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Silicon-Containing Neurotensin Analogues as Radiopharmaceuticals for NTS1-Positive Tumors Imaging
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    Silicon-Containing Neurotensin Analogues as Radiopharmaceuticals for NTS1-Positive Tumors Imaging
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    • Roberto Fanelli
      Roberto Fanelli
      Institut des Biomolécules Max Mousseron, IBMM, UMR-5247, CNRS, Université de Montpellier, ENSCM, Place Eugène Bataillon, Montpellier 34095 Cedex 5, France
    • Adrien Chastel
      Adrien Chastel
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
    • Santo Previti
      Santo Previti
      Institut des Biomolécules Max Mousseron, IBMM, UMR-5247, CNRS, Université de Montpellier, ENSCM, Place Eugène Bataillon, Montpellier 34095 Cedex 5, France
    • Elif Hindié
      Elif Hindié
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
      More by Elif Hindié
    • Delphine Vimont
      Delphine Vimont
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
    • Paolo Zanotti-Fregonara
      Paolo Zanotti-Fregonara
      Houston Methodist Research Institute, Houston, Texas 77030, United States
    • Philippe Fernandez
      Philippe Fernandez
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
    • Philippe Garrigue
      Philippe Garrigue
      Aix-Marseille University, INSERM, Institut National de la Recherche Agronomique, Centre de Recherche en Cardiovasculaire et Nutrition, Marseille 13385, France
      Aix-Marseille University, Centre Européen de Recherche en Imagerie Médicale, Marseille 13005, France
    • Frédéric Lamare
      Frédéric Lamare
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
    • Romain Schollhammer
      Romain Schollhammer
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
    • Laure Balasse
      Laure Balasse
      Aix-Marseille University, INSERM, Institut National de la Recherche Agronomique, Centre de Recherche en Cardiovasculaire et Nutrition, Marseille 13385, France
    • Benjamin Guillet
      Benjamin Guillet
      Aix-Marseille University, INSERM, Institut National de la Recherche Agronomique, Centre de Recherche en Cardiovasculaire et Nutrition, Marseille 13385, France
      Aix-Marseille University, Centre Européen de Recherche en Imagerie Médicale, Marseille 13005, France
    • Emmanuelle Rémond
      Emmanuelle Rémond
      Institut des Biomolécules Max Mousseron, IBMM, UMR-5247, CNRS, Université de Montpellier, ENSCM, Place Eugène Bataillon, Montpellier 34095 Cedex 5, France
    • Clément Morgat*
      Clément Morgat
      University of Bordeaux, CNRS, EPHE, INCIA, UMR 5287, Bordeaux F-33000, France
      Nuclear Medicine Department, University Hospital of Bordeaux, Bordeaux F-33000, France
      *Email: [email protected]
    • Florine Cavelier*
      Florine Cavelier
      Institut des Biomolécules Max Mousseron, IBMM, UMR-5247, CNRS, Université de Montpellier, ENSCM, Place Eugène Bataillon, Montpellier 34095 Cedex 5, France
      *Email: [email protected]
    Other Access OptionsSupporting Information (1)

    Bioconjugate Chemistry

    Cite this: Bioconjugate Chem. 2020, 31, 10, 2339–2349
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.bioconjchem.0c00419
    Published September 4, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Abstract Image

    Several independent studies have demonstrated the overexpression of NTS1 in various malignancies, which make this receptor of interest for imaging and therapy. To date, radiolabeled neurotensin analogues suffer from low plasmatic stability and thus insufficient availability for high uptake in tumors. We report the development of 68Ga-radiolabeled neurotensin analogues with improved radiopharmaceutical properties through the introduction of the silicon-containing amino acid trimethylsilylalanine (TMSAla). Among the series of novel radiolabeled neurotensin analogues, [68Ga]Ga-JMV6659 exhibits high hydrophilicity (log D7.4 = −3.41 ± 0.14), affinity in the low nanomolar range toward NTS1 (Kd = 6.29 ± 1.37 nM), good selectivity (Kd NTS1/Kd NTS2 = 35.9), and high NTS1-mediated internalization. It has lower efflux and prolonged plasmatic half-life in human plasma as compared to the reference compound ([68Ga]Ga-JMV6661 bearing the minimum active fragment of neurotensin and the same linker and chelate as other analogues). In nude mice bearing HT-29 xenograft, [68Ga]Ga-JMV6659 uptake reached 7.8 ± 0.54 %ID/g 2 h post injection. Uptake was decreased to 1.38 ± 0.71 %ID/g with injection of excess of non-radioactive neurotensin. Radiation dose as extrapolated to human was estimated as 2.35 ± 0.6 mSv for a standard injected activity of 100MBq. [68Ga]Ga-JMV6659 was identified as a promising lead compound suitable for PET imaging of NTS1-expressing tumors.

    Copyright © 2020 American Chemical Society

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    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.bioconjchem.0c00419.

    • Synthesis and control of peptides, characterization of NTS1 and NTS2 expressions in HT-29 cells, quality controls of 68Ga-neurotensin analogues, stability of 68Ga-radiolabeling in PBS and in human plasma, biodistribution assessed on PET images and after animal sacrifice, and plasma protein binding of [68Ga]Ga-JMV6659 (PDF)

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    Cited By

    Click to copy section linkSection link copied!

