4.8 Article

Chloride Ligands on DNA-Stabilized Silver Nanoclusters

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 19, 页码 10721-10729

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c01366

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DNA-stabilized silver nanoclusters (AgN-DNAs) can possess additional chloride ligands, which increase their stability in biologically relevant concentrations of chloride. This finding provides a new route to expand the structure-property relationships of AgN-DNAs and to enhance their stability for biophotonics applications.
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 spectrom-etry 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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