ray Absorption Spectroscopy(XAS) and Resonant Inelastic X-ray Scattering (RIXS) in the soft X-ray region to energy related systems. The main work of this thesis has been to develop a reaction cell that allowed for in situ XAS and RIXS investigations of the partial epoxidation of ethylene over a Ag catalyst at 1 atm and up to 250C. The developed in situ cell can be used in two sample modes: 1) the Ag catalyst is deposited directly onto the vacuum separating membrane with the reaction gases flowing beneath it or 2) a slightly compressed Ag powder sample is at a distance to the vacuum membrane with the reaction gases flowing between the Ag powder sample and the membrane.Both sample modes offers the total florescence yield, TFY, and the total electron yield, TEY, to be recorded simultaneously. By means of the developed in situ cell a number of oxygen species, residing in/on the Ag surface or in the Ag bulk, have been detected. We claim to detect adsorbed O2 under epoxidation conditions, as well as Ag–O–H groups. We are also able to monitor changes of the absorbed oxygen as we change the composition of the reaction gas feed. The first charging cycle of Li-ion batteries have been investigate by ex situ measurements on the cathode Li2-xMnSiO4 and the anode composite LixNi0:5TiOPO4/C . The initial crystalline material becomes amorphous due to lithiation during the first first charging. We find that the redox behaviors of these two states are significantly different. Sulfidation of natural copper oxides are is found to be strongly promoted when it is grown on the host metal by a disproportionation.

Place, publisher, year, edition, pages
Uppsala: Arkitektkopia, Uppsala, 2013. 64 p.
Keyword
In situ, XAS, RIXS, heterogeneous catalysis
National Category
Atom and Molecular Physics and Optics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-209204 (URN)
Public defence
2013-11-05, Å2005, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
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Available from: 2013-10-15 Created: 2013-10-15 Last updated: 2013-10-16

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Kristiansen, PawDuda, LaurentC

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