Advanced oxidation processes based on high-valent metal species have attracted much attention due to their high reactivity and selectivity in degrading refractory organic pollutants, but the preparation of such catalysts remains a great challenge. Herein, FeCoCu-nitrogen-doped carbon (FeCoCu-NC), a trimetallic catalyst capable of producing high-valent metal species, was synthesized by direct carbonization of core–shell Metal-organic frameworks (MOFs). The rationally designed catalyst exhibited high catalytic activity in wide pH range and high resistance to common radical scavengers, anions and natural organics. The incorporation of Cu in FeCoCu-NC (TNC_X) not only enhanced the catalytic activity but also changed the activation mechanism of peroxymonosulfate (PMS) from a radical pathway to a non-radical pathway dominated by high-valent metal species. In addition, the TNC₅/PMS system showed higher trichlorophenol (TCP) removal efficiency and PMS utilization compared to the radical-dominated FeCo-NC/PMS system and the ¹O₂-dominated CoCu-NC/PMS system. This study provides a facile strategy to the preparation of advanced catalysts from multi-metal MOFs and is expected to provide guidance for the design of heterogeneous high-valent metal catalysts.

基于高价金属物种的高级氧化工艺因其在降解难降解有机污染物方面的高反应性和选择性而备受关注，但此类催化剂的制备仍然是一个巨大的挑战。在此，FeCoCu-氮掺杂碳（FeCoCu-NC）是一种能够产生高价金属物种的三金属催化剂，通过核壳金属有机框架（MOF）的直接碳化合成。合理设计的催化剂在宽pH范围内表现出高催化活性，对常见的自由基清除剂、阴离子和天然有机物具有高抵抗力。在 FeCoCu-NC (TNC _X)不仅提高了催化活性，而且将过氧单硫酸盐(PMS)的活化机制从自由基途径转变为以高价金属物种为主的非自由基途径。此外，与自由基主导的FeCo-NC/PMS系统和¹ O ₂主导的CoCu-NC/PMS系统相比，TNC _{5 /PMS系统显示出更高的三氯苯酚(TCP)去除效率和PMS利用率。}该研究为多金属MOFs制备先进催化剂提供了一种简便的策略，有望为多相高价金属催化剂的设计提供指导。