Rationally designing efficient, low-cost and stable catalysts toward the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR) is of significant importance to the development of renewable energy technologies. In this work, we have systematically investigated a series of potentially efficient and stable single late transition metal atom doped phthalocyanines (TM@Pcs, TM = Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ir and Pt) as single-atom catalysts (SACs) for applications toward the OER and ORR through a computational screening approach. Our calculations indicate that TM atoms can tightly bind with Pc monolayers with high diffusion energy barriers to prevent the isolated atoms from clustering. The interaction strength between intermediates and TM@Pc governs the catalytic activities for the OER and ORR. Among all the considered TM@Pc catalysts, Ir@Pc and Rh@Pc were found to be efficient OER electrocatalysts with overpotentials η^OER of 0.41 and 0.44 V, respectively, and for the ORR, Rh@Pc exhibits the lowest overpotential η^ORR of 0.44 V followed by Ir@Pc (0.55 V), suggesting that Rh@Pc is an efficient bifunctional catalyst for both the OER and ORR. Moreover, it is worth noting that the Rh@Pc catalyst can remain stable against dissolution under the pH = 0 condition. Ab initio molecular dynamic calculations suggest that Rh@Pc could remain stable at 300 K. Our findings highlight a novel family of two-dimensional (2D) materials as efficient and stable SACs and offer a new strategy for catalyst design.

中文翻译：

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用于析氧和还原的过渡金属掺杂酞菁单分子层的计算筛选

合理设计高效、低成本、稳定的析氧反应（OER）和氧还原反应（ORR）催化剂对可再生能源技术的发展具有重要意义。在这项工作中，我们系统地研究了一系列潜在有效且稳定的单后过渡金属原子掺杂的酞菁（TM@Pcs，TM = Mn、Fe、Co、Ni、Cu、Ru、Rh、Pd、Ir 和 Pt）作为通过计算筛选方法应用于 OER 和 ORR 的单原子催化剂 (SAC)。我们的计算表明，TM 原子​​可以与具有高扩散能垒的 Pc 单层紧密结合，以防止孤立的原子聚集。中间体和 TM@Pc 之间的相互作用强度决定了 OER 和 ORR 的催化活性。η ^OER分别为 0.41 和 0.44 V，对于 ORR，Rh@Pc 表现出最低的过电势η ^ORR为 0.44 V，其次是 Ir@Pc (0.55 V)，这表明 Rh@Pc 是一种有效的双功能催化剂OER 和 ORR。此外，值得注意的是，Rh@Pc 催化剂在 pH = 0 条件下可以保持稳定的溶解。从头算分子动力学计算表明，Rh@Pc 可以在 300 K 时保持稳定。我们的研究结果强调了一种新型的二维 (2D) 材料家族作为高效且稳定的 SAC，并为催化剂设计提供了新的策略。