Iron-based catalysts are promising for the catalytic oxidation of H₂S owing to their non-toxicity, abundance, and high conversion efficiency. However, their industrial applications are hampered by the low selectivity and poor durability. Herein, we reported a simple one-step pyrolysis approach to synthesize isolated Fe–Nχ sites confined in graphitic carbon nitride (Fe-CN-NHχ). The creation of isolated Fe–Nχ sites was evidenced by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray absorption spectroscopy (XAS), UV-vis-NIR diffuse reflectance spectroscopy (DRS), and X-ray photoelectron spectroscopy (XPS). The well dispersed Fe–Nχ sites offer additional active centers for the reaction, and such form of Fe presence effectively resists the deep oxidation of H₂S. As a result, the obtained Fe-CN-NH5 catalyst exhibited outstanding catalytic performance with high sulfur selectivity. Significantly, the Fe–Nχ sites are resistance to sulfur poisoning, leading to excellent durability in the reaction. No obvious decrease of catalytic activity was observed in a reaction period of 180 h, which is better than those of reported iron-based catalysts.

铁基催化剂有望用于H ₂的催化氧化由于其无毒，丰富和高转化效率。但是，它们的工业应用受到选择性低和耐久性差的困扰。在本文中，我们报道了一种简单的一步热解方法来合成局限在石墨氮化碳（Fe-CN-NHX）中的孤立Fe-Nχ位点。像差校正的高角度环形暗场扫描透射电子显微镜（HAADF-STEM），X射线吸收光谱（XAS），UV-vis-NIR漫反射光谱（DRS）证明了孤立的Fe–Nχ位点的产生。 ）和X射线光电子能谱（XPS）。良好分散的Fe–Nχ位点为反应提供了额外的活性中心，这种形式的Fe存在有效地抵抗了H ₂的深度氧化结果，获得的Fe-CN-NH5催化剂表现出优异的催化性能和高硫选择性。值得注意的是，Fe–Nχ位点具有抗硫中毒的能力，因此在反应中具有出色的耐久性。在180 h的反应时间内，没有观察到明显的催化活性下降，这优于已报道的铁基催化剂。