Zeolite-catalyzed conversions of alkyl halides, produced via the halogen-mediated activation of alkanes under mild conditions, are attractive upgrading processes but suffer from rapid deactivation. Understanding hydrocarbon generation in these reactions, which resemble the widely studied conversion of methanol to hydrocarbons, requires advanced spectroscopic approaches to distinguish the complex mechanisms governing C–C bond formation, chain growth, and the deposition of carbonaceous species that severely limit catalyst productivity. This talk discusses recent achievements using operando photoelectron photoion coincidence (PEPICO) spectroscopy and electron paramagnetic resonance spectroscopy as complementary tools to map paths to hydrocarbon pool species and gain insight into their impact on deactivation processes. Comparing the transformations of methyl chloride and methanol sheds light on similarities and distinctions of the underlying processes. The operando PEPICO results offer direct experimental evidence of methyl radicals in both reactions and ketene formation in methanol-to-hydrocarbons. The potential of the presented methods to provide valuable mechanistic insights into complex reaction networks and current challenges will be discussed.

Tracking reactive intermediates in zeolite-catalyzed hydrocarbon transformations

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