Air oxidation behavior of wet-mechanochemically synthesized pyrite FeS<sub>2</sub>: Fenton performance regulated by Fe species, sulfur vacancy and crystal facet ratio

doi:10.1016/j.cej.2025.161166

IMR OpenIR

	Air oxidation behavior of wet-mechanochemically synthesized pyrite FeS₂: Fenton performance regulated by Fe species, sulfur vacancy and crystal facet ratio
	Wen, Zunqing 1; Shi, Xiaoguo 1; Sui, Huiying 1; Zhang, Minglu 1; Zhang, Longquan 1; Gu, Yawei 1; Feng, Qing 1; Ma, Ke 2; Zhang, Na 1; Wang, Mingzhe 1; Zhang, Ruiyan 1; Xu, Chongqing 1,3; Li, Zengjin 4; Xue, Rong 1
通讯作者	Shi, Xiaoguo(shixg@qlu.edu.cn) ; Xue, Rong(xr@qlu.edu.cn)
	2025-04-01
发表期刊	CHEMICAL ENGINEERING JOURNAL
ISSN	1385-8947
卷号	509 页码:11
摘要	Numerous studies have revealed that air oxidation behavior profoundly impacts pyrite properties. Whereas its influence on pyrite Fenton performance remains controversial. Herein, pyrite FeS2 nanoparticles synthesized by facile wet-mechanochemical method was employed as oxidation model and its oxidation degree was evaluated by XPS depth profiling technique. Based on theoretical calculation and experimental evidence, the properties and Fenton performance of surface oxidized pyrite (SOPx) were comprehensively assessed. With oxidation degree increase, free radical generation selectivity was alternated from center dot O2- to center dot OH, and the selectivity to center dot OH showed strong correlations with {210} facet ratio, Fe(II)-O and sulfur vacancies (SVs) contents. The oxidation degree dependence in center dot OH selective production primarily stemmed from different electron-donating and Fe2+ releasing capacity. Moderately oxidized pyrite (SOP4) with high {210} facet ratio, SVs and Fe(II)-O contents could donate electrons for H2O2 barrierless dissociation and Fe2+/Fe3+ redox-cycle, and cause more Fe2+ releasing to enhance homogeneous Fenton reaction. As the oxidation degree increased (from SOP0 to SOP4), the Fenton systems demonstrated a significant enhancement in sulfadiazine (SDZ) degradation kinetics, with the rate constant increasing from 0.02039 to 0.06904 min-1. The superior SDZ removal efficiency in SOP4 system at wide pH range (5-9) indicated moderate oxidation significantly improved its decontamination and practical application ability. However, the amorphous iron oxide layer generated in the over-oxidized pyrite (SOP6) impaired its catalytic activity, resulting in a decrease of the rate constant (0.0485 min-1). These findings unveiled the mystery of Fenton performance regulated by FeS2 oxidation via {210} facet, SVs and Fe(II)-O, and offered fresh insights into developing targeted structures for tunable performance.
关键词	pyrite FeS2 Oxidation Crystal facet ratio Sulfur vacancy Fenton performance
资助者	Science, Education and Industry Integration Pilot Projects of Qilu University of Technology (Shandong Academy of Sciences) ; Talent and Scientific Research Project of Qilu University of Technology (Shandong Academy of Sciences) ; Major Innovation Projects of Science, Education, and Industry Integration of Qilu University of Technology (Shandong Academy of Science) ; Natural Science Foundation of Shandong Province ; Youth Innovation Team Plan of Higher Education in Shandong Province ; Technology Development Project - Zhongding Special Metals QHD Technology Co., LTD
DOI	10.1016/j.cej.2025.161166
收录类别	SCI
语种	英语
资助项目	Science, Education and Industry Integration Pilot Projects of Qilu University of Technology (Shandong Academy of Sciences)[2023PX016] ; Science, Education and Industry Integration Pilot Projects of Qilu University of Technology (Shandong Academy of Sciences)[2023PX049] ; Talent and Scientific Research Project of Qilu University of Technology (Shandong Academy of Sciences)[2023RCKY109] ; Talent and Scientific Research Project of Qilu University of Technology (Shandong Academy of Sciences)[2023RCKY113] ; Major Innovation Projects of Science, Education, and Industry Integration of Qilu University of Technology (Shandong Academy of Science)[2022JBZ02-05] ; Natural Science Foundation of Shandong Province[ZR2021QE042] ; Youth Innovation Team Plan of Higher Education in Shandong Province[2023K139] ; Technology Development Project - Zhongding Special Metals QHD Technology Co., LTD[QL2023017] ; Technology Development Project - Zhongding Special Metals QHD Technology Co., LTD[2024ZDZX10]
WOS研究方向	Engineering
WOS类目	Engineering, Environmental ; Engineering, Chemical
WOS记录号	WOS:001441764200001
出版者	ELSEVIER SCIENCE SA
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/179715
专题	中国科学院金属研究所
通讯作者	Shi, Xiaoguo; Xue, Rong
作者单位	1.Qilu Univ Technol, Shandong Acad Sci, Sch Environm Sci & Engn, Jinan 250353, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Qilu Univ Technol, Ecol Inst, Shandong Acad Sci, Jinan 250013, Peoples R China 4.Shandong Lanran Environm Technol Co Ltd, Jinan 25000, Peoples R China
推荐引用方式 GB/T 7714	Wen, Zunqing,Shi, Xiaoguo,Sui, Huiying,et al. Air oxidation behavior of wet-mechanochemically synthesized pyrite FeS₂: Fenton performance regulated by Fe species, sulfur vacancy and crystal facet ratio[J]. CHEMICAL ENGINEERING JOURNAL,2025,509:11.
APA	Wen, Zunqing.,Shi, Xiaoguo.,Sui, Huiying.,Zhang, Minglu.,Zhang, Longquan.,...&Xue, Rong.(2025).Air oxidation behavior of wet-mechanochemically synthesized pyrite FeS₂: Fenton performance regulated by Fe species, sulfur vacancy and crystal facet ratio.CHEMICAL ENGINEERING JOURNAL,509,11.
MLA	Wen, Zunqing,et al."Air oxidation behavior of wet-mechanochemically synthesized pyrite FeS₂: Fenton performance regulated by Fe species, sulfur vacancy and crystal facet ratio".CHEMICAL ENGINEERING JOURNAL 509(2025):11.