4.7 Article

The p and d hybridization interaction in Fe-N-C boosts peroxymonosulfate non-radical activation

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DOI: 10.1016/j.seppur.2020.118025

关键词

Non-free radicals; Peroxymonosulfate; Fe-N-C; p and d Hybridization; Bisphenol A

资金

  1. Central goverment guidance for local science and technology development projects for Hubei province [ZYYD2020000027, 2019ZYYD068]
  2. Guangdong Provincial Natural Science Foundation [2016A030306033]

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This research enhanced metalloid properties and electronic activity by incorporating Fe into g-C3N4 (CN) to form an Fe-N-C electronic bond bridge. Experimental results showed that the FeCN/PMS system effectively removed BPA in an electronic circuit of PMS/catalyst/water or pollutants.
Advanced oxidation processes based on non-radicals are used to remove pollutants and have attracted attention due to their adaptability to complex water environments. In this work, we dope Fe to g-C3N4 (CN) to form an Fe-N-C electronic bond bridge. Characterization and density functional theory (DFT) calculations prove that the p and d orbital hybridization of FeCN improves metalloid properties and improves electronic activity. Due to the difference of electronegativity, the local polarization electric field of C-N-Fe on the electronic bond bridge is formed. An electronic circuit of PMS/catalyst/water or pollutants is formed, which promotes the electron transfer in the process of non-radical reactions. The reaction kinetic results showed that the degradation rate constant of bisphenol A (BPA) increased by 54 times. The normalization treatment and poisoning experiment proved the catalytic active sites of Fe. Similarly, the FeCN/PMS system can satisfactorily remove BPA in a wide pH range (3-9), in the presence of inorganic anions and natural water matrix. This work provides a method for improving the process of non-radical electron transfer and provides strong technical support for stimulating the practical application of persulfate.

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