Intermediate stabilization for tuning photocatalytic selective oxidation of CH4 to CH3OH over Co3O4/ZnO

Artificial photocatalysis provides a promising approach for CH4 selective conversion into CH3OH under mild reaction conditions. However, the over-oxidization by the active oxygen radical species impedes for the high efficiency of photocatalytic conversion of CH4 to CH3OH. Here, we proposed a strategy of the transfer of key intermediates .CH3 from host photocatalyst surface for stability to improve CH4 conversion to CH3OH products. A Co3O4/ZnO composited photocatalyst was designed to efficiently convert CH4 to CH3OH with a rate of 366 lmol g-1h-1 under simulated sunlight irradiation, while the parent ZnO only completely overoxidized CH4 into CO2. We uncovered that Co(3)O(4 )played a new role as the active site for the adsorption of .CH3 key intermediates and the desorption of CH3OH to suppress CH4 overoxidation on ZnO surface. This work highlights cocatalyst for .CH3 intermediate stabilization to control the pathway of photocatalytic selective oxidation of CH4 into CH3OH . (C) 2022 Elsevier Inc. All rights reserved.

Automated summary

Artificial photocatalysis is a promising method for selective conversion of CH4 to CH3OH, but the over-oxidization by active oxygen radicals hinders its efficiency. In this study, a strategy of transferring key intermediates for stability was proposed. A Co3O4/ZnO composite photocatalyst effectively converted CH4 to CH3OH under simulated sunlight irradiation, while pure ZnO only over-oxidized CH4 into CO2. Co(3)O(4) was found to play a crucial role in adsorbing .CH3 key intermediates and desorbing CH3OH to suppress CH4 over-oxidation on the ZnO surface.