Thiolated DNA-templated silver nanoclusters with strong fluorescence emission and a long shelf-life

Zhang, Xiaohong; Qian, Yunxia; Ma, Xuejuan; Xia, Mengfan; Li, Shuangqin; Zhang, Yaodong

doi:10.1039/c7nr06358j

Cited by 26 publications

(6 citation statements)

References 39 publications

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“…Ultra-tiny monolayer ligand-protected noble metal nanoclusters usually have precise atom arrangement, and they attract much attention in different research fields due to the size-related optical, , electronic, and catalytic properties. − Among the metals, Pd is an important precious metal with wide applications in catalysis. However, compared to extensively studied gold, , silver, , and copper , clusters, studies on Pd nanoclusters (Pd NCs) are still scarce, partly due to the lack of effective synthesis processes to lower the core size.…”

Section: Introductionmentioning

confidence: 99%

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

Zhuang

Yang

Chen

2019

ACS Sustainable Chem. Eng.

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Palladium has aroused multitudinous concerns in recent years because of its highly catalytic activity with applications in many reactions. However, the synthesis of atomically precise Pd nanoclusters (Pd NCs) under mild conditions is still challenging. Here, a new facile method is developed to synthesize subnanometer-sized Pd clusters with the molecular formula of Pd6(C12H25S)11 under very mild conditions. The composition, morphology, and optical properties of the Pd6 clusters are characterized by MS, XPS, HRTEM, FT-IR, and UV–vis spectroscopy. The Pd NCs loaded on carbon black show an ultrahigh catalytic activity for the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). After annealing treatment, the Pd NCs can catalyze the reduction of 4-NP to 4-AP with a 100% conversion in only 0.5 min, which is the highest efficiency so far among the reported Pd-based catalysts. The significantly enhanced catalytic activity can be ascribed to the large fraction of Pd atoms on the surface of subnanoclusters with low coordination and the clean surface after the removal of ligands. The present work not only provides a facile method for synthesizing ultrasmall metal clusters but also indicates that subnanometer-sized Pd clusters can be used as highly efficient catalyst for the degradation of environmental pollutants.

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Section: Introductionmentioning

confidence: 99%

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

Zhuang

Yang

Chen

2019

ACS Sustainable Chem. Eng.

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“…Various techniques have been developed for the synthesis of stable, water‐soluble silver NCs by using dendrimers, polymers, polypeptides, thiols, DNA, thiolated DNA, and other ligands to stabilize silver ions . The influence of various thiolates on binding energy with silver NCs has been studied in details .…”

Section: Introductionmentioning

confidence: 99%

Predicting absorption spectra of silver‐ligand complexes

Buglak

Pomogaev

Kononov

2019

Int J of Quantum Chemistry

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The detailed structures of most of ligand-stabilized metal nanoclusters (NCs) remain unknown due to the absence of crystal structure data for them. In such a situation, quantum-chemical modeling is of particular interest. We compared the performance of different theoretical methods of geometry optimization and absorption spectra calculation for silver-thiolate complexes. We showed that the absorption spectra calculated with the ADC(2) method were consistent with the spectra obtained with CC2 method. Three DFT functionals (B3LYP, CAM-B3LYP, and M06-2X) failed to reproduce the CC2 absorption spectra of the silver-thiolate complexes. K E Y W O R D SADC(2), CAM-B3LYP, CC2, M062X, silver nanoclusters, silver-thiolate complexes, TDDFT | INTRODUCTIONLigand protected metal nanoclusters (NCs) have gained much attention in the last decade due to their unique physicochemical properties. These metal NCs typically measure less than 2 nm. [1,2] Electronic, chemical, and optical properties of NCs differ from both bulk and atomic scale materials. Optically active NCs may possess strong visible or near infrared luminescence, [3] which can be used in various applications, such as bioimaging, biosensing, and optical detection of biomolecules. [4] Among the great variety of NCs, gold (Au) NCs are the most extensively investigated due to their chemical stability. [5] However, fluorescent silver (Ag) clusters are the brightest, exhibiting high quantum yield and large absorption cross-section. [6] Various techniques have been developed for the synthesis of stable, water-soluble silver NCs by using dendrimers, [7] polymers, [8] polypeptides, [9,10] thiols, [11] DNA, [12,13] thiolated DNA, [14] and other ligands to stabilize silver ions. [15] The influence of various thiolates on binding energy with silver NCs has been studied in details. [16] The nature of the ligand seems to have a strong effect on fluorescent properties of noble metal NCs. [17] Noble metal NCs protected with thiolate ligands have been of interest because of their long-term stability, which allows one to use them as building blocks constructing assembled systems with novel and improved functions. [2] Silver-thiolate and silver-amino acid complexes are studied in many laboratories nowadays both theoretically and experimentally. [18][19][20] It is assumed that silver nanoclusters are stabilized by cysteine residues in protein matrices. [21,22] While the composition of the ligand-protected NCs can be analyzed using mass-spectroscopy technique, [23] their detailed structures remain unknown in many cases. In this respect, quantum-chemical modeling of silver-ligand complexes is of particular interest. [24][25][26][27][28][29][30][31][32] Gell and coworkers investigated thiolate-protected silver NCs that contained zero, two, or four confined electrons in the cluster core. [33] They found that the number of confined electrons determine the spectroscopic patterns. For systems with two or four confined electrons, strong absorption and fluorescence in the visible or even IR energ...

