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Soft X-ray Heterogeneous Radiolysis of Pyridine in the Presence of Hydrated Strontium-Hydroxyhectorite and its Monitoring by Near-Ambient Pressure Photoelectron Spectroscopy
Sorbonne Univ, CNRS UMR 7614, Lab Chim Phys Matiere & Rayonnement, 4 Pl Jussieu, F-75252 Paris 05, France..
Sorbonne Univ, CNRS UMR 7614, Lab Chim Phys Matiere & Rayonnement, 4 Pl Jussieu, F-75252 Paris 05, France.;Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France..ORCID iD: 0000-0001-9316-559X
Sorbonne Univ, CNRS UMR 7614, Lab Chim Phys Matiere & Rayonnement, 4 Pl Jussieu, F-75252 Paris 05, France..
Sorbonne Univ, CNRS UMR 7614, Lab Chim Phys Matiere & Rayonnement, 4 Pl Jussieu, F-75252 Paris 05, France.;Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France..
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2018 (English)In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 8, article id 6164Article in journal (Refereed) Published
Abstract [en]

The heterogeneous radiolysis of organic molecules in clays is a matter of considerable interest in astrochemistry and environmental sciences. However, little is known about the effects of highly ionizing soft X-rays. By combining monochromatized synchrotron source irradiation with in situ Near Ambient Pressure X-ray Photoelectron Spectroscopy (in the mbar range), and using the synoptic view encompassing both the gas and condensed phases, we found the water and pyridine pressure conditions under which pyridine is decomposed in the presence of synthetic Sr2+-hydroxyhectorite. The formation of a pyridine/water/Sr2+ complex, detected from the Sr 3d and N 1s core-level binding energies, likely presents a favorable situation for the radiolytic breaking of the O-H bond of water molecules adsorbed in the clay and the subsequent decomposition of the molecule. However, decomposition stops when the pyridine pressure exceeds a critical value. This observation can be related to a change in the nature of the active radical species with the pyridine loading. This highlights the fact that the destruction of the molecule is not entirely determined by the properties of the host material, but also by the inserted organic species. The physical and chemical causes of the present observations are discussed.

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NATURE PUBLISHING GROUP , 2018. Vol. 8, article id 6164
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Inorganic Chemistry
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URN: urn:nbn:se:kth:diva-227221DOI: 10.1038/s41598-018-24329-8ISI: 000430280600016PubMedID: 29670155Scopus ID: 2-s2.0-85045725505OAI: oai:DiVA.org:kth-227221DiVA, id: diva2:1209003
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QC 20180521

Available from: 2018-05-21 Created: 2018-05-21 Last updated: 2018-05-21Bibliographically approved

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