An iron single-atom catalyst, composed of robust FeN₄ moieties anchored on a nitrogen-doped porous carbon matrix (Fe-SAC/NC), has been developed via a surfactant-coordinated metal-organic framework (MOF) approach for application in heterogeneous electro-Fenton (HEF) process. The cohesive interaction between the surfactant and MOF precursor enabled the formation of abundant and stable FeN₄ moieties. The Fe-SAC/NC-catalyzed HEF allowed the complete degradation of 2,4-dichlorophenol with low iron leaching (1.2 mg L^-1), being superior to nanoparticle catalyst synthesized without surfactant. The experiments and density functional theory (DFT) calculations demonstrated the dominant role of single-atom FeN₄ sites to activate the electrogenerated H₂O₂ yielding ^•OH. The dense FeN₄ moieties allowed harnessing the modulated electronic structure of the SAC to facilitate the electron transfer, whereas the adjacent pyrrolic N enhanced the adsorption of target organic pollutants. Moreover, the excellent catalysis, recyclability and viability of the Fe-SAC/NC were verified by successfully treating several organic pollutants even in urban wastewater.

已通过表面活性剂配位金属有机骨架 (MOF) 方法开发了一种铁单原子催化剂，由锚定在氮掺杂多孔碳基质 (Fe-SAC/NC) 上的坚固的 FeN ₄部分组成，用于非均相应用电芬顿 (HEF) 工艺。表面活性剂和 MOF 前体之间的内聚相互作用能够形成丰富且稳定的 FeN ₄部分。^{Fe-SAC/NC催化的HEF能够以低铁浸出（1.2 mg L -1} ）完全降解2,4-二氯苯酚，优于没有表面活性剂合成的纳米颗粒催化剂。实验和密度泛函理论 (DFT) 计算证明了单原子 FeN _{4的主导作用}位点激活电生成的 H ₂ O ₂产生^• OH。密集的 FeN ₄部分允许利用 SAC 的调制电子结构来促进电子转移，而相邻的吡咯 N 增强了目标有机污染物的吸附。此外，通过成功处理城市废水中的几种有机污染物，验证了 Fe-SAC/NC 的优异催化性、可回收性和可行性。