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    Article

    Manipulating Nanoparticle Aggregates Regulates Receptor–Ligand Binding in Macrophages
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    • Yuri Kim
      Yuri Kim
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
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    • Hee Joon Jung
      Hee Joon Jung
      Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
      International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208, United States
      NUANCE Center, Northwestern University, Evanston, Illinois 60208, United States
      More by Hee Joon Jung
      Orcidhttps://orcid.org/0000-0001-7963-0897
    • Yunjung Lee
      Yunjung Lee
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering, Seoul National University, Seoul 08826, Republic of Korea
      More by Yunjung Lee
    • Sagang Koo
      Sagang Koo
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering, Seoul National University, Seoul 08826, Republic of Korea
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      Orcidhttps://orcid.org/0000-0001-8154-7881
    • Ramar Thangam
      Ramar Thangam
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
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      Orcidhttps://orcid.org/0000-0002-6209-7149
    • Woo Young Jang
      Woo Young Jang
      Department of Orthopedic Surgery, Korea University Anam Hospital, Seoul 02841, Republic of Korea
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    • Seong Yeol Kim
      Seong Yeol Kim
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
      More by Seong Yeol Kim
    • Sangwoo Park
      Sangwoo Park
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
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    • Sungkyu Lee
      Sungkyu Lee
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
      More by Sungkyu Lee
    • Gunhyu Bae
      Gunhyu Bae
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
      More by Gunhyu Bae
    • Kapil Dev Patel
      Kapil Dev Patel
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
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    • Qiang Wei
      Qiang Wei
      College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials and Engineering, Sichuan University, Chengdu 610065, China
      More by Qiang Wei
      Orcidhttps://orcid.org/0000-0001-5194-8262
    • Ki-Bum Lee
      Ki-Bum Lee
      Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, New Jersey 08854, United States
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      Orcidhttps://orcid.org/0000-0002-8164-0047
    • Ramasamy Paulmurugan
      Ramasamy Paulmurugan
      Department of Radiology, Molecular Imaging Program at Stanford, Stanford University School of Medicine, Stanford University, Palo Alto, California 94304, United States
      Department of Radiology, Canary Center at Stanford for Cancer Early Detection, Stanford University School of Medicine, Stanford University, Palo Alto, California 94304, United States
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      Orcidhttps://orcid.org/0000-0001-7155-4738
    • Woong Kyo Jeong
      Woong Kyo Jeong
      Department of Orthopedic Surgery, Korea University Anam Hospital, Seoul 02841, Republic of Korea
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    • Taeghwan Hyeon
      Taeghwan Hyeon
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering, Seoul National University, Seoul 08826, Republic of Korea
      More by Taeghwan Hyeon
      Orcidhttps://orcid.org/0000-0001-5959-6257
    • Dokyoon Kim*
      Dokyoon Kim
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      Department of Bionano Engineering and Bionanotechnology, Hanyang University, Ansan 15588, Republic of Korea
      *[email protected]
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    • Heemin Kang*
      Heemin Kang
      Department of Materials Science and Engineering, Korea University, Seoul 02841, Republic of Korea
      Department of Biomicrosystem Technology, Korea University, Seoul 02841, Republic of Korea
      *[email protected]
      More by Heemin Kang
      Orcidhttps://orcid.org/0000-0003-2694-9882
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 13, 5769–5783
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c08861
    Published March 11, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    The receptor–ligand interactions in cells are dynamically regulated by modulation of the ligand accessibility. In this study, we utilize size-tunable magnetic nanoparticle aggregates ordered at both nanometer and atomic scales. We flexibly anchor magnetic nanoparticle aggregates of tunable sizes over the cell-adhesive RGD ligand (Arg-Gly-Asp)-active material surface while maintaining the density of dispersed ligands accessible to macrophages at constant. Lowering the accessible ligand dispersity by increasing the aggregate size at constant accessible ligand density facilitates the binding of integrin receptors to the accessible ligands, which promotes the adhesion of macrophages. In high ligand dispersity, distant magnetic manipulation to lift the aggregates (which increases ligand accessibility) stimulates the binding of integrin receptors to the accessible ligands available under the aggregates to augment macrophage adhesion-mediated pro-healing polarization both in vitro and in vivo. In low ligand dispersity, distant control to drop the aggregates (which decreases ligand accessibility) repels integrin receptors away from the aggregates, thereby suppressing integrin receptor–ligand binding and macrophage adhesion, which promotes inflammatory polarization. Here, we present “accessible ligand dispersity” as a novel fundamental parameter that regulates receptor–ligand binding, which can be reversibly manipulated by increasing and decreasing the ligand accessibility. Limitless tuning of nanoparticle aggregate dimensions and morphology can offer further insight into the regulation of receptor–ligand binding in host cells.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c08861.

    • Supplementary Movie S1: The internalization of magnetic nanoparticle aggregates into macrophages is negligible (MP4)

    • Supplementary Movie S2: Negligible physical rupture of magnetic nanoparticle aggregates under a magnetic field (MP4)

    • Experimental Section: Characterization of magnetic nanoparticle aggregates composed of iron oxide nanoparticle ensemble (via SAD pattern, zeta potential, FTIR, TEM, DLS, VSM, AFM, and SEM); distant manipulation of the accessible ligand dispersity on integrin β1 expression, macrophage adhesion and polarization involving myosin II, actin polymerization, and ROCK; substrate stability in vivo; host macrophage and neutrophil adhesion (confocal immunofluorescence imaging, Western blotting, and SEM) (PDF)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 13, 5769–5783
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c08861
    Published March 11, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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