Diatomic Active Sites Embedded Graphyne as Electrocatalysts for Ammonia Synthesis.

Ammonia (NH) is a vital chemical compound in industry and agriculture, and the electrochemical nitrogen reduction reaction (eNRR) is considered a promising approach for NH synthesis. However, the development of eNRR faces the challenge of high overpotential and low Faradaic efficiency. In this work, graphyne (GY) is anchored by 3d, 4d, and 5d dual transition metal atoms to form diatomic catalysts (DACs) and is roundly investigated as an electrocatalyst for eNRR via density functional theory calculations.

Two-Dimensional Single-Atom Catalyst TM(HAB) Monolayers for Electrocatalytic Dinitrogen Reduction Using Hierarchical High-Throughput Screening.

As an environmentally friendly and sustainable strategy to produce ammonia, the electrocatalytic nitrogen reduction reaction (eNRR) is facing the challenge of low conversion rates and high overpotential, to solve which efficient catalysts are urgently needed. Here, a new class of two-dimensional metal-organic layers (MOLs) TM(HAB) (TM = 30 transition metals; HAB = hexaaminobenzene) were evaluated a three-step high-throughput screening combined with the spin-polarized density functional theory (DFT) method to obtain eligible TM(HAB) catalysts embedded with transition metal atoms from 3d to 5d. Our investigation revealed that Nb(HAB), Mo(HAB), and Tc(HAB) are eligible NRR candidates, among which Tc(HAB) possesses the best catalytic performance with a lowest onset potential of -0.