Design of Boron Doped C(2)N-C(3)N Coplanar Conjugated Heterostructure for Efficient HER Electrocatalysis

Hydrogen evolution reaction (HER) via the electrocatalytic reduction of water on metal-free catalysts may become a promising method for a sustainable energy supply in the future. However, compared with noble metals or transition metals, the carbon-based metal-free electrocatalysts show poor activity. Here, a novel coplanar metal-free catalyst (C(2)N-C(3)N) was designed for the first time to achieve better efficiency for electron transfer and water reduction. Through the DFT calculations, we discovered that the unique coplanar C(2)N-C(3)N structure can promote the directional transfer of electrons from C(3)N to C(2)N under the drive of built-in electric potential in the π-conjugated plane. To achieve higher performance in HER, the single atom doping by the substitution of boron is carried out. Remarkably, after the boron is doped, the barrier in the Tafel step decreases from 2.35 eV to 0.86 eV. Our results indicate that the novel B-doped coplanar C(2)N-C(3)N structure is a promising metal-free catalyst for HER.