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
作者： Gu, Lin 1 ; Cao, Xiao 1 ; Yang, Haiyan 1 ; He, Yiyang 1 ; Wang, Xin 1 ; Wen, Haifeng 1 ; Zhang, Hanlin 2 ; Xu, Suyun 1 ; Yuan, Haiping 3 ; Hu, Ke 1 ;
作者机构： 1.Univ Shanghai Sci & Technol, Sch Environm & Architecture, Shanghai 200093, Peoples R China
2.Shanghai Acad Agr Sci, Ecoenvironm Protect Inst, Shanghai 201403, Peoples R China
3.Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
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.
- 相关文献
作者其他论文 更多>>
-
Bacillus velezensis SS-20 as a potential and efficient multifunctional agent in biocontrol, saline-alkaline tolerance, and plant-growth promotion
作者：Chen, Zhaoliang;Zhang, Haiyun;Lv, Weiguang;Zhang, Siyi;Li, Shuangxi;Zhang, Hanlin;Zheng, Xianqing;Zhang, Juanqin;Bai, Naling;Du, Linna;Li, Shuangxi;Zhang, Hanlin;Zheng, Xianqing;Zhang, Juanqin;Bai, Naling;Li, Shuangxi;Zhang, Hanlin;Zheng, Xianqing;Zhang, Juanqin;Bai, Naling;Zhang, Tinglin
关键词：Bacillus velezensis; Antagonistic activity; Saline-alkaline tolerance; Growth promotion; Whole-genome sequencing
-
The synergistic role of sludge conditioner FeCl3/Rice husk on co-combustion with coal gangue: Thermaldynamic behavior, gases pollutants control and bottom ash stabilization
作者：Li, Jixin;He, Yiyang;Wang, Xin;Cao, Xiao;Yang, Haiyan;Chen, Lu;Xu, Suyun;Wen, Haifeng;Gu, Lin;Zhang, Hanlin
关键词：Coal gangue; Dewatered sludge; Co-combustion; TG-FTIR; Kinetics
-
Predicting the penetration behavior of colloidal foulants into membrane pore channels using A collision-attachment-based particle capture model
作者：Fu, Wei;Zhou, Yangfan;Liu, Bingzhi;Liu, Junxia;Guo, Hao;Huang, Weiwei;Yang, Haiyan;Tang, Chuyang Y.
关键词：Particle capture; Collision attachment; Energy barrier; Pore size; Membrane thickness
-
Nitrogen Fertilizer Reduction in Rice-Eel Co-Culture System Improves the Soil Microbial Diversity and Its Functional Stability
作者：Ma, Mengqian;Lv, Weiguang;Huang, Yu;Zhang, Juanqin;Li, Shuangxi;Bai, Naling;Zhang, Haiyun;Zhu, Xianpu;Xu, Chenglong;Zhang, Hanlin;Lv, Weiguang;Zhang, Juanqin;Li, Shuangxi;Bai, Naling;Zhang, Haiyun;Zhu, Xianpu;Xu, Chenglong;Zhang, Hanlin;Lv, Weiguang;Zhang, Juanqin;Li, Shuangxi;Bai, Naling;Zhang, Haiyun;Zhang, Hanlin;Zhu, Xianpu;Xu, Chenglong;Zhang, Hanlin
关键词：paddy soil; rice-eel co-culture system; soil bacterial community; earthworms
-
Thermal hydrolysis-induced molecular transformations in sludge: Implications for photochemical reactivity and dissolved antibiotics photodissipation
作者：Wen, Haifeng;Wang, Xin;Zhang, Xinchao;He, Yiyang;Gu, Lin;Zhang, Hanlin;Wu, Peize
关键词：Sludge thermal hydrolysis; Dissolved organic matter; Photodegradation; Reactive oxygen species; Electron transfer capacity
-
Stratified EPS from sewage sludge as a multifunctional modulator for FeCN photocatalyst: Interfacial engineering and enhanced norfloxacin degradation
作者：Cao, Xiao;Zhang, Xinchao;He, Yiyang;Xu, Suyun;Gu, Lin;Zhang, Hanlin;Yuan, Haiping
关键词：Photocatalysis; Antibiotic degradation; Extracellular polymeric substances (EPS); FeCN@SEPS; Norfloxacin
-
Efficient biodegradation of enrofloxacin by Citrobacter sp. SAASenr-X1: Characteristics, performance, pathways, risk assessment, and practical applications
作者：Xu, Chenglong;Zhu, Xianpu;Li, Shuangxi;Bai, Naling;Zhang, Juanqin;Zhang, Hanlin;Lv, Weiguang;Li, Yunhao;Lu, Jialei;Xu, Chenglong;Li, Shuangxi;Zhang, Hanlin;Lv, Weiguang;Xu, Chenglong;Li, Shuangxi;Zhang, Hanlin;Lv, Weiguang
关键词：Enrofloxacin biotransformation; Citrobacter sp. SAASenr-X1; Degradation pathways; Ecological safety; Practical applications
