Graphene/Hexagonal Boron Nitride Heterostructures for O2 Activation and CO Oxidation: Metal-Free Catalysts by Design

J Phys Chem Lett. 2024 Jan 25;15(3):785-793. doi: 10.1021/acs.jpclett.3c03383. Epub 2024 Jan 17.

Abstract

Pristine graphene and h-BN monolayers are chemically inert to oxygen and thus exhibit very limited catalytic activity toward O2 activation. Herein, we show that graphene/h-BN heterostructures exhibit a surprising O2 activation capability. We theoretically designed ten graphene/h-BN heterostructures with three types of interfaces and investigated their catalytic activities toward O2 activation and CO-oxidation. In general, O2 can be molecularly chemisorbed and activated on electron-rich graphene/h-BN heterostructures. Electron-deficient graphene/h-BN heterostructures can lead to dissociative O2 adsorption with relatively low dissociation energy barriers (<0.4 eV). For CO-oxidation, the computed energy barrier can be as low as 0.67 eV. The high catalytic activities toward O2 stem from either electron-deficient heterostructures' accumulated electrons or electron richness and low work function for the electron-rich heterostructures. Although the catalytic activities of graphene/h-BN heterostructures depend strongly on the interface type, they are insensitive to the patterns of BN-substitutes, hence benefiting applicability of a wide range of heterostructures.