    This article is cited by 14 publications.

    1. Sacha Bodin, Lisa C. Peuker, Emmanuelle Jestin, Isabel D. Alves, Valérie Velasco, Imade Ait-Arsa, Romain Schollhammer, Frédéric Lamare, Delphine Vimont, Gaétan MacGrogan, Elif Hindié, Annette G. Beck-Sickinger, Clément Morgat. Development of Radiopharmaceuticals for NPY Receptor-5 (Y5) Nuclear Imaging in Tumors by Synthesis of Specific Agonists and Investigation of Their Binding Mode. Bioconjugate Chemistry 2023, 34 (11) , 2014-2021. https://doi.org/10.1021/acs.bioconjchem.3c00313
    2. Sacha Bodin, Santo Previti, Emmanuelle Jestin, Delphine Vimont, Imade Ait-Arsa, Frédéric Lamare, Emmanuelle Rémond, Elif Hindié, Florine Cavelier, Clément Morgat. Design, Synthesis, and Biological Evaluation of the First Radio-Metalated Neurotensin Analogue Targeting Neurotensin Receptor 2. ACS Omega 2023, 8 (7) , 6994-7004. https://doi.org/10.1021/acsomega.2c07814
    3. Emma Renard, Mathieu Moreau, Pierre-Simon Bellaye, Mélanie Guillemin, Bertrand Collin, Aurélie Prignon, Franck Denat, Victor Goncalves. Positron Emission Tomography Imaging of Neurotensin Receptor-Positive Tumors with 68Ga-Labeled Antagonists: The Chelate Makes the Difference Again. Journal of Medicinal Chemistry 2021, 64 (12) , 8564-8578. https://doi.org/10.1021/acs.jmedchem.1c00523
    4. Jenny-Lee Panayides, Darren Lyall Riley, Felix Hasenmaile, Willem A. L. van Otterlo. The role of silicon in drug discovery: a review. RSC Medicinal Chemistry 2024, 95 https://doi.org/10.1039/D4MD00169A
    5. Santo Previti, Sacha Bodin, Emmanuelle Rémond, Delphine Vimont, Elif Hindié, Clément Morgat, Florine Cavelier. Rational design of NT-PSMA heterobivalent probes for prostate cancer theranostics. RSC Medicinal Chemistry 2024, 10 https://doi.org/10.1039/D4MD00491D
    6. C. Dupire, P. Chennell, B. Pereira, N. Courtiol, S. Buj, R. Cueff, S. Crauste-Manciet, V. Sautou, C. Morgat. A proof of principle study using radiopharmaceuticals to quantify and localize container-content interactions in medical syringes. Scientific Reports 2023, 13 (1) https://doi.org/10.1038/s41598-023-29923-z
    7. Hegine I. Hakobyan, Silva M. Jamgaryan, Armen S. Sargsyan, Yuri M. Danghyan, Vladimir A. Larionov, Victor I. Maleev, Ashot S. Saghyan, Zorayr Z. Mardiyan. A Stereoselective Entry to Enantiopure (S)-2-Amino-2-methyl-5-arylpent-4-ynoic Acids and Evaluation of Their Inhibitory Activity against Bacterial Collagenase G. Symmetry 2023, 15 (10) , 1924. https://doi.org/10.3390/sym15101924
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    9. Sergey N. Adamovich, Igor A. Ushakov, Elizaveta N. Oborina, Svetlana V. Lukyanova, Vladislav Y. Komarov. New 3-Aminopropylsilatrane Derivatives: Synthesis, Structure, Properties, and Biological Activity. International Journal of Molecular Sciences 2023, 24 (12) , 9965. https://doi.org/10.3390/ijms24129965
    10. Mariacristina Failla, Giuseppe Floresta, Vincenzo Abbate. Peptide-based positron emission tomography probes: current strategies for synthesis and radiolabelling. RSC Medicinal Chemistry 2023, 14 (4) , 592-623. https://doi.org/10.1039/D2MD00397J
    11. Romain Schollhammer, Marie-Laure Quintyn Ranty, Henri de Clermont Gallerande, Florine Cavelier, Ibai E. Valverde, Delphine Vimont, Elif Hindié, Clément Morgat. Theranostics of Primary Prostate Cancer: Beyond PSMA and GRP-R. Cancers 2023, 15 (8) , 2345. https://doi.org/10.3390/cancers15082345
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    13. Clément Morgat, Véronique Brouste, Adrien Chastel, Valérie Vélasco, Gaétan Macgrogan, Elif Hindié. Expression of neurotensin receptor-1 (NTS1) in primary breast tumors, cellular distribution, and association with clinical and biological factors. Breast Cancer Research and Treatment 2021, 190 (3) , 403-413. https://doi.org/10.1007/s10549-021-06402-5
    14. Mária Bodnár Mikulová, Peter Mikuš. Advances in Development of Radiometal Labeled Amino Acid-Based Compounds for Cancer Imaging and Diagnostics. Pharmaceuticals 2021, 14 (2) , 167. https://doi.org/10.3390/ph14020167

    Bioconjugate Chemistry

    Cite this: Bioconjugate Chem. 2020, 31, 10, 2339–2349
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.bioconjchem.0c00419
    Published September 4, 2020
    Copyright © 2020 American Chemical Society

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