Tailoring peroxyacetic acid (PAA) activation by sewage sludge derived atomic-Fe clusters/Fe-N4 catalyst via thermally driven spin manipulation

文献类型： 外文期刊

第一作者： Gu, Lin

作者： Gu, Lin;Cao, Xiao;Yang, Haiyan;He, Yiyang;Wang, Xin;Wen, Haifeng;Xu, Suyun;Hu, Ke;Zhang, Hanlin;Gu, Lin;Yuan, Haiping

作者机构：

关键词： Sewage sludge; Fe single-atom catalyst; Fe nanoclusters; Peracetic acid activation; Singlet oxygen

期刊名称：JOURNAL OF COLLOID AND INTERFACE SCIENCE （ 影响因子：9.7； 五年影响因子：8.9 ）

ISSN： 0021-9797

年卷期： 2025 年 686 卷

页码：

收录情况： SCI

摘要： Fe nanoclusters/FeN4 units embedded in graphitized carbon derived from biomass are highly efficient catalysts. However, simple physical mixing of precursors during pyrolysis tends to cause Fe to agglomerate into large nanoparticles. In this study, we introduce a novel peroxyacetic acid (PAA) conditioning strategy to transform sewage sludge (SS) into an enhanced Fe single-atom catalyst. This strategy modulates the evolution of Fe active sites by promoting the formation of adjacent Fe atomic clusters through thermal treatment. During sludge conditioning, PAA/Fe2+ triggers the dissolution and breakdown of SS, exposing nitrogen (N) and oxygen (O) atoms that bind with iron, thereby creating Fe immobilization sites. Characterization results show that conditioning promotes the formation of highly dispersed, few-atom Fe clusters/Fe-N4 sites (FeN4-FeNCP@SBC) at elevated temperatures, with Fe content exceeding 2.34 %. In contrast, untreated samples easily form Fe nano- particles. The FeN4-FeNCP@SBC can be used as superior Fenton-like catalyst in PAA-triggered antibiotic degradation. Singlet oxygen (1O2) plays a dominant role in degradation, as demonstrated by scavenging and ESR analysis. O2 and HO center dot are identified as important intermediates in the generation of 1O2 and are recognized as key species in FeN4-FeNCP@SBC-initiated PAA activation. The atomic-Fe cluster induced shift of the Fe center from low-spin (t2g 6 eg0) to medium-spin (t2g 5 eg1) facilitates partial occupation of the dz2 orbital, forming a sigma* bond with center dot OH. This promotes H being lost from OH to form O, and subsequent direct desorption of O can generate 1O2. The study provides a method to create SS catalysts with single atoms and Fe clusters for PAA and antibiotic degradation.

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