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Methanol-to-Olefins Studied by UV Raman Spectroscopy as Compared to Visible Wavelength: Capitalization on Resonance Enhancement.
Campbell, Emma; Sazanovich, Igor V; Towrie, Michael; Watson, Michael J; Lezcano-Gonzalez, Ines; Beale, Andrew M.
Affiliation
  • Campbell E; Cardiff Catalysis Institute School of Chemistry, Cardiff University, Cardiff CF10 3AT, U.K.
  • Sazanovich IV; Research Complex at Harwell (RCaH), Harwell, Didcot, Oxfordshire OX11 0FA, U.K.
  • Towrie M; Central Laser Facility, Research Complex at Harwell, Rutherford Appleton Laboratories, Harwell Campus, Didcot OX11 0QX, U.K.
  • Watson MJ; Central Laser Facility, Research Complex at Harwell, Rutherford Appleton Laboratories, Harwell Campus, Didcot OX11 0QX, U.K.
  • Lezcano-Gonzalez I; Johnson Matthey Technology Centre, P O Box 1, Belasis Avenue, Billingham TS23 1LB, U.K.
  • Beale AM; Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
J Phys Chem Lett ; 15(26): 6826-6834, 2024 Jul 04.
Article in En | MEDLINE | ID: mdl-38916593
ABSTRACT
Resonance Raman spectroscopy can provide insights into complex reaction mechanisms by selectively enhancing the signals of specific molecular species. In this work, we demonstrate that, by changing the excitation wavelength, Raman bands of different intermediates in the methanol-to-hydrocarbons reactions can be identified. We show in particular how UV excitation enhances signals from short-chain olefins and cyclopentadienyl cations during the induction period, while visible excitation better detects later-stage aromatics. However, visible excitation is prone to fluorescence that can obscure Raman signals, and hence, we show how fast fluorescence rejection techniques like Kerr gating are necessary for extracting useful information from visible excitation measurements.