Xiaojie Wei , Xuelian Li , Honggang Sun , Qihan Feng , Youxuan Wang , Jiemin Li , Xingyu Liu , Li Wang
{"title":"fe基非晶合金中FeSx层的原位形成:硫化物层形成机理及催化活性的提高","authors":"Xiaojie Wei , Xuelian Li , Honggang Sun , Qihan Feng , Youxuan Wang , Jiemin Li , Xingyu Liu , Li Wang","doi":"10.1016/j.jallcom.2025.180899","DOIUrl":null,"url":null,"abstract":"<div><div>Sulfidated zero-valent iron (S-ZVI) has been demonstrated as a reliable approach for improving the surface passivation and accelerating electron transfer of ZVI. However, consumption of the iron sulfide layer resulted in a short lifespan. In this study, sulfidated FeBCCr<sub>1</sub> amorphous ribbons were successfully fabricated to effectively activate the persulfate (PS) for RhB degradation over a wide initial pH range (2.0–10.0), with a result of nearly 100 % of the color and 66.3 % of the total organic carbon removal efficiency. Based on the experiment results and adsorption phenomena, a surface-mediated heterogeneous activation mechanism was proposed. The in situ “self-reconstruction” iron sulfide layer (FeS<sub>x</sub>) generated on the surface of the amorphous ribbon acted as a cocatalyst to promote electron transfer from the matrix Fe<sup>0</sup> and continually accelerated the circulation of Fe<sup>3+</sup>/Fe<sup>2+</sup>. The continuous generation of FeS<sub>x</sub> during degradation prevented the layer aging and ensured the catalytic activity of the FeBCCr<sub>1</sub> amorphous ribbons. More importantly, the co-existence of Fe<sup>3+</sup> dramatically improved the stability of sulfide layer, electron utilization efficiency and material reusability, which was attributed to the improved conversion of Fe<sup>3+</sup> to Fe<sup>2+</sup> through charge transfer and the low consumption of Fe<sup>0</sup> in FeBCCr<sub>1</sub>/PS/Fe<sup>3+</sup> system. This work provides a new strategy for designing FeS<sub>x</sub> co-catalyst layer in FeBCCr<sub>1</sub>/PS system and provides an effective approach for macroscopic preparation of sulfidated Fe-based amorphous ribbons, establishing a solid foundation for the application of zero valent iron in the environmental field.</div></div>","PeriodicalId":344,"journal":{"name":"Journal of Alloys and Compounds","volume":"1030 ","pages":"Article 180899"},"PeriodicalIF":6.3000,"publicationDate":"2025-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In situ formation of FeSx layer on Fe-based amorphous alloys: Improvement of catalytic activity and mechanism of sulfide layer formation\",\"authors\":\"Xiaojie Wei , Xuelian Li , Honggang Sun , Qihan Feng , Youxuan Wang , Jiemin Li , Xingyu Liu , Li Wang\",\"doi\":\"10.1016/j.jallcom.2025.180899\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Sulfidated zero-valent iron (S-ZVI) has been demonstrated as a reliable approach for improving the surface passivation and accelerating electron transfer of ZVI. However, consumption of the iron sulfide layer resulted in a short lifespan. In this study, sulfidated FeBCCr<sub>1</sub> amorphous ribbons were successfully fabricated to effectively activate the persulfate (PS) for RhB degradation over a wide initial pH range (2.0–10.0), with a result of nearly 100 % of the color and 66.3 % of the total organic carbon removal efficiency. Based on the experiment results and adsorption phenomena, a surface-mediated heterogeneous activation mechanism was proposed. The in situ “self-reconstruction” iron sulfide layer (FeS<sub>x</sub>) generated on the surface of the amorphous ribbon acted as a cocatalyst to promote electron transfer from the matrix Fe<sup>0</sup> and continually accelerated the circulation of Fe<sup>3+</sup>/Fe<sup>2+</sup>. The continuous generation of FeS<sub>x</sub> during degradation prevented the layer aging and ensured the catalytic activity of the FeBCCr<sub>1</sub> amorphous ribbons. More importantly, the co-existence of Fe<sup>3+</sup> dramatically improved the stability of sulfide layer, electron utilization efficiency and material reusability, which was attributed to the improved conversion of Fe<sup>3+</sup> to Fe<sup>2+</sup> through charge transfer and the low consumption of Fe<sup>0</sup> in FeBCCr<sub>1</sub>/PS/Fe<sup>3+</sup> system. This work provides a new strategy for designing FeS<sub>x</sub> co-catalyst layer in FeBCCr<sub>1</sub>/PS system and provides an effective approach for macroscopic preparation of sulfidated Fe-based amorphous ribbons, establishing a solid foundation for the application of zero valent iron in the environmental field.</div></div>\",\"PeriodicalId\":344,\"journal\":{\"name\":\"Journal of Alloys and Compounds\",\"volume\":\"1030 \",\"pages\":\"Article 180899\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2025-05-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Alloys and Compounds\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0925838825024600\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Alloys and Compounds","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0925838825024600","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
In situ formation of FeSx layer on Fe-based amorphous alloys: Improvement of catalytic activity and mechanism of sulfide layer formation
Sulfidated zero-valent iron (S-ZVI) has been demonstrated as a reliable approach for improving the surface passivation and accelerating electron transfer of ZVI. However, consumption of the iron sulfide layer resulted in a short lifespan. In this study, sulfidated FeBCCr1 amorphous ribbons were successfully fabricated to effectively activate the persulfate (PS) for RhB degradation over a wide initial pH range (2.0–10.0), with a result of nearly 100 % of the color and 66.3 % of the total organic carbon removal efficiency. Based on the experiment results and adsorption phenomena, a surface-mediated heterogeneous activation mechanism was proposed. The in situ “self-reconstruction” iron sulfide layer (FeSx) generated on the surface of the amorphous ribbon acted as a cocatalyst to promote electron transfer from the matrix Fe0 and continually accelerated the circulation of Fe3+/Fe2+. The continuous generation of FeSx during degradation prevented the layer aging and ensured the catalytic activity of the FeBCCr1 amorphous ribbons. More importantly, the co-existence of Fe3+ dramatically improved the stability of sulfide layer, electron utilization efficiency and material reusability, which was attributed to the improved conversion of Fe3+ to Fe2+ through charge transfer and the low consumption of Fe0 in FeBCCr1/PS/Fe3+ system. This work provides a new strategy for designing FeSx co-catalyst layer in FeBCCr1/PS system and provides an effective approach for macroscopic preparation of sulfidated Fe-based amorphous ribbons, establishing a solid foundation for the application of zero valent iron in the environmental field.
期刊介绍:
The Journal of Alloys and Compounds is intended to serve as an international medium for the publication of work on solid materials comprising compounds as well as alloys. Its great strength lies in the diversity of discipline which it encompasses, drawing together results from materials science, solid-state chemistry and physics.