Mechanistic Insights into Light-Alkane Formation from Photoexcited Uranyl complexes
Year: 2026
Type: preprint
Abstract: This work describes a uranyl-catalysed photo-induced methodology for generating methane from acetic acid. The reaction proceeds in water as the only solvent, with roughly 10 vol % acetic acid — a composition mimicking ommercial vinegar — and only 1 mol % of UO 2 (NO 3 ) 2 , a by-product of the nuclear fuel cycle. The mechanism underlying this transformation was examined in detail through luminescence measurements, EPR spectroscopy, isotope-labelling experiments, and speciation studies. DFT calculations show that the process involves an unstable intermediate, U V O 2 + -AcOH template, which is prompt to disproportionation into inactive U IV and appears to be responsible for the low TON, which is reported. However, the speciation studies also suggest that the equatorial environment of UO 2 2+ would stabilize this UV intermediate and therefore influence the CH 4 production as well as decreasing the potential additional competitive paths, leading to greater selectivity.
Source: ChemRxiv
Language: English
Subfield: Inorganic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7213284527