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.