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The optimized Fenton-like activity of Fe single-atom sites by Fe atomic clusters–mediated electronic configuration modulation

Authors :
Fan Mo
Chunlin Song
Qixing Zhou
Wendan Xue
Shaohu Ouyang
Qi Wang
Zelin Hou
Shuting Wang
Jianling Wang
Source :
Proceedings of the National Academy of Sciences. 120
Publication Year :
2023
Publisher :
Proceedings of the National Academy of Sciences, 2023.

Abstract

The performance optimization of isolated atomically dispersed metal active sites is critical but challenging. Here, TiO 2 @Fe species-N-C catalysts with Fe atomic clusters (ACs) and satellite Fe-N 4 active sites were fabricated to initiate peroxymonosulfate (PMS) oxidation reaction. The AC-induced charge redistribution of single atoms (SAs) was verified, thus strengthening the interaction between SAs and PMS. In detail, the incorporation of ACs optimized the HSO 5 - oxidation and SO 5 ·− desorption steps, accelerating the reaction progress. As a result, the Vis/TiFeAS/PMS system rapidly eliminated 90.81% of 45 mg/L tetracycline (TC) in 10 min. The reaction process characterization suggested that PMS as an electron donor would transfer electron to Fe species in TiFeAS, generating 1 O 2 . Subsequently, the h VB + can induce the generation of electron-deficient Fe species, promoting the reaction circulation. This work provides a strategy to construct catalysts with multiple atom assembly–enabled composite active sites for high-efficiency PMS-based advanced oxidation processes (AOPs).

Subjects

Subjects :
Multidisciplinary

Details

ISSN :
10916490 and 00278424
Volume :
120
Database :
OpenAIRE
Journal :
Proceedings of the National Academy of Sciences
Accession number :
edsair.doi...........26f63544e435588887ddb19785682828