A Simple Descriptor toward Optimizing Electrocatalytic N₂ Oxidation to HNO₃ Performance over Graphene-Based Single-Atom Catalysts

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2742 - 2751

Published: March 7, 2025

Single-atom catalysts (SACs) exhibit tremendous advantages in the electrochemical N2 oxidation reaction (EN2OR) to HNO3, which is an eco-friendly alternative synthesis of conventional industrial nitric acid and nitrates, but methods rationally design rapidly screen high-efficiency EN2OR SACs are unclear. Herein, taking pyridinic nitrogen-doped graphene-supported as example, a simple descriptor has been proposed evaluate performance through systematically constructing surface phase diagram. This comprised merely geometric information inherent atomic properties (occupied d electron number, electronegativity, coordinate number) that can accurately predict activity selectivity EN2OR, independent DFT simulations. Based on this descriptor, high-throughput screening executed partially N/C/O coordinated SACs, including 160 candidates; 13 candidates with overpotential less than 1.0 V selected then validated by calculations mean absolute error (MAE) low 0.09 V, indicating reliability descriptor. Meanwhile, screened CoO2N2-G RhO2N2-G lower 0.64 0.68 more negative UL(EN2OR) - UL(OER) values -0.34 -0.44 comparison other candidates, respectively, demonstrating excellent EN2OR. work offers route rapid discovery high-performance for

Language: Английский

Enhancing photocatalyst stability for hydrogen peroxide synthesis through promoting oxygen-centered organic radical formation

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 31, 2025

Language: Английский