RNA-Mediated Metal-Metal Bond Formation in the Synthesis of Hexagonal Palladium Nanoparticles

Gugliotti, Lina A.; Feldheim, Daniel L.; Eaton, Bruce E.

doi:10.1126/science.1095678

Cited by 190 publications

(181 citation statements)

References 27 publications

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“…11 The silver nanoclusters were synthesized by adding AgNO 3 to the DNA and then adding NaBH 4 , followed by vigorous shaking for 1-2 min. Unless otherwise specified, the concentrations were 15 µM dC 12 , 90 µM Ag + , and 90 µM BH 4 − . The aqueous solutions of NaBH 4 were prepared by dissolving the solid in water and adding the appropriate volume to the DNA/Ag + sample within 30 s. Silver nanoparticles were synthesized following the procedure of Creighton et al 12 Buffers with pH values from 3.0 to 5.5 were prepared using 5 mM formate/formic acid and acetate/acetic acid solutions.…”

Section: Methodsmentioning

confidence: 99%

“…6 In addition, the sequence of the bases and the types of bases can be readily altered to impact on the types of nanoparticles that form. 4 The DNA-mediated synthesis of metal nanostructures is facilitated by the well-known interactions of metal cations with DNA. 7 These bound ions are reduced to form structures that have the form of the template, as illustrated by the synthesis of nanowires.…”

Section: Introductionmentioning

confidence: 99%

“…2 Importantly, the arrangement and types of these binding sites can be altered to affect the selection and synthesis of nanoparticles, and nucleic acids offer important advantages as templates. [3][4][5] The organization of nanoparticles associated with DNA strands is accomplished by using complementary interactions between the bases. 6 In addition, the sequence of the bases and the types of bases can be readily altered to impact on the types of nanoparticles that form.…”

Section: Introductionmentioning

confidence: 99%

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Ag Nanocluster Formation Using a Cytosine Oligonucleotide Template

et al. 2006

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The reduction of silver cations bound to the oligonucleotide dC 12 was used to form silver nanoclusters. Mass spectra show that the oligonucleotides have 2-7 silver atoms that form multiple species, as evident from the number of transitions in the fluorescence and absorption spectra. The variations in the concentrations of the nanoclusters with time are attributed to the changing reducing capacity of the solution, and the formation of oxidized nanoclusters is proposed. Via mass spectrometry and circular dichroism spectroscopy, double-stranded structures with Ag + -mediated interactions between the bases are observed, but these structures are not maintained with the reduced nanoclusters. Through variations in the pH, the nanoclusters are shown to bind with the N3 of cytosine.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Ag Nanocluster Formation Using a Cytosine Oligonucleotide Template

et al. 2006

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“…Experimental strategies are therefore required which enable rapid screening of a potentially vast reaction space. As an elegant approach, DNA-based technologies have been used to evolve libraries of nucleic acids, [ 14 ] short polypeptides [ 15 ] and enzymes [ 16 ] which, when combined with appropriate screening technologies, can be used to identify active biopolymer sequences. However, plate-reader (Figure 1 B).…”

Section: Doi: 101002/adma201403185mentioning

confidence: 99%

Genetic Algorithm‐Guided Discovery of Additive Combinations That Direct Quantum Dot Assembly

