Immobilization of Sb(V) by secondary Fe (oxyhydr)oxides during Fe(II) oxygenation: Insights into Sb(V) incorporation and Fe(II) mineralization mechanisms

IF 3.6 2区地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS

Chemical Geology Pub Date : 2024-12-16 DOI:10.1016/j.chemgeo.2024.122567

Yiqing Wang, Mengchang He, Chunye Lin, Wei Ouyang, Xitao Liu

{"title":"Immobilization of Sb(V) by secondary Fe (oxyhydr)oxides during Fe(II) oxygenation: Insights into Sb(V) incorporation and Fe(II) mineralization mechanisms","authors":"Yiqing Wang, Mengchang He, Chunye Lin, Wei Ouyang, Xitao Liu","doi":"10.1016/j.chemgeo.2024.122567","DOIUrl":null,"url":null,"abstract":"Abiotic Fe(II) oxygenation to form secondary Fe (oxyhydr)oxides commonly occurs in natural environments and critically affects the mobility and fate of metalloids such as antimony (Sb). However, the Sb(V) immobilization process and mechanism during Fe(II) oxygenation are not well understood, and the interactions between Sb(V) and formed Fe (oxyhydr)oxides need further study. This study comprehensively investigated Sb(V) immobilization and secondary Fe (oxyhydr)oxides formation during Fe(II) oxygenation for 10 h in the presence of Sb(V). The results indicated that Sb(V) was immobilized by secondary Fe (oxyhydr)oxides mainly via coprecipitation rather than adsorption. Extended X-ray absorption fine structure (EXAFS) analysis further verified that Sb(V) was structurally incorporated into the formed lepidocrocite mainly via edge-sharing linkage and into goethite via edge-sharing and double corner-sharing linkages between SbO<ce:inf loc=\"post\">6</ce:inf> and FeO<ce:inf loc=\"post\">6</ce:inf> octahedra, thus resulting in the formation of various secondary Fe (oxyhydr)oxides. Additionally, Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and X-ray diffraction (XRD) characterization demonstrated that Sb(V) incorporation inhibited lepidocrocite formation and favored goethite formation at pH 6 and 7 with initial Sb(V)/Fe(II) molar ratios above 0.01 and 0.04, respectively, and it also hindered magnetite formation at pH 8. Transmission electron microscopy (TEM) suggested that Sb(V) incorporation affected the morphologies of formed Fe (oxyhydr)oxides. Overall, our findings provide valuable insights into Sb(V) immobilization and Fe (oxyhydr)oxides formation during Fe(II) oxygenation, and are conducive to clarifying the geochemical behavior of Sb(V) coupled with Fe(II) at dynamic redox interfaces in Sb(V)-contaminated environments.","PeriodicalId":9847,"journal":{"name":"Chemical Geology","volume":"64 1","pages":""},"PeriodicalIF":3.6000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Geology","FirstCategoryId":"89","ListUrlMain":"https://doi.org/10.1016/j.chemgeo.2024.122567","RegionNum":2,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"GEOCHEMISTRY & GEOPHYSICS","Score":null,"Total":0}

引用次数: 0

Abstract

Abiotic Fe(II) oxygenation to form secondary Fe (oxyhydr)oxides commonly occurs in natural environments and critically affects the mobility and fate of metalloids such as antimony (Sb). However, the Sb(V) immobilization process and mechanism during Fe(II) oxygenation are not well understood, and the interactions between Sb(V) and formed Fe (oxyhydr)oxides need further study. This study comprehensively investigated Sb(V) immobilization and secondary Fe (oxyhydr)oxides formation during Fe(II) oxygenation for 10 h in the presence of Sb(V). The results indicated that Sb(V) was immobilized by secondary Fe (oxyhydr)oxides mainly via coprecipitation rather than adsorption. Extended X-ray absorption fine structure (EXAFS) analysis further verified that Sb(V) was structurally incorporated into the formed lepidocrocite mainly via edge-sharing linkage and into goethite via edge-sharing and double corner-sharing linkages between SbO6 and FeO6 octahedra, thus resulting in the formation of various secondary Fe (oxyhydr)oxides. Additionally, Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and X-ray diffraction (XRD) characterization demonstrated that Sb(V) incorporation inhibited lepidocrocite formation and favored goethite formation at pH 6 and 7 with initial Sb(V)/Fe(II) molar ratios above 0.01 and 0.04, respectively, and it also hindered magnetite formation at pH 8. Transmission electron microscopy (TEM) suggested that Sb(V) incorporation affected the morphologies of formed Fe (oxyhydr)oxides. Overall, our findings provide valuable insights into Sb(V) immobilization and Fe (oxyhydr)oxides formation during Fe(II) oxygenation, and are conducive to clarifying the geochemical behavior of Sb(V) coupled with Fe(II) at dynamic redox interfaces in Sb(V)-contaminated environments.

查看原文本刊更多论文

求助全文

约1分钟内获得全文求助全文

来源期刊

Chemical Geology 地学-地球化学与地球物理

CiteScore

7.20

自引率

10.30%

发文量

374

审稿时长

3.6 months

期刊介绍： Chemical Geology is an international journal that publishes original research papers on isotopic and elemental geochemistry, geochronology and cosmochemistry. The Journal focuses on chemical processes in igneous, metamorphic, and sedimentary petrology, low- and high-temperature aqueous solutions, biogeochemistry, the environment and cosmochemistry. Papers that are field, experimentally, or computationally based are appropriate if they are of broad international interest. The Journal generally does not publish papers that are primarily of regional or local interest, or which are primarily focused on remediation and applied geochemistry. The Journal also welcomes innovative papers dealing with significant analytical advances that are of wide interest in the community and extend significantly beyond the scope of what would be included in the methods section of a standard research paper.