Well-dispersed iron and nitrogen co-doped hollow carbon microsphere anchoring by g-C3N4 for efficient peroxymonosulfate activation

Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C3N4 catalyst (HFeNC-g-C3N4) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C3N4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N-x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C3N4 catalyst with single-atom Fe-N-x active sites, verified by XRD, XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe2+ catalyst. The mechanism of O-2(center dot-) dominated radical combined with nonradical O-1(2) pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C3N4/PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.

Automated summary

This study developed a novel cascade anchoring strategy to synthesize a catalyst with single-atom Fe and N co-doping, exhibiting efficient Fenton-like activity for PMS activation in wastewater treatment. Characterization by XRD, XPS, and HAADF-STEM confirmed the presence of single-atom Fe-N-x active sites, achieving a significantly higher turnover frequency compared to homogeneous catalysts. The mechanism of O-2(center dot-) dominated radical combined with nonradical O-1(2) pathway was proposed, contributing to the improved pH adaptability and interference immunity of the catalyst/PMS system.