Synergistic enhancement of arsenic immobilization in magnetite-persulfate systems: mechanistic insights into adsorption-oxidation processes
文献类型：期刊论文
| 作者 | Liu, Siyan1; Gao, Yu1,4; Yan, Xiulan1; Begum, Farida3; Yang, Xiao1; Zhou, Yaoyu2 |
| 刊名 | SEPARATION AND PURIFICATION TECHNOLOGY
 |
| 出版日期 | 2025-12-31 |
| 卷号 | 379页码:135078 |
| 关键词 | Arsenic immobilization Magnetite Adsorption Interface regulation Persulfate |
| ISSN号 | 1383-5866 |
| DOI | 10.1016/j.seppur.2025.135078 |
| 产权排序 | 1 |
| 文献子类 | Article |
| 英文摘要 | Magnetite (Mt), while demonstrating arsenic adsorption potential, suffers from compromised efficacy due to the changeable arsenic speciation under dynamic redox conditions. To address this limitation, we developed a magnetite-persulfate (Mt-PDS) system and systematically investigated its absorptive performance and mechanisms toward As. The addition of persulfate (PDS) significantly enhanced the removal efficiency of Mt to As, by which increasing the maximum adsorption capacities for 1.98 to 3.21 mgg(-1) for As(III) and from 3.69 to 4.02 mgg(-1) for As(V). Kinetic data fitted well with the pseudo-second-order model (R-2 > 0.99), indicating chemisorption-dominated processes. Isothermal adsorption experiments demonstrated superior arsenic removal efficiency across a broad pH range in the Mt-PDS system compared to Mt alone. Specifically, PDS addition enhanced As(III) adsorption capacity by 121 % and 78.28 % under acidic and alkaline conditions, respectively, while As(V) adsorption increased by 15.80 % and 44.71 %. Electron paramagnetic resonance analysis coupled with quenching tests revealed that PDS activation through Fe(II)/Fe(III) redox cycling generated sulfate (SO4(-)) and hydroxyl (OH) radicals, which oxidized As(III) to As(V), substantially improving overall arsenic removal efficiency. Density functional theory calculations confirmed arsenate anions preferentially adopt a bidentate coordination with Mt in presence of PDS, which evidenced by reduced adsorption energies and shortened As-Fe bonds. Structural characterization revealed multiple arsenic immobilization mechanisms, including surface hydroxyl complexation, hydrogen bonding interactions, sulfur-mediated coordination, and precipitation. Notably, the formation of scorodite and arsenopyrite through precipitation emerged as a critical pathway for arsenic immobilization, which in turn mitigating the risk of arsenic remobilization from Mt surfaces. This study provides mechanistic insights into the synergistic enhancement of arsenic management through integrated adsorption-oxidation processes. |
| URL标识 | 查看原文 |
| WOS关键词 | IRON |
| WOS研究方向 | Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:001583963500008 |
| 出版者 | ELSEVIER |
| 源URL | [http://ir.igsnrr.ac.cn/handle/311030/217481]  |
| 专题 | 陆地表层格局与模拟院重点实验室_外文论文 |
| 通讯作者 | Yan, Xiulan; Yang, Xiao |
| 作者单位 | 1.Chinese Acad Sci, Key Lab Land Surface Pattern & Simulat, Inst Geog Sci & Nat Resources Res, Beijing 100101, Peoples R China; 2.Hunan Agr Univ, Coll Environm & Ecol, Changsha 410128, Peoples R China 3.Karakoram Int Univ, Dept Environm Sci, Gilgit, Gilgit Baltista, Pakistan; 4.Univ Chinese Acad Sci, Coll Resources & Environm, Beijing 100190, Peoples R China; |
| 推荐引用方式 GB/T 7714 | Liu, Siyan,Gao, Yu,Yan, Xiulan,et al. Synergistic enhancement of arsenic immobilization in magnetite-persulfate systems: mechanistic insights into adsorption-oxidation processes[J]. SEPARATION AND PURIFICATION TECHNOLOGY,2025,379:135078. |
| APA | Liu, Siyan,Gao, Yu,Yan, Xiulan,Begum, Farida,Yang, Xiao,&Zhou, Yaoyu.(2025).Synergistic enhancement of arsenic immobilization in magnetite-persulfate systems: mechanistic insights into adsorption-oxidation processes.SEPARATION AND PURIFICATION TECHNOLOGY,379,135078. |
| MLA | Liu, Siyan,et al."Synergistic enhancement of arsenic immobilization in magnetite-persulfate systems: mechanistic insights into adsorption-oxidation processes".SEPARATION AND PURIFICATION TECHNOLOGY 379(2025):135078. |
入库方式： OAI收割
来源：地理科学与资源研究所
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