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Open Access Photoelectron Photoion Coincidence Spectroscopy to Unveil Reaction Mechanisms by Isomer-selective Detection of Elusive Molecules: From Combustion to Catalysis

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This article is Open Access under the terms of the Creative Commons CC BY-NC-ND licence.

Elusive and reactive intermediates, such as radicals, play a central role in reaction mechanisms. Photoelectron photoion coincidence spectroscopy with tunable vacuum ultraviolet synchrotron radiation offers a multiplexed, sensitive, mass- and isomer-selective way to identify and, in some cases, determine mole fractions of reactive species. It thus helps to unveil the missing link(s) between reactants and products. After a brief overview of the technique, we review two systems in three different reactive environments. First, the unimolecular decomposition mechanism of ortho-xylyl radicals is revealed in pyrolysis experiments. Second, the insights gained are used to analyze a fuel-rich meta-xylene flame, which suggests that important xylyl isomerization reactions are currently missing in combustion models. Third, photoion mass-selected threshold photoelectron spectra identify the fulvenone ketene as the crucial intermediate in the catalytic fast pyrolysis of a lignin model compound and help map heterogeneous catalysis mechanisms.

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Keywords: PHOTOELECTRON SPECTROSCOPY; PYROLYSIS; REACTION MECHANISM; REACTIVE INTERMEDIATES; VACUUM ULTRAVIOLET SYNCHROTRON RADIATION

Document Type: Research Article

Affiliations: 1: Laboratory for Femtochemistry and Synchrotron Radiation, Paul Scherrer Institute, CH-5232 Villigen, Switzerland. [email protected] 2: Laboratory for Femtochemistry and Synchrotron Radiation, Paul Scherrer Institute, CH-5232 Villigen, Switzerland

Publication date: April 1, 2018

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  • International Journal for Chemistry and Official Membership Journal of the Swiss Chemical Society (SCS) and its Divisions

    CHIMIA, a scientific journal for chemistry in the broadest sense, is published 10 times a year and covers the interests of a wide and diverse readership. Contributions from all fields of chemistry and related areas are considered for publication in the form of Review Articles and Notes. A characteristic feature of CHIMIA are the thematic issues, each devoted to an area of great current significance.

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