Hierarchical porous-enhanced peroxymonosulfate activation via 3D ordered macro-microporous Fe-NC: Role of high-valent iron-oxo species and electron-transfer mechanism

Developing improved eco-friendly catalysts possessing high activity and simultaneously exhibiting adequate stability remains a bottleneck to date. By the means of introducing Fe along with constructing architecture, the novel 3D ordered macro-microporous Fe-NC catalyst (3DOM Fe-NC) was designed, which make the improve-ment on both activity and durability of carbonaceous catalysts become a reality. The introduction of Fe induces transformation of the active centers from carbonaceous framework to the formed FeNx sites, as well as alters PMS activation pathways, resulting in high-performance nonradical oxidation processes controlled by electro-n-transfer mechanism and high-valent iron-oxo species. Remarkably, owing to the alteration of active center, pollution adsorption on the carbonaceous frameworks is avoided that allows the 3DOM Fe-NC to prolong durability. Moreover, benefiting from the unique hierarchical architecture, the 3DOM Fe-NC/PMS system achieves superior activity and adaptability to the pollutants with different sizes. This work hopes to provide a new design concept for high-performance catalysts toward sustainable environmental remediation.