Carbon Matrix with Atomic Dispersion of Binary Cobalt/Iron-N Sites as Efficient Peroxymonosulfate Activator for Organic Pollutant Oxidation.

ZHANG, Bofan, LI, Xianquan, BINGHAM, Paul, AKIYAMA, Kazuhiko and KUBUKI, Shiro (2023). Carbon Matrix with Atomic Dispersion of Binary Cobalt/Iron-N Sites as Efficient Peroxymonosulfate Activator for Organic Pollutant Oxidation. Chemical Engineering Journal, 451 (Part 2): 138574.

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Official URL: https://www.sciencedirect.com/science/article/pii/...
Open Access URL: https://www.sciencedirect.com/science/article/pii/... (Published version)
Link to published version:: https://doi.org/10.1016/j.cej.2022.138574
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    Abstract

    Monometallic single atom catalysts have exhibited excellent catalytic capacity due to their unique structural features. However, it remains challenging to promote the limited number of active sites and realize high-efficiency and stability during Fenton-like catalysis. Herein, a nitrogenized graphitic carbon matrix containing Fe-Co dual single atoms (FeCoNC) manifested enhanced catalytic capacity in persulfate activation for tetracycline hydrochloride (TC) oxidation. Nonradical singlet oxygen (1O2) was identified as dominant reactive species in both FeCoNC and CoNC systems, while the formation pathways of 1O2 and TC catalysis processes were distinct different. 57Fe Mössbauer spectroscopy and theoretical calculations revealed that the dynamic electronic structure and covalency of Fe-N/Co-N bond configuration after coordinating with a second neighboring metal atom induced promoted electron transfer and tuned reactive species transformation pathways. Benefiting from the optimized N3-Fe-Co-N3 structure and synergistic effect of dual metal sites, the FeCoNC catalyst was endowed with lowered reaction barriers, adaptability and excellent stability, demonstrating promising practical application potential. This work unveiled the intrinsically regulated mechanism of dual single metal sites towards refractory organic oxidation and delivered enhanced understanding of covalency and electronic configuration on PMS-AOPs based catalysis processes.

    Item Type: Article
    Uncontrolled Keywords: Chemical Engineering; 0904 Chemical Engineering; 0905 Civil Engineering; 0907 Environmental Engineering
    Identification Number: https://doi.org/10.1016/j.cej.2022.138574
    SWORD Depositor: Symplectic Elements
    Depositing User: Symplectic Elements
    Date Deposited: 09 Aug 2022 10:38
    Last Modified: 22 Aug 2022 16:15
    URI: http://shura.shu.ac.uk/id/eprint/30568

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