Uniformed core-shell FeSe2+x@C nanocube superlattices for Fenton-like reaction: Coordinative roles of cation and anion

Simultaneously adjusting the coordination environment of Fenton-like catalysts and engineering their architectures is a viable strategy to promote catalytic reaction. Herein, two-dimensional (2D) porous core-shell FeSe2+x @C nanocube superlattices (NCSLs) with unsaturated selenium are for the first time prepared via one-step selenization of Fe3O4@C NCSLs and tested for peroxymonosulfate (PMS)-based Fenton-like reaction. The 2D porous superlattice structure can preferably expand Fe sites exposure and accelerate the large-scale transport and utilization of nanocrystals. The unsaturated selenium can optimize the electronic state of cationic Fe, not only promoting the Fe3+/Fe2+ cycle, regulating PMS adsorption, and improving the charge density, but also accelerating interfacial electron transport of the catalyst to lower the energy barrier of PMS decomposition to yield SO4•−. This work demonstrates a new application of nanocrystal superlattices and provides more insights to active components of catalyst design for enhancing catalytic activity via structural control and coordination engineering in various application scenarios. [Display omitted] •2D core-shell FeSe2+x@C nanocube superlattices was designed for PMS activation.•Unique NCSLs structure leads to risen active sites, mass diffusion, and stability.•The coordinative roles of cation/anion of FeSe2+x@C-3 NCSLs were well elucidated.•FeSe2+x@C-3 NCSLs/PMS system shows high activity in organic pollutant degradation.