Work function-regulated two-dimensional porous C7N6-based single-atom catalysts for the hydrogen evolution reaction

Abstract

Due to the high cost of Pt catalysts, designing low-cost and high-efficiency electrocatalysts for the hydrogen evolution reaction (HER) has become a key challenge in the development of renewable energy technology. Here, a novel single-atom catalyst (SAC) is constructed by using a C₇N₆ monolayer as a substrate, which anchors transition metal (TM) atoms through the unsaturated nitrogen atoms around the pore. The catalytic performance of 20 TM centers is evaluated, revealing that partial d-orbital occupancy enables near-thermoneutral values. More importantly, a linear correlation between the work function (Φ) of the support surface and is revealed. This discovery provides a theoretical framework for the construction of catalytic materials with a tunable electronic structure and offers important guiding significance for the efficient design and screening of low-cost supported electrocatalysts.