The widespread application of S doping in Fe-N-C materials aims to enhance the catalytic activity for oxygen reduction reactions (ORR). However, the current doping strategies are primarily centered on the first coordination layer encompassing Fe atoms. Consequently, this study employs first-principles calculations to compute the formation and binding energies of FeN doped with S atom. It further delves into the influence of diverse doping sites on catalyst stability and meticulously analyzes the configurations and corresponding ORR activities of four catalysts, namely FeNS-N (Number=0∼3), utilizing a constant-potential implicit solvent model to simulate authentic electrocatalytic environments. The findings reveal that under vacuum conditions, FeNS1 exhibits the utmost ORR activity, boasting a potential of 0.53 V. Conversely, within the constant-potential implicit solvation model, FeNS2 emerges as the catalyst with the highest ORR activity, achieving a potential of 0.39 V. Therefore, calculations leveraging the constant-potential solvation model offer more realistic insights into catalyst design, thereby guiding the development of superior catalysts.

中文翻译：

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在恒电位溶剂化模型中探索 S 掺杂 Fe-NC 材料对 ORR 机制的影响

S掺杂在Fe-NC材料中的广泛应用旨在增强氧还原反应（ORR）的催化活性。然而，当前的掺杂策略主要集中在包含 Fe 原子的第一配位层。因此，本研究采用第一性原理计算来计算掺杂 S 原子的 FeN 的形成能和结合能。进一步深入研究了不同掺杂位点对催化剂稳定性的影响，并仔细分析了四种催化剂FeNS-N（Number=0∼3）的构型和相应的ORR活性，利用恒电位隐式溶剂模型模拟真实的电催化环境。研究结果表明，在真空条件下，FeNS1 表现出最大的 ORR 活性，电位达到 0.53 V。相反，在恒电位隐式溶剂化模型中，FeNS2 成为具有最高 ORR 活性的催化剂，电位达到 0.39 V因此，利用恒电位溶剂化模型的计算为催化剂设计提供了更现实的见解，从而指导优质催化剂的开发。