Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H₂O₂ production

Despite the growing demand for hydrogen peroxide it is almost exclusively manufactured by the energy-intensive anthraquinone process. Alternatively, H₂O₂ can be produced electrochemically via the two-electron oxygen reduction reaction, although the performance of the state-of-the-art electrocatalysts is insufficient to meet the demands for industrialization. Interestingly, guided by first-principles calculations, we found that the catalytic properties of the Co–N₄ moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic properties of metalloenzymes. Using this principle, we designed and synthesized a single-atom electrocatalyst that comprises an optimized Co–N₄ moiety incorporated in nitrogen-doped graphene for H₂O₂ production and exhibits a kinetic current density of 2.8 mA cm⁻² (at 0.65 V versus the reversible hydrogen electrode) and a mass activity of 155 A g⁻¹ (at 0.65 V versus the reversible hydrogen electrode) with negligible activity loss over 110 hours.