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“…The binding between plasmid DNA and DTT–Au NCs can be characterized by agarose gel electrophoresis, where free DNA gradually decreased following the increase of the content of DTT–Au NCs (Figure c,d). Notably, there existed strong affinity between DNA and transition metals, particularly gold . This supramolecular force possibly played an important role in generating raspberry‐like DTT–Au NCs@DNA structure ( Figure c).…”

Section: Resultsmentioning

confidence: 99%

DTT–Au NCs Interact with DNA to Form Raspberry‐Like Particles

Zhang

Jing

et al. 2019

Part & Part Syst Charact

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Noble metal nanoclusters (NCs) have emerged as intriguing nanomaterials with widespread interest. Previously, it was shown that dithiothreitol (DTT)‐conjugated gold nanoclusters (Au NCs) respond to copper ions in aqueous solution. Here, it is shown that these DTT–Au NCs can interact with DNA by forming raspberry‐like particles. The raspberry‐like structures protect the capped DNA from enzymatic attack and show excellent biocompatibility. Moreover, these supramolecular complexes cross the plasma membrane of yeast cells and express green fluorescent protein encoded by the DNA, suggesting that DTT–Au NCs can serve as an efficient carrier for gene delivery.

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Thiolated DNA-templated silver nanoclusters with strong fluorescence emission and a long shelf-life

Abstract: Thiolated DNA (DNA-SH) was employed as a template in the synthesis and stabilization of AgNCs (DNA-SH-AgNCs). Resulting from the synergistic protective effect of specific Ag-DNA interactions and Ag-S bonding, DNA-SH-AgNCs exhibited high quantum yields and resistance to oxidation.

Cited by 26 publications

References 39 publications

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

Predicting absorption spectra of silver‐ligand complexes

DTT–Au NCs Interact with DNA to Form Raspberry‐Like Particles

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Thiolated DNA-templated silver nanoclusters with strong fluorescence emission and a long shelf-life

Abstract: Thiolated DNA (DNA-SH) was employed as a template in the synthesis and stabilization of AgNCs (DNA-SH-AgNCs). Resulting from the synergistic protective effect of specific Ag-DNA interactions and Ag-S bonding, DNA-SH-AgNCs exhibited high quantum yields and resistance to oxidation.

Cited by 26 publications

References 39 publications

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd6(C12H25S)11 Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd6(C12H25S)11 Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

Predicting absorption spectra of silver‐ligand complexes

DTT–Au NCs Interact with DNA to Form Raspberry‐Like Particles

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Product

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One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction

One-Step Rapid and Facile Synthesis of Subnanometer-Sized Pd₆(C₁₂H₂₅S)₁₁ Clusters with Ultra-High Catalytic Activity for 4-Nitrophenol Reduction