Water Radiocatalysis for Selective Aqueous-Phase Methane Carboxylation with Carbon Dioxide into Acetic Acid at Room Temperature.

Methane (CH 4 ) carboxylation with carbon dioxide (CO 2 ) into acetic acid (CH 3 COOH) is an ideal chemical reaction to utilize both greenhouse gases with 100% atom efficiency but remains a great challenge under mild conditions. Herein, we introduce a concept of water (H 2 O) radiocatalysis for efficient and selective aqueous-phase CH 4 carboxylation with CO 2 into CH 3 COOH at room temperature. H 2 O radiolysis occurs under γ-ray radiation to produce ·OH radicals and hydrated electrons that efficiently react with CH 4 and CO 2 , respectively, to produce ·CH 3 radicals and ·CO 2 - species facilely coupling to produce CH 3 COOH. CH 3 COOH selectivity as high as 96.9 and 96.6% calculated respectively from CH 4 and CO 2 and a CH 3 COOH production rate of as high as 121.9 μmol·h -1 are acquired. The water radiocatalysis driven by γ-rays is also applicable to selectively produce organic acids from other hydrocarbons and CO 2 .