Aunano-Fe1 tandem catalysis for promoted methane conversion to acetic acid by O2 oxidation

Tuning metal size from nanoscale to uniform single atoms holds the potential to promote the oxygenates selectivity for direct methane conversion, but suffers from low kinetics when utilizing O 2 as oxidant. Herein, we report a Au nano -Fe 1 -ZSM-5 catalyst for enhanced acetic acid production from CH 4 , CO, and O 2 in aqueous solution. The Au nano nanoparticles enable upgrading of O 2 into active hydroxyl radicals (•OH) via net reaction between O 2 , H 2 O and CO. The Fe 1 single atoms within 5-nm range from Au nano could be converted into active Fe 1 IV -O by •OH oxidation, which catalyzes rapid H-abstraction from CH 4 and subsequent C-C coupling with CO for acetic acid production. Such closely adjacent but separate active centers, i.e., Au nano and Fe 1 for decoupled O 2 and CH 4 activation, respectively, enable a high reactivity of 982 mmol/g metal /h for methane conversion with O 2 oxidant while retaining a high acetic acid selectivity of 81 % at 150 °C.