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La–[18/19F]fluoride complexes: a novel addition to the radiofluorination family.

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Title: La–[18/19F]fluoride complexes: a novel addition to the radiofluorination family.
Authors: Behe, Martin1 (AUTHOR), Gruber, Stefan2 (AUTHOR), Li, Cen3 (AUTHOR), Schreckenbach, Georg3 (AUTHOR), Mu, Linjing2 (AUTHOR), Schottelius, Margret4 (AUTHOR), Faizova, Radmila1,2,4 (AUTHOR)
Source: Dalton Transactions: An International Journal of Inorganic Chemistry. 4/21/2026, Vol. 55 Issue 15, p5944-5951. 8p.
Subjects: Fluorination, Ligands (Chemistry), Density functional theory, Radiopharmaceuticals, Positron emission tomography, Companion diagnostics, Coordinate covalent bond
Abstract: Here, we report the synthesis and evaluation of La–[18/19F]fluoride coordination complexes with macrocyclic ligands, expanding the family of metal–[18F]fluoride coordination species for PET imaging applications. Fluorination of a series of La complexes with macrocyclic chelators (L = DOTA, DOTAM, macropa, and DOTpy) was explored, and the resulting products were characterized using 19F and 1H NMR, mass spectrometry, and X-ray spectroscopy. The stability of these complexes in water was found to inversely correlate with the electron-donating properties of the chelator. Notably, [LaF(L)]x complexes with macropa and DOTpy exhibited high stability in organic solution, with [LaF(DOTpy)]OTf2 also demonstrating stability in water. DFT study (PBE-D3(BJ)/TZ2P, COSMO) indicates that the ΔΔG magnitudes between [LaFL] and [La(H2O)L] could explain these results: much higher for DOTpy (21.66 kcal mol−1) and DOTAM (15.86 kcal mol−1) than for DOTA (6.78 kcal mol−1) and Macropa (8.05 kcal mol−1) supports the observed stabilities. Radiofluorination of [LaF(DOTpy)]OTf2 afforded [18F][LaF(DOTpy)]2+ in high radiochemical purity, representing the first example of a La–[18F]fluoride coordination complex. These findings expand the scope of metal–[18F]fluoride coordination chemistry and lay the groundwork for developing La/Ac-based fluoride complexes as theranostic pairs, with applications in 225Ac-based radiopharmaceuticals for personalized dosimetry and PET-guided therapy monitoring. [ABSTRACT FROM AUTHOR]
Copyright of Dalton Transactions: An International Journal of Inorganic Chemistry is the property of Royal Society of Chemistry 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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  Data: La–[<superscript>18/19</superscript>F]fluoride complexes: a novel addition to the radiofluorination family.
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  Data: <searchLink fieldCode="AR" term="%22Behe%2C+Martin%22">Behe, Martin</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Gruber%2C+Stefan%22">Gruber, Stefan</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Li%2C+Cen%22">Li, Cen</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Schreckenbach%2C+Georg%22">Schreckenbach, Georg</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Mu%2C+Linjing%22">Mu, Linjing</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Schottelius%2C+Margret%22">Schottelius, Margret</searchLink><relatesTo>4</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Faizova%2C+Radmila%22">Faizova, Radmila</searchLink><relatesTo>1,2,4</relatesTo> (AUTHOR)
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  Data: <searchLink fieldCode="DE" term="%22Fluorination%22">Fluorination</searchLink><br /><searchLink fieldCode="DE" term="%22Ligands+%28Chemistry%29%22">Ligands (Chemistry)</searchLink><br /><searchLink fieldCode="DE" term="%22Density+functional+theory%22">Density functional theory</searchLink><br /><searchLink fieldCode="DE" term="%22Radiopharmaceuticals%22">Radiopharmaceuticals</searchLink><br /><searchLink fieldCode="DE" term="%22Positron+emission+tomography%22">Positron emission tomography</searchLink><br /><searchLink fieldCode="DE" term="%22Companion+diagnostics%22">Companion diagnostics</searchLink><br /><searchLink fieldCode="DE" term="%22Coordinate+covalent+bond%22">Coordinate covalent bond</searchLink>
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  Label: Abstract
  Group: Ab
  Data: Here, we report the synthesis and evaluation of La–[18/19F]fluoride coordination complexes with macrocyclic ligands, expanding the family of metal–[18F]fluoride coordination species for PET imaging applications. Fluorination of a series of La complexes with macrocyclic chelators (L = DOTA, DOTAM, macropa, and DOTpy) was explored, and the resulting products were characterized using 19F and 1H NMR, mass spectrometry, and X-ray spectroscopy. The stability of these complexes in water was found to inversely correlate with the electron-donating properties of the chelator. Notably, [LaF(L)]x complexes with macropa and DOTpy exhibited high stability in organic solution, with [LaF(DOTpy)]OTf2 also demonstrating stability in water. DFT study (PBE-D3(BJ)/TZ2P, COSMO) indicates that the ΔΔG magnitudes between [LaFL] and [La(H2O)L] could explain these results: much higher for DOTpy (21.66 kcal mol−1) and DOTAM (15.86 kcal mol−1) than for DOTA (6.78 kcal mol−1) and Macropa (8.05 kcal mol−1) supports the observed stabilities. Radiofluorination of [LaF(DOTpy)]OTf2 afforded [18F][LaF(DOTpy)]2+ in high radiochemical purity, representing the first example of a La–[18F]fluoride coordination complex. These findings expand the scope of metal–[18F]fluoride coordination chemistry and lay the groundwork for developing La/Ac-based fluoride complexes as theranostic pairs, with applications in 225Ac-based radiopharmaceuticals for personalized dosimetry and PET-guided therapy monitoring. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Dalton Transactions: An International Journal of Inorganic Chemistry is the property of Royal Society of Chemistry 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:
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      – Type: doi
        Value: 10.1039/d5dt02645h
    Languages:
      – Code: eng
        Text: English
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      Pagination:
        PageCount: 8
        StartPage: 5944
    Subjects:
      – SubjectFull: Fluorination
        Type: general
      – SubjectFull: Ligands (Chemistry)
        Type: general
      – SubjectFull: Density functional theory
        Type: general
      – SubjectFull: Radiopharmaceuticals
        Type: general
      – SubjectFull: Positron emission tomography
        Type: general
      – SubjectFull: Companion diagnostics
        Type: general
      – SubjectFull: Coordinate covalent bond
        Type: general
    Titles:
      – TitleFull: La–[18/19F]fluoride complexes: a novel addition to the radiofluorination family.
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            NameFull: Li, Cen
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            – D: 21
              M: 04
              Text: 4/21/2026
              Type: published
              Y: 2026
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            – TitleFull: Dalton Transactions: An International Journal of Inorganic Chemistry
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