Reasonable design and synthesis of Fe/N/C-based catalysts is one of the most promising way for developing precious metal-free oxygen reduction reaction (ORR) catalysts in acidic mediums. Herein, we developed a highly active metal–organic framework-derived S-doped Fe/N/C catalyst [S-Fe/Z8/2-aminothiazole (2-AT)] prepared by thermal treatment. The S-Fe/Z8/2-AT catalyst with uniform S-doping possesses a three-dimensional macro–meso–micro hierarchically porous structure. Moreover, the chemical composition and structural features have been well-optimized and characterized for such S-Fe/Z8/2-AT catalysts; and their formation mechanism was also revealed. Significantly, applying the optimal S-Fe/Z8/2-AT catalysts into electrocatalytic test exhibits remarkable ORR catalytic activity with a half-wave potential of 0.82 V (vs reversible hydrogen electrode) and a mass activity of 18.3 A g^–1 at 0.8 V in 0.1 M H₂SO₄ solution; the polymer electrolyte membrane fuel cell test also confirmed their excellent catalytic activity, which gives a maximal power density as high as 800 mW cm^–2 at 1 bar. A series of designed experiments disclosed that the favorable structural merits and desirable chemical compositions of S-Fe/Z8/2-AT catalysts are critical factors for efficient electrocatalytic performance. The work provides a new approach to open an avenue for accurately controlling the composition and structure of Fe/N/C catalysts with highly activity for ORR.

中文翻译：

---

具有多层孔隙率的S掺杂Fe / N / C三维网络，可有效减少聚合物电解质膜燃料电池中的氧气

合理设计和合成Fe / N / C基催化剂是在酸性介质中开发无贵金属无氧还原反应（ORR）催化剂的最有前途的方法之一。在这里，我们开发了通过热处理制备的高活性金属-有机骨架衍生的S掺杂的Fe / N / C催化剂[S-Fe / Z8 / 2-氨基噻唑（2-AT）]。具有均匀S掺杂的S-Fe / Z8 / 2-AT催化剂具有三维宏观-中观-微观层次结构的多孔结构。而且，对于这种S-Fe / Z8 / 2-AT催化剂，化学组成和结构特征已经被充分优化和表征。并揭示了它们的形成机理。重要的是，将最佳的S-Fe / Z8 / 2-AT催化剂应用于电催化测试显示出显着的ORR催化活性，其半波电势为0。在0.1 MH ₂ SO ₄溶液中，在0.8 V时为^–1；聚合物电解质膜燃料电池测试还证实了其出色的催化活性，在1 bar压力下的最大功率密度高达800 mW cm ^–2。一系列设计实验表明，S-Fe / Z8 / 2-AT催化剂的良好结构优点和理想的化学组成是有效电催化性能的关键因素。这项工作提供了一种新方法，为精确控制对ORR具有高活性的Fe / N / C催化剂的组成和结构开辟了一条途径。