Methane Carboxylation Using Electrochemically Activated Carbon Dioxide
Yucheng Yuan, Yuhan Zhang, Haoyi Li, Muchun Fei, Hongna Zhang, John Santoro, Dunwei Wang
Abstract
Abstract Direct synthesis of CH 3 COOH from CH 4 and CO 2 is an appealing approach for the utilization of two potent greenhouse gases that are notoriously difficult to activate. In this Communication , we report an integrated route to enable this reaction. Recognizing the thermodynamic stability of CO 2 , our strategy sought to first activate CO 2 to produce CO (through electrochemical CO 2 reduction) and O 2 (through water oxidation), followed by oxidative CH 4 carbonylation catalyzed by Rh single atom catalysts supported on zeolite. The net result was CH 4 carboxylation with 100 % atom economy. CH 3 COOH was obtained at a high selectivity (>80 %) and good yield ( ca . 3.2 mmol g −1 cat in 3 h). Isotope labelling experiments confirmed that CH 3 COOH is produced through the coupling of CH 4 and CO 2 . This work represents the first successful integration of CO/O 2 production with oxidative carbonylation reaction. The result is expected to inspire more carboxylation reactions utilizing preactivated CO 2 that take advantage of both products from the reduction and oxidation processes, thus achieving high atom efficiency in the synthesis.