The optimized Fenton-like activity of Fe single-atom sites by Fe atomic clusters-mediated electronic configuration modulation.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37011202.
- Also identified by DOI 10.1073/pnas.2300281120 and PMC identifier 10104488.
- Licence recorded as CC BY-NC-ND.
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Abstract
The performance optimization of isolated atomically dispersed metal active sites is critical but challenging. Here, TiO<sub>2</sub>@Fe species-N-C catalysts with Fe atomic clusters (ACs) and satellite Fe-N<sub>4</sub> 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<sub>5</sub><sup>-</sup> oxidation and SO<sub>5</sub><sup>·- </sup>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 <sup>1</sup>O<sub>2</sub>. Subsequently, the h<sub>VB</sub><sup>+</sup> 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).