Engineered carbon supported single iron atom sites and iron clusters from Fe-rich Enteromorpha for Fenton-like reactions via nonradical pathways

Enteromorpha-derived Fe-N-C exhibits a high activity and stability in the heterogeneous activation of peroxymonosulfate (PMS) via nonradical oxidations including high-valence iron-oxo species and an electron-transfer pathway. [Display omitted] •The intrinsic Fe in Enteromorpha was transformed into a...

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Bibliographic Details
Published in:	Applied catalysis. B, Environmental Vol. 287; p. 119963
Main Authors:	Peng, Lijng, Duan, Xiaoguang, Shang, Yanan, Gao, Baoyu, Xu, Xing
Format:	Journal Article
Language:	English
Published:	Elsevier B.V 15-06-2021
Subjects:	Enteromorpha High-Valence iron Nonradical oxidation Peroxymonosulfate Single atom sites Enteromorpha Single atom sites High-Valence iron Nonradical oxidation Peroxymonosulfate
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Summary:	Enteromorpha-derived Fe-N-C exhibits a high activity and stability in the heterogeneous activation of peroxymonosulfate (PMS) via nonradical oxidations including high-valence iron-oxo species and an electron-transfer pathway. [Display omitted] •The intrinsic Fe in Enteromorpha was transformed into atomically dispersed Fe sites.•High PMS catalytic activity of the Enteromorpha-derived Fe-N-C was obtained.•High-valent iron-oxo species and electron transfer dominated the oxidations.•The single Fe atoms acted as the dominant species of Fe to form FeIV=O and FeV=O. Enteromorpha as a seawater pollutant was innovatively converted into a functional carbocatalyst to driven Fenton-like reactions.After direct pyrolysis of Enteromorpha at 900 °C without additional chemicals, a large number of Fe clusters and single Fe sites are anchored onto N-doped carbon matrixes (Enteromorpha-derived Fe-N-C) with a high Fe loading of 0.84 wt.%. The Enteromorpha-derived Fe-N-C exhibits a high activity in the heterogeneous activation of peroxymonosulfate (PMS) for organic pollutant degradation. Radical quenching experiments and electrochemical analysis tests verify the nonradical oxidation by high-valence iron-oxo species and an electron-transfer pathway. The single Fe atoms, which only accounted for the minority of the Fe species in Fe-N-C, acted as the dominated reactive sites for the formation of highly oxidizing FeIV=O and FeV=O sites. This work unveils the evolution of bio-Fe in Enteromorpha during thermal pyrolysis and the role of the derived Fe-N-C in PMS activation and organic degradation.
ISSN:	0926-3373 1873-3883
DOI:	10.1016/j.apcatb.2021.119963