Fe Single-Atom Catalyst for Cost-Effective yet Highly Efficient Heterogeneous Fenton Catalysis

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Abstract

High energy consumption in pyrolyzing precursors for catalyst preparation would limit the application of nitrogen-doped carbon-based single-atom catalysts in actual pollutant remediation. Herein, we report an Fe single atom (7.67 wt %) loaded polyaniline catalyst (Fe-PANI) prepared via a simple impregnation process without pyrolysis. Both experimental characterizations and density functional theory calculations demonstrated that isolated −N═ group sites can fasten Fe atoms through Fe–N coordination in PANI, leading to a high stability of Fe atoms in a heterogeneous Fenton reaction. Highly dispersive yet dense −N═ groups in PANI can be protonated to be adsorption sites, which largely reduce the migration distance between reactive radicals and organics. More significantly, frontier molecular orbitals and spin-density distributions reveal that electrons can transfer from reduction groups of PANI to an Fe(III) site to accelerate its reduction. As a result, a remarkably boosted degradation behavior of organics under near-neutral conditions (pH 6), with low H2O2 concentration, was achieved. This cost-effective Fe-PANI catalyst with high catalytic activity, stability, and adsorption performance has great potential for industrial-level wastewater treatment.

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