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Nanoscale and molecular evidences for adsorptive fractionation of dissolved organic matter at the interfaces of Al-bearing ferrihydrite and water.

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Title: Nanoscale and molecular evidences for adsorptive fractionation of dissolved organic matter at the interfaces of Al-bearing ferrihydrite and water.
Authors: Li, Li1,2 (AUTHOR), Zhang, Hanyue1,3 (AUTHOR) zhanghy@cib.ac.cn, Li, Xiaojuan4 (AUTHOR), Hu, Shiwen1,5 (AUTHOR) swhu@soil.cd.cn
Source: Water Research. Sep2025, Vol. 283, pN.PAG-N.PAG. 1p.
Subjects: Points of zero charge, Isomorphous structures, Adsorption capacity, Microscopy, Gibbsite, Dissolved organic matter
Abstract: • Al substitution altered the morphology, composition, and structure of ferrihydrite. • Ferrihydrite with 30 %mol Al substitution owned highest adsorption capacity for DOM. • C spatial distribution at nanoscale and binding mechanism of mineral-DOM were uncovered. • 30 %mol Al-substituted ferrihydrite depicted most pronounced DOM molecular fractionation. Ferrihydrite (Fh) usually exists in the form of Al-bearing Fh in soils and sediments, and Al substitution may have a remarkable influence on Fh characteristics, controlling its reaction with dissolved organic matter (DOM). Yet, little is known about the impacts of Al-bearing Fh on the fate of DOM. Here, selective binding and molecular fractionation of DOM was investigated at the interfaces of Al-bearing Fh and water. Al substitution altered surface properties such as point of zero charge (PZC), surface OH groups, and specific surface areas (SSA), structure, composition, and adsorption capacity of Fh. Specifically, within 30 mol% Al substitution, Al entered into ferrihydrite structure by isomorphous substitution to form Al-substituted ferrihydrite and immobilized DOM increased with Al substitution owing to increasing surface OH groups, SSA, and pore volumes. Once the amount of added Al exceeds 30 mol%, gibbsite was formed except for Al-substituted Fh, and adsorbed DOM decreased with Al addition. The coordination environment of Al-substituted Fh consisted of Fe-O and edge- and corner-sharing FeO 6 octahedral. Microscopic analysis at nanoscale disclosed that DOM was evenly distributed within Al-bearing Fh aggregates and on gibbsite surface, and DOM immobilized within Al-bearing Fh nanopores had a higher oxidation state. Mass spectrometry analysis at molecular scale revealed that compared with gibbsite, high molecular weight substances and substances containing more oxygenated groups or highly in unsaturation preferentially bound to Al-bearing Fh, and Fh with 30 mol% Al substitution induced most pronounced molecular fractionation. Collectively, these findings shed novel insights into the impact of Al substitution on interfacial adsorptive fractionation of DOM, contributing to in-depth understanding geochemical cycling of C and predicting organic C cycling across aquatic-terrestrial interfaces. [Display omitted] [ABSTRACT FROM AUTHOR]
Copyright of Water Research is the property of Pergamon Press - An Imprint of Elsevier Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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DbLabel: Engineering Source
An: 186161501
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  Label: Title
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  Data: Nanoscale and molecular evidences for adsorptive fractionation of dissolved organic matter at the interfaces of Al-bearing ferrihydrite and water.
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  Data: <searchLink fieldCode="AR" term="%22Li%2C+Li%22">Li, Li</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Zhang%2C+Hanyue%22">Zhang, Hanyue</searchLink><relatesTo>1,3</relatesTo> (AUTHOR)<i> zhanghy@cib.ac.cn</i><br /><searchLink fieldCode="AR" term="%22Li%2C+Xiaojuan%22">Li, Xiaojuan</searchLink><relatesTo>4</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Hu%2C+Shiwen%22">Hu, Shiwen</searchLink><relatesTo>1,5</relatesTo> (AUTHOR)<i> swhu@soil.cd.cn</i>
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  Data: <searchLink fieldCode="JN" term="%22Water+Research%22">Water Research</searchLink>. Sep2025, Vol. 283, pN.PAG-N.PAG. 1p.
