Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 310, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121327
Keywords
Enzyme-mimicking,Single-atom catalysis; Photo-Fenton-like reaction; Synergistic effects; Antibiotics
Funding
- Independent Designing Scientific Research Project of Zhejiang Normal University [2020ZS0302]
- Key R&D Project of Zhejiang Province [2021C03163]
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In this study, bio-inspired single-atom Fe sites with pyrrole-type FeN4 coordinations were successfully incorporated into graphitic carbon nitride, resulting in improved photo-Fenton-like reaction performance. The study revealed that the pyrrole-type FeN4 sites were more conducive to charge distribution and exhibited higher intrinsic activity and stability than the pyridine-type FeN4 sites. This work provides important guidance for the rational design of robust bio-inspired single-atom catalysts for environmental remediation.
In this study, bio-inspired single-atom Fe (bio-SA-Fe) sites with pyrrole-type FeN4 coordinations were embedded in graphitic carbon nitride (g-C3N4) via facile copolymerization approach. The bio-SA-Fe/g-C3N4 outperforms pure g-C3N4 and Fe-doped g-C3N4 (pyridine-type FeN4 sites) in photo-Fenton-like reaction with a broad operating pH range (3-9), low consumption of H2O2, and remarkable stability and durability. Bader charge and differential charge distribution reveals the pyrrole-type FeN4 sites are more conducive to charge distribution than the pyridine-type FeN4 sites in g-C3N4, enabling faster electron transfer between the conjugated bio-SA-Fe sites and the g-C3N4 substrate. Density functional theory calculations further verified that the bio-SA-Fe sites are more stable and possess higher intrinsic activity for heterogeneous Fenton reaction than the pyridine-type FeN4 sites in g-C3N4. This work provides important guidance for the rational design of robust bio-inspired single-atom catalysts for environmetal remediation and wide implications for other aqueous redox reactions.
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