Chloride Ligands on DNA-Stabilized Silver Nanoclusters
Gonzàlez-Rosell, A., Malola, S., Guha, R., Arevalos, N. R., Matus, M. F., Goulet, M. E., Haapaniemi, E., Katz, B. B., Vosch, T., Kondo, J., Häkkinen, H., & Copp, S. M. (2023). Chloride Ligands on DNA-Stabilized Silver Nanoclusters. Journal of the American Chemical Society, 145(19), Article 10721-10729. https://doi.org/10.1021/jacs.3c01366
Julkaistu sarjassa
Journal of the American Chemical SocietyTekijät
Päivämäärä
2023Tekijänoikeudet
© 2023 The Authors. Published by American Chemical Society
DNA-stabilized silver nanoclusters (AgN-DNAs) are known to have one or two DNA oligomer ligands per nanocluster. Here, we present the first evidence that AgN-DNA species can possess additional chloride ligands that lead to increased stability in biologically relevant concentrations of chloride. Mass spectrometry of five chromatographically isolated near-infrared (NIR)-emissive AgN-DNA species with previously reported X-ray crystal structures determines their molecular formulas to be (DNA)2[Ag16Cl2]8+. Chloride ligands can be exchanged for bromides, which red-shift the optical spectra of these emitters. Density functional theory (DFT) calculations of the 6-electron nanocluster show that the two newly identified chloride ligands were previously assigned as low-occupancy silvers by X-ray crystallography. DFT also confirms the stability of chloride in the crystallographic structure, yields qualitative agreement between computed and measured UV–vis absorption spectra, and provides interpretation of the 35Cl-nuclear magnetic resonance spectrum of (DNA)2[Ag16Cl2]8+. A reanalysis of the X-ray crystal structure confirms that the two previously assigned low-occupancy silvers are, in fact, chlorides, yielding (DNA)2[Ag16Cl2]8+. Using the unusual stability of (DNA)2[Ag16Cl2]8+ in biologically relevant saline solutions as a possible indicator of other chloride-containing AgN-DNAs, we identified an additional AgN-DNA with a chloride ligand by high-throughput screening. Inclusion of chlorides on AgN-DNAs presents a promising new route to expand the diversity of AgN-DNA structure–property relationships and to imbue these emitters with favorable stability for biophotonics applications.
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American Chemical Society (ACS)ISSN Hae Julkaisufoorumista
0002-7863Asiasanat
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https://converis.jyu.fi/converis/portal/detail/Publication/183126657
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This work was supported by NSF Biophotonics CBET2025790. A.G.-R. acknowledges a Balsells Graduate Fellowship. The computational work was supported by the Academy of Finland and by the Excellence Funding from the JYU rector.Lisenssi
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