et al. 2014

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these techniques are limited by the requirement for complex enzymatic reactions. As an alternative strategy that bypasses the need for genetic engineering, combinatorial methods can be employed. These can be used to explore tens to hundreds of reaction conditions, where the most promising or "lead" conditions may be selected based on the structures or properties of the resultant material. [ 17,18 ] Lead conditions can then be used to narrow the reaction landscape in successive screening rounds. Surprisingly, although combinatorial methods are often used in solid-state chemistry to explore, for example, different reagent compositions, [ 18 ] we are not aware of their use in identifying soluble additives capable of directing mineralization.In this article we demonstrate how combinatorial methods can be used in conjunction with effi cient screening processes to rapidly identify combinations of small organic molecules that are capable of directing the formation of photoluminescent quantum dot minerals in aqueous solution and at room temperature. Indeed, a key feature of biomineralization processes is that control over mineral formation is achieved using many soluble additives that operate in concert. That this feature has seldom been addressed in bioinspired methods is almost certainly due to the vast number of potential variables, which renders a full, systematic exploration intractable. As a solution to this challenge, we here utilize a genetic algorithm as a bioinspired heuristic that mimics natural evolution. Genetic algorithms use selection, recombination, and mutation strategies to rapidly identify and optimize the combination of conditions (here, soluble additives), which gives rise to materials with target properties. [ 19 ] Using a pipetting robot to prepare reaction sets and a UV-light table to rapidly assess the reactions for the formation of photoluminescent minerals, we are able to rapidly identify the key additives that promote the formation of quantum dot superstructures from one-pot aqueous reactions.Our initial library of organic mediators included 23 components, of which 17 were amino acids and 6 were surfactants. Stock solutions of the amino acids were prepared to initial concentrations of 100 × 10 −3 M , and explored at concentrations ranging from 0.01 to 50 × 10 −3 M , while surfactants were prepared to near their solubility limits in water. Surfactants were included as potential structure-directing agents to drive hierarchical assembly in aqueous solution. The overall screening approach used to identify the key additive set is summarized in Figure 1 . First, library amino acids and surfactants were randomly mixed in 48 wells of a multi-well plate, such that each well contained between 1-6 amino acids and 1-3 surfactants (Figure 1 A). Cadmium chloride and thioacetic acid (as a sulfur source) [ 20 ] were then added to a concentration of 1 × 10 −3 M in all wells, as precursors for CdS. After 3 d the plate was viewed under UV illumination (Figure 1 A) and with a fl uorimetric Biomineralization, whi...

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“…In contrast to the wide diversity of biomolecules required for natural biomineralization (13), only short stretches of polypeptides (6,8,10) or polynucleic acids (14) have been systematically searched by genetic screening for defined mineral interactions in vitro. In contrast to load-bearing (4,15) or other material properties (16,17) that are directly selected in nature, laboratory screening has focused on either simple mineral binding (6,8,10) or precipitation (14) as the primary selection criterion. The challenge of engineering increasingly complex biomolecular behavior is critically dependent on the development of laboratory platforms in which genetic information can be expressed and analyzed in new ways.…”

mentioning

confidence: 99%

Evolutionary selection of enzymatically synthesized semiconductors from biomimetic mineralization vesicles

Bawazer

Izumi

Kolodin

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

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The way nature evolves and sculpts materials using proteins inspires new approaches to materials engineering but is still not completely understood. Here, we present a cell-free synthetic biological platform to advance studies of biologically synthesized solid-state materials. This platform is capable of simultaneously exerting many of the hierarchical levels of control found in natural biomineralization, including genetic, chemical, spatial, structural, and morphological control, while supporting the evolutionary selection of new mineralizing proteins and the corresponding genetically encoded materials that they produce. DNA-directed protein expression and enzymatic mineralization occur on polystyrene microbeads in waterin-oil emulsions, yielding synthetic surrogates of biomineralizing cells that are then screened by flow sorting, with light-scattering signals used to sort the resulting mineralized composites differentially. We demonstrate the utility of this platform by evolutionarily selecting newly identified silicateins, biomineralizing enzymes previously identified from the silica skeleton of a marine sponge, for enzyme variants capable of synthesizing silicon dioxide (silica) or titanium dioxide (titania) composites. Mineral composites of intermediate strength are preferentially selected to remain intact for identification during cell sorting, and then to collapse postsorting to expose the encoding genes for enzymatic DNA amplification. Some of the newly selected silicatein variants catalyze the formation of crystalline silicates, whereas the parent silicateins lack this ability. The demonstrated bioengineered route to previously undescribed materials introduces in vitro enzyme selection as a viable strategy for mimicking genetic evolution of materials as it occurs in nature. directed evolution | in vitro compartmentalization | DNA shuffling | metal oxide nanoparticles | self-assembly

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RNA-Mediated Metal-Metal Bond Formation in the Synthesis of Hexagonal Palladium Nanoparticles

Cited by 190 publications

References 27 publications

Ag Nanocluster Formation Using a Cytosine Oligonucleotide Template

Ag Nanocluster Formation Using a Cytosine Oligonucleotide Template

Genetic Algorithm‐Guided Discovery of Additive Combinations That Direct Quantum Dot Assembly

Evolutionary selection of enzymatically synthesized semiconductors from biomimetic mineralization vesicles

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