Designing graphene as a new frustrated Lewis pair catalyst for hydrogen activation by co-doping.

Boron and nitrogen co-doped bilayer graphene (BN-G) and graphene ribbon (BN-GR) as Frustrated Lewis Pair (FLP) catalysts are investigated for hydrogen molecule activation. The nitrogen and boron atoms are separated as they are in different layers of BN-G/GR. Calculations show that this novel FLP catalyst is capable of activating hydrogen molecules. From the Bader charge, Mayer bond order, and the geometrical structures, it can be seen that the hydrogen molecules undergo heterolytic scission and have a late product-like transition state. More interestingly, the active sites are identified as being the carbon atoms around dopants for BN-G. The BN-G/GR catalysts deliver performances comparable to that of the reported FLP catalyst when considering their barrier and reaction energy values. The current work demonstrates the great potential of doped carbon catalysts as FLP catalysts and paves the way to nanostructured carbon catalyst applications in reactions by directly utilizing hydrogen molecules.