The development of highly-efficient electrocatalysts with bifunctional catalytic activity for oxygen reduction reaction (ORR) and oxygen evolution reaction.

(OER) still remains a great challenge for the large-scale application of renewable energy conversion and storage technologies. Herein, by means of comprehensive density functional theory (DFT) computations, we systematically explored the potential of pyrrolic-N doped graphene (pyrrolic-N₄-G) supported various transition metal atoms (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Mo, Ru, Pd, W, Os, Ir, and Pt) as electrocatalysts for the ORR and OER. Our results revealed that these TM/pyrrolic-N₄-G candidates exhibit high electrochemical stability due to their positive dissolution potentials. Especially, the Ir/pyrrolic-N₄-G can perform as a promising bifunctional electrocatalyst for both ORR and OER with the low overpotentials (η^ORR = 0.34 V and η^OER = 0.32 V). Interestingly, multiple-level descriptors, including energy descriptor (ΔG_OH* - ΔG_O*), (ΔG_OH*), structure descriptor ($\phi$), and d-band center (ε) can well rationalize the origin of the high catalytic activity of Ir/pyrrolic-N₄-G for the ORR/OER. Our findings not only further enrich the SACs, but also open a new avenue to develop novel 2D materials-based SACs for highly efficient oxygen electrocatalysts.

开发对氧还原反应（ORR）和析氧反应具有双功能催化活性的高效电催化剂。

（OER）对于可再生能源转换和存储技术的大规模应用仍然是一个巨大的挑战。在此，通过综合密度泛函理论 (DFT) 计算，我们系统地探索了吡咯-N 掺杂石墨烯 (pyrrolic-N ₄ -G) 支持各种过渡金属原子 (TM = Sc, Ti, V, Cr, Mn 、Fe、Co、Ni、Cu、Mo、Ru、Pd、W、Os、Ir 和 Pt）作为 ORR 和 OER 的电催化剂。我们的结果表明，这些 TM/吡咯-N ₄ -G 候选物由于其正溶解电位而表现出高电化学稳定性。特别是，Ir/吡咯-N ₄ -G 可以作为一种有前途的双功能电催化剂用于 ORR 和 OER，具有低过电位（η ^ORR = 0.34 V 和 η ^OER  = 0.32 V）。有趣的是，多级描述符，包括能量描述符（Δ G _OH* - Δ G _O*）、（Δ G _OH*）、结构描述符（$\phi$) 和 d 带中心 (ε) 可以很好地解释 Ir/吡咯-N ₄ -G 对 ORR/OER的高催化活性的起源。我们的发现不仅进一步丰富了 SAC，而且为开发用于高效氧电催化剂的新型二维材料 SAC 开辟了新途径。