Binary Rhodium Atom Catalyst for Selective Catalytic Conversion of Methane to Methanol.

Using monometallic catalysts to selectively catalyze methane to methanol while suppressing the formation of liquid-phase overoxide products is beneficial for industrial applications. However, the balance between yield and selectivity over monometallic active sites remains challenging. This work proposes a strategy anchoring binary rhodium species to influence their surface dispersion properties. Binary Rh species are located both on the inert SBA-15 support surface and in the defect sites, resulting in a sizable methanol yield of 4360 μmol·gcat-1·h-1 and excellent liquid phase selectivity of ∼99%. It has been demonstrated that the reaction mechanism is closely associated with the adsorption state of reaction intermediates on the catalyst surface. The formation of Rh-O-Rh sites leads to significant charge transfer, making the adsorption strength of CO more favorable for generating the key Rh-O active sites. Further exploration shows that the Rh/SBA-15 catalyst facilitates the activation of methane at the Rh-O sites to form *CH3OH adsorbate species, promoting its desorption when CO is coadsorbed.