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  Data: <searchLink fieldCode="DE" term="%22Points+of+zero+charge%22">Points of zero charge</searchLink><br /><searchLink fieldCode="DE" term="%22Isomorphous+structures%22">Isomorphous structures</searchLink><br /><searchLink fieldCode="DE" term="%22Adsorption+capacity%22">Adsorption capacity</searchLink><br /><searchLink fieldCode="DE" term="%22Microscopy%22">Microscopy</searchLink><br /><searchLink fieldCode="DE" term="%22Gibbsite%22">Gibbsite</searchLink><br /><searchLink fieldCode="DE" term="%22Dissolved+organic+matter%22">Dissolved organic matter</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: • Al substitution altered the morphology, composition, and structure of ferrihydrite. • Ferrihydrite with 30 %mol Al substitution owned highest adsorption capacity for DOM. • C spatial distribution at nanoscale and binding mechanism of mineral-DOM were uncovered. • 30 %mol Al-substituted ferrihydrite depicted most pronounced DOM molecular fractionation. Ferrihydrite (Fh) usually exists in the form of Al-bearing Fh in soils and sediments, and Al substitution may have a remarkable influence on Fh characteristics, controlling its reaction with dissolved organic matter (DOM). Yet, little is known about the impacts of Al-bearing Fh on the fate of DOM. Here, selective binding and molecular fractionation of DOM was investigated at the interfaces of Al-bearing Fh and water. Al substitution altered surface properties such as point of zero charge (PZC), surface OH groups, and specific surface areas (SSA), structure, composition, and adsorption capacity of Fh. Specifically, within 30 mol% Al substitution, Al entered into ferrihydrite structure by isomorphous substitution to form Al-substituted ferrihydrite and immobilized DOM increased with Al substitution owing to increasing surface OH groups, SSA, and pore volumes. Once the amount of added Al exceeds 30 mol%, gibbsite was formed except for Al-substituted Fh, and adsorbed DOM decreased with Al addition. The coordination environment of Al-substituted Fh consisted of Fe-O and edge- and corner-sharing FeO 6 octahedral. Microscopic analysis at nanoscale disclosed that DOM was evenly distributed within Al-bearing Fh aggregates and on gibbsite surface, and DOM immobilized within Al-bearing Fh nanopores had a higher oxidation state. Mass spectrometry analysis at molecular scale revealed that compared with gibbsite, high molecular weight substances and substances containing more oxygenated groups or highly in unsaturation preferentially bound to Al-bearing Fh, and Fh with 30 mol% Al substitution induced most pronounced molecular fractionation. Collectively, these findings shed novel insights into the impact of Al substitution on interfacial adsorptive fractionation of DOM, contributing to in-depth understanding geochemical cycling of C and predicting organic C cycling across aquatic-terrestrial interfaces. [Display omitted] [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Water Research is the property of Pergamon Press - An Imprint of Elsevier Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.1016/j.watres.2025.123896
    Languages:
      – Code: eng
        Text: English
    PhysicalDescription:
      Pagination:
        PageCount: 1
        StartPage: N.PAG
    Subjects:
      – SubjectFull: Points of zero charge
        Type: general
      – SubjectFull: Isomorphous structures
        Type: general
      – SubjectFull: Adsorption capacity
        Type: general
      – SubjectFull: Microscopy
        Type: general
      – SubjectFull: Gibbsite
        Type: general
      – SubjectFull: Dissolved organic matter
        Type: general
    Titles:
      – TitleFull: Nanoscale and molecular evidences for adsorptive fractionation of dissolved organic matter at the interfaces of Al-bearing ferrihydrite and water.
        Type: main
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      – PersonEntity:
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            NameFull: Li, Li
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            NameFull: Zhang, Hanyue
      – PersonEntity:
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            NameFull: Li, Xiaojuan
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            NameFull: Hu, Shiwen
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          Dates:
            – D: 01
              M: 09
              Text: Sep2025
              Type: published
              Y: 2025
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            – Type: issn-print
              Value: 00431354
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            – Type: volume
              Value: 283
          Titles:
            – TitleFull: Water Research
              Type: main
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