Fluorescent DNA‐Templated Silver Nanoclusters from Silver(I)‐Mediated Base Pairs

Léon, Jean-Claude; Gonzalez-Abradelo, Dario; Strassert, Cristian A.; Müller, Jens

doi:10.1002/chem.201801858

Cited by 40 publications

(20 citation statements)

References 47 publications

(34 reference statements)

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“…As shown by Müller et al. in 2018, metallo‐base pairing with Ag I in shorter duplex sequences with opposing 6C stretches (or non‐native imidazole groups) can lead to highly fluorescent AgNCs upon reduction …”

Section: Resultsmentioning

confidence: 94%

Formation and Structure of Fluorescent Silver Nanoclusters at Interfacial Binding Sites Facilitating Oligomerization of DNA Hairpins

et al. 2020

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Fluorescent, DNA‐stabilized silver nanoclusters (DNA‐AgNCs) are applied in a range of applications within nanoscience and nanotechnology. However, their diverse optical properties, mechanism of formation, and aspects of their composition remain unexplored, making the rational design of nanocluster probes challenging. Herein, a synthetic procedure is described for obtaining a high yield of emissive DNA‐AgNCs with a C‐loop hairpin DNA sequence, with subsequent purification by size‐exclusion chromatography (SEC). Through a combination of optical spectroscopy, gel electrophoresis, inductively coupled plasma mass spectrometry (ICP‐MS), and small‐angle X‐ray scattering (SAXS) in conjunction with the systematic study of various DNA sequences, the low‐resolution structure and mechanism of the formation of AgNCs were investigated. Data indicate that fluorescent DNA‐AgNCs self‐assemble by a head‐to‐head binding of two DNA hairpins, bridged by a silver nanocluster, resulting in the modelling of a dimeric structure harboring an Ag12 cluster.

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Section: Resultsmentioning

confidence: 94%

Formation and Structure of Fluorescent Silver Nanoclusters at Interfacial Binding Sites Facilitating Oligomerization of DNA Hairpins

et al. 2020

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“…[8] The respective degree of stabilization depends on the chosen nucleobasea nd hence on the typeo fc oordinating metal ion. Severala pplications have been put forward for DNA with metal-mediated base pairs, including metal-responsive structural and catalytic transformations, [9] sensors for metal ions or oligonucleotides, [10] modulation of the charge-transfer capabilities of DNA, [11] generation of metal nanoclusters, [12] and several more. [7a] While even the naturally occurringnucleobases are capable of forming metal-mediated base pairs, [13] the majority of published metal-mediated base pairs contains artificial nucleosides, [8] based on monodentate, [14] bidentate, [15] tridentate [16] or even tetradentate [17] ligands.…”

Section: Introductionmentioning

confidence: 99%

Silver(I) Coordination in Silver(I)‐Mediated Homo Base Pairs of 6‐Pyrazolylpurine in DNA Duplexes Involves the Watson–Crick Edge

Escher

Müller

2020

Chemistry A European J

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DNA duplexes comprising 6-(1H-pyrazol-1-yl)-9Hpurine (6PP), 1-deaza-6PP (1D 6PP), 7-deaza-6PP (7D 6PP) and 1,7-dideaza-6PP (1,7D 6PP) 2'-deoxyribonucleosides, respectively,w ere investigated towards their ability to form metalmediated base pairs in the presenceo fA g I .I n6 PP and 7D 6PP,t he Ag I ion can coordinate to the nucleobase via the endocyclic N1 nitrogena tom, that is, via the Watson-Crick edge. In contrast, this nitrogen atom is not available in 1D 6PP and 1,7D 6PP,s ot hat in 1D 6PP an Ag I coordination is only possible via the Hoogsteen edge (N7). Reference duplexesw ith eithera denine:adenine mispairs or canonical adenine:thymine base pairs were used to investigatet he impact of the pyrazolyl moiety on the Ag I-binding properties. To determine the thermala nd structurald uplex stabilities in the absence or presence of Ag I ,a ll duplexes weree xamined by UV and circulardichroism spectroscopics tudies. These investigations shed light on the questiono fw hether N1-or N7-coordination is preferred in purine-based metal-mediated base pairs.

