One of the most challenging topics in catalysis today is the development of efficient catalytic processes for the direct conversion of methane. The co-presence of platinum or palladium along with copper enhances the yield of methanol than monometallic copper-zeolites, which findings motivate us to further investigate more possibilities to tune the structural-electronic properties of the active sites by doping with other transition metals and analyze their reactivity toward methane oxidation. In this work, by using the periodic DFT method to study a series of dual-metal binuclear Cu-oxo active sites in ZSM-5, we will be able to explore the effect of doping 3-5d metal on catalytic properties, the scaling relations of the reactivity and stability with different energetic, geometry, electronic descriptors, and screening the target dual-metal binuclear Cu-oxo active sites. We further explain why ΔEa (the methane activation barrier) for the homolytic C-H bond cleavage in methane correlates well with ΔEH (the hydrogen affinity) using bond strength and the main factor affecting ΔEH. As a whole, we expect that the structure-activity relationships developed will accelerate computational screening and provide a set of promising catalyst design criteria that can directly activate methane under moderate conditions.

Descriptor-based design of dual-metal binuclear Cu-oxo active sites in ZSM-5 zeolite for methane activation

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