H₂O₂ production by electroreduction of oxygen is an attractive alternative to replace the current complex anthraquinone method. However, it is still challenging to realize efficient electrochemical H₂O₂ production in acid by using cost-effective catalysts. Herein, we report a pyrimidine-assisted chemical-vapor-deposition method to synthesize sulfur-and-nitrogen-codoped few-layered graphene (SNGL) with exceptional activity and selectivity for two-electron oxygen reduction reaction (2e⁻ ORR) in acidic electrolyte (pH = 1). The H₂O₂ selectivity reaches 90%–100% over a potential range of 0.20–0.55 V, and the maximum H₂O₂ production rate (4.8 mol g⁻¹·h⁻¹) exceeds all of the reported H₂O₂ production performance for carbon-material-based catalysts. Experiments and density functional theory (DFT) simulations reveal that the synergy effect of the combined oxidized sulfur and pyridinic N functional motif can lower the Fermi level of valence electronic states of active edge carbon sites and thus leads to suitable binding strength of ∗OOH intermediate for high selectivity and performance 2e⁻ ORR for H₂O₂ formation.

通过氧气的电还原生产H ₂ O ₂是替代当前复杂的蒽醌方法的有吸引力的替代方法。然而，通过使用具有成本效益的催化剂在酸中实现高效的电化学 H ₂ O ₂生产仍然具有挑战性。在此，我们报告了一种嘧啶辅助化学气相沉积法合成硫和氮共掺杂的少层石墨烯 (SNGL)，该方法对酸性电解质中的双电子氧还原反应 (2e ^- ORR) 具有出色的活性和选择性(pH = 1)。在0.20~0.55 V的电位范围内， H ₂ O ₂选择性达到90%~100%，最大H ₂ O ₂产率（4.8 mol g ^-1 ·h ^-1）超过了所有报道的碳材料基催化剂的H ₂ O _{2生产性能。}实验和密度泛函理论 (DFT) 模拟表明，结合的氧化硫和吡啶 N 功能基序的协同效应可以降低活性边缘碳位点的价电子态的费米能级，从而导致 ∗OOH 中间体的合适结合强度H ₂ O ₂形成的高选择性和性能 2e ^- ORR 。