Targeted synthesis of covalently linked Ni-MOFs nanosheets/graphene for oxygen evolution reaction by computational screening of anchoring primers

Hybridization of Metal-Organic frameworks (MOFs) with conductive materials has proven to be an efficient way to enhance their oxygen evolution reaction (OER) performance. Here we present a novel primer-induced in situ hybridization method to covalently link the nickel-based two-dimensional (2D) ultrathin MOFs nanosheets and graphene. By considering the energetically favorable anchoring process, thermodynamically prohibited self-polymerization side reaction and high delocalization of lowest unoccupied molecular orbitals (LUMO), the optimal phenylenebisboronic acid (PBA) primer were rapidly identified by screening thousands of primers via a high-throughput periodic density functional theory (DFT) workflow. Aided by the computational results, the PBA molecules were used to be covalently bonded to graphene successfully and then induce the in-situ growth of ultrathin Ni-MOFs nanosheets with terephthalic acid (TPA) as the ligand (denoted as Ni-HMOF@GE-PBA). The as-prepared Ni-HMOF@GE-PBA was demonstrated as a high-performance electrocatalyst for OER, delivering a much lower onset potential than that of simple blending of graphene and Ni-MOFs nanosheets by 150 mV. This design and construction strategy would pave an efficient pathway to rapid exploration and synthesis of new 2D–2D hybrid catalytic materials with excellent performance for OER.