An effective descriptor for identifying the electrocatalytic activity and selectivity of bilayer carbon-based heterojunction catalysts

The usage of composite carbon-based materials supported by graphene has emerged as a powerful selection for designing electrocatalytic electrodes due to their agile electronic transmission and diversiform redox active sites. Here, we constructed fresh electroactive organic catalysts for hydrogen carrier synthesis by stacking a series of organic molecules on transition metal azide doped graphene substrates, in anticipation of these bilayer heterostructures to breathe new life into electrocatalysis. As expected, several promising cathodic catalysts were speculated through first principles calculations, such as Co-PMDT for H2 generation and Co-PQ for ammonia (NH3) synthesis. However, facing such an intricate interface engineering and electronic structure regulation undoubtedly poses a challenge to the time-consuming computational screening work. To tackle this, an effective descriptor was proposed as a predictive tool for identifying the activity and selectivity toward diverse chemical reactions, which allows us to systematically fine-tune the catalysts' properties in order to enhance their electrocatalytic performance. Our work may offer feasible approaches for the rational design of advanced electrocatalysts.