Hollow-Structured N-doped carbon-embedded CoFe NanoAlloy for boosting activation of Monopersulfate: Engineered interface and heteroatom Doping-Induced enhancements

Abstract

While transition metals are useful for activating monopersulfate (MPS) to degrade contaminants, bimetallic alloys exhibit stronger catalytic activities owing to several favorable effects. Therefore, even though Co is an efficient metal for MPS activation, CoFe alloys are even more promising heterogeneous catalysts for MPS activation. Immobilization/embedment of CoFe alloy nanoparticles (NPs) onto hetero-atom-doped carbon matrices appears as a practical strategy for evenly dispersing CoFe NPs and enhancing catalytic activities via interfacial synergies between CoFe and carbon. Herein, N-doped carbon-embedded CoFe alloy (NCCF) is fabricated here to exhibit a unique hollow-engineered nanostructure and the composition of CoFe alloy by using Co-ZIF as a precursor after the facile etching and Fe doping. The Fe dopant embeds CoFe alloy NPs into the hollow-structured N-doped carbon substrate, enabling NCCF to possess the higher mesoscale porosity, active N species as well as more superior electrochemical properties than its analogue without Fe dopants, carbon matrix-supported cobalt (NCCo). Thus, NCCF exhibits a considerably larger activity than NCCo and the benchmark catalyst, Co3O4 NP, for MPS activation to degrade an environmental hormone, dihydroxydiphenyl ketone (DHPK). Besides, NCCF + MPS shows an even lower activation energy for DHPK degradation than literatures, and retains its high efficiency for eliminating DHPK in different water media. DHPK degradation pathway and ecotoxicity assessment are unraveled based on the insights from the computational chemistry, demonstrating that DHPK degradation by NCCF + MPS did not result in the formation of toxic and highly toxic by-products. These features make NCCF a promising heterogeneous catalyst for MPS activation to degrade DHPK.