Work function-regulated two-dimensional porous C 7 N 6 -based single-atom catalysts for hydrogen evolution reaction

Abstract

Due to the high cost of Pt catalyst, developing low-cost and high-efficiency electrocatalysts for hydrogen evolution reaction has become a key challenge for hydrogen energy industrialization. Here, a novel monoatomic catalytic system is constructed by using a C 7 N 6 monolayer with natural pore size as a carrier and anchoring transition metal atoms through the unsaturated triangular coordination configuration of nitrogen atoms around the pore. The calculation results show that Rh, Mn, Fe, W, Ta, and Ti embedded C 7 N 6 have excellent HER activity, and their ∆G H* are -0.04, -0.08, 0.08, -0.04, -0.06 and 0.08 eV, respectively, which are significantly better than commercial Pt/C catalysts.More importantly, through the systematic analysis of 20 transition metal systems, the linear correlation between the work function (Φ) of the carrier surface and ∆G H* was revealed. This discovery provides a theoretical framework for the construction of catalytic materials with adjustable electronic structure, and has important guiding significance for the efficient design and screening of low-cost supported electrocatalysts.