Great increasing N content in Fe-embedded carbon nanotubes to effectively activate persulfate for radical and nonradical degradation of organic contaminants

SEPARATION AND PURIFICATION TECHNOLOGY(2024)

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Abstract
N atoms in carbonaceous catalysts are usually considered as the key active centers for catalytic/activated re -actions. However, the raise of N content in metal-carbonaceous composites is still a great challenge. In this work, the N content in Fe-embedded carbon nanotubes (Fe@CNTs) was greatly enriched via a Zn-N linkage process, giving Fe-embedded N-rich carbon nanotubes (Fe@NRCNTs). The N content of Fe@NRCNTs was up to 7.43 atom %, reaching the highest value among other Fe-embedded carbonaceous materials. Zn-N linkage could induce more active C sites in g-C3N4 intermediate for N-doping and inhibit the release of N-containing gases, resulting in N enrichment during the formation of Fe@NRCNTs. More importantly, the as-obtained Fe@NRCNTs exhibited excellent performance towards persulfate activation for tetracycline degradation, and its rate constant was four times higher than that of Fe@CNTs. The high N content provided more active site for nonradical activation, and also accelerated the electron transfer between Fe and CNTs, beneficial for radical activation. Furthermore, Fe@NRCNTs could work in a very wide pH range (2.2-10.3), accompanying with high adaptability and reus-ability. This work provided a feasible strategy to increase N content in metal-embedded carbonaceous materials for highly efficient radical and nonradical persulfate activation.
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Key words
Active site regulation,Persulfate activation,Fe-embedded carbon nanotubes,N enrichment,Zn -N linkage
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