Mechanistic insights into catalytic conversion of methane under non-oxidative conditions
Methane is a chemical feedstock that can be directly converted into hydrocarbons and hydrogen, which are essential platforms for the production of chemicals, polymers, and liquid fuels. Using operando photoelectron photoion coincidence (iPEPICO) spectroscopy, the role of elusive C2+ radical intermediates participating in the complex gas-phase reaction network was unveiled. Different C2-C5 radical species allow for a stepwise growth of the hydrocarbon chains. Propargyl radicals are identified as essential for the formation of benzene, an important product but also the precursor of heavier hydrocarbon products via hydrogen abstraction - acetylene addition routes (HACA mechanism). We provide mechanistic insights of significant importance to improve the performance of methane conversion under non-oxidative conditions both from a chemical and engineering point of view as well as to serve as a basis to understand other relevant catalysts.
More information can be accessed online by clicking on the following links: paper in Angewandte Chemie International Editioncall_made and highlight of the VUV (x04db) beamline of the Swiss Light Source of the Paul Scherrer Institutecall_made.