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“…The duplex structure of DNA also provides a chiral template for the assembly and stabilization of metallic nanoclusters . When thiolated DNA (DNASH) conjugates with silver to form nanoclusters, the resulting conjugates show strong fluorescence emission and extended shelf‐time, which can be used for nuclear imaging .…”

Section: Man‐made Dna Materials For Immunoengineeringmentioning

confidence: 99%

DNA‐Based Biomaterials for Immunoengineering

Maeda

Kojima

Song

et al. 2018

Adv Healthcare Materials

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of extracellular DNA in tissues and in circulation. [5] Extracellular DNA is capable of engaging with the immune system as depicted in Figure 1; therefore, as synthetic DNA-based biomaterials emerge, their potential immune responses must be considered. DNA sensors are mediators of extracellular DNA immune responses observed in vivo, including cyclic guanosine monophosphate-adenosine monophosphate synthase (cGAS) and toll-like receptors (TLRs). Defining novel DNA sensors and their mechanisms is an active area of investigation. [6] Likewise, the structural and chemical properties of DNA that triggers DNA sensors continue to be uncovered. [6] This review summarizes known DNA interaction modalities with the immune system, the sources of extracellular DNA, and, finally, the relevant and emerging biotechnologies that incorporate DNA molecules. A focus is geared toward innate immune responses and doublestranded DNA (dsDNA). Leveraging the immunomodulatory capacity of DNA enables tailoring materials to initiate specific immune outcomes depending on the application, for instance, priming aggressive immune responses for localized tumor-interfacing biomaterials or immunosuppressive functions to prevent chronic inflammation on implant surfaces. Achieving this requires an improved understanding of the DNA properties, such as backbone chemistry, base pair sequence, charge, and length, that can function as design levers for the immune response. The Role of Extracellular DNA in the Immune ResponseThe immune system is designed to protect the host against infections by distinguishing between self-and non-self motifs, and by identifying pathogen and damage signals. Upon recognition of a "non-self" or foreign molecule, an array of effector functions are triggered and orchestrated by immune cells to achieve pathogen clearance and restore homeostasis. [7] These immunoactivating defense mechanisms include the release of proinflammatory cytokines, immune cell recruitment, programmed cell death, and phagocytosis. Ideally, immunoactivating responses are supplanted by immunosuppressive functions once the pathogen or agonist is resolved. This immune resolution is necessary to coordinate healing and anti-inflammatory functions such as diminished chemokine and cytokine secretion, replacement Man-made DNA materials hold the potential to modulate specific immune pathways toward immunoactivating or immunosuppressive cascades. DNAbased biomaterials introduce DNA into the extracellular environment during implantation or delivery, and subsequently intracellularly upon phagocytosis or degradation of the material. Therefore, the immunogenic functionality of biological and synthetic extracellular DNA should be considered to achieve desired immune responses. In vivo, extracellular DNA from both endogenous and exogenous sources holds immunoactivating functions which can be traced back to the molecular features of DNA, such as sequence and length. Extracellular DNA is recognized as damage-associated molecular patterns (DAMPs), or pathogen-associated mole...

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Fluorescent DNA‐Templated Silver Nanoclusters from Silver(I)‐Mediated Base Pairs

Cited by 40 publications

References 47 publications

Formation and Structure of Fluorescent Silver Nanoclusters at Interfacial Binding Sites Facilitating Oligomerization of DNA Hairpins

Formation and Structure of Fluorescent Silver Nanoclusters at Interfacial Binding Sites Facilitating Oligomerization of DNA Hairpins

Silver(I) Coordination in Silver(I)‐Mediated Homo Base Pairs of 6‐Pyrazolylpurine in DNA Duplexes Involves the Watson–Crick Edge

DNA‐Based Biomaterials for Immunoengineering

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