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DNA-Encoded Morphological Evolution of Bimetallic Pd@Au Core-shell Nanoparticles from a High-indexed Core.

ABSTRACT: DNA-mediated synthesis of nanoparticles with different morphologies has proven to be a powerful method to synthesize and access many exclusive shapes and surface properties. While previous studies employ seeds that contain relatively low-energy facets, such as a simple cubic palladium seed in the synthesis of Pd-Au bimetallic nanoparticles, few studies have investigated whether DNA molecules can still exert their influence when the synthesis uses a seed that contains high-energy facets. Seeds that are enclosed by such high-energy facets or sites are known to act as easy nucleation sites in nanoparticles growth and could potentially suppress the effect of DNA. To answer this question, we herein report DNA-encoded control of morphological evolution of bimetallic Pd@Au core-shell nanoparticles from a concave palladium nanocube seed that contains high indexed facets. Based on detailed spectroscopic and SEM studies of time-dependent growth of the bimetallic nanoparticles, we found that each of 10-mer DNA molecules (T10, G10, C10 and A10) has a unique way of interacting with both the seed's surface and the precursor. Among them, the most important factor is the binding affinity of the nucleobase to the Pd surface, with the A10 possessing the highest binding affinity and thus capable of stabilizing the seed's high energy surfaces. Furthermore, for bases with lower binding affinity (T10, G10 and C10) than A10, the growth is completely dictated by the seed's surface energy initially, but the later growth can still be influenced by the different DNA sequences, resulting in four unique morphologically different Pd@Au bimetallic nanoparticles. The effect of these DNA molecules with medium binding affinity can only be observed when there is more deposition of Au. Based on the above results, a scheme for the DNA controlled growth is proposed. Together these results have provided insights into factors governing DNA-mediated growth of core-shell structures using seeds with high-energy sites, and the insights can readily be applied to other bimetallic systems that adopt seed-mediated synthesis.

SUBMITTER: Reddy Satyavolu NS

PROVIDER: S-EPMC6424367 | biostudies-literature | 2018 Sep

REPOSITORIES: biostudies-literature

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DNA-Encoded Morphological Evolution of Bimetallic Pd@Au Core-shell Nanoparticles from a High-indexed Core.

Reddy Satyavolu Nitya Sai NS Pishevaresfahani Nikou N Tan Li Huey LH Lu Yi Y

Nano research 20180327 9

DNA-mediated synthesis of nanoparticles with different morphologies has proven to be a powerful method to synthesize and access many exclusive shapes and surface properties. While previous studies employ seeds that contain relatively low-energy facets, such as a simple cubic palladium seed in the synthesis of Pd-Au bimetallic nanoparticles, few studies have investigated whether DNA molecules can still exert their influence when the synthesis uses a seed that contains high-energy facets. Seeds th ...[more]

PMID: 30906510

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Project description:It is well-known that Ag-Au bimetallic nanoplates have attracted significant research interest due to their unique plasmonic properties and surface-enhanced Raman scattering (SERS). In recent years, there have been many studies on the fabrication of bimetallic nanostructures. However, controlling the shape, size, and structure of bimetallic nanostructures still has many challenges. In this work, we present the results of the synthesis of silver nanoplates (Ag NPls), and Ag-Au bimetallic core/shell and alloy nanostructures, using seed-mediated growth under green LED excitation and a gold salt (HAuCl4) as a precursor of gold. The results show that the optical properties and crystal structure strongly depend on the amount of added gold salt. Interestingly, when the amount of gold(x) in the sample was less than 0.6 μmol (x < 0.6 μmol), the structural nature of Ag-Au was core/shell, in contrast x > 0.6 μmol gave the alloy structure. The morphology of the obtained nanostructures was investigated using the field emission scanning electron microscopy (FESEM) technique. The UV-Vis extinction spectra of Ag-Au nanostructures showed localized surface plasmon resonance (LSPR) bands in the spectral range of 402-627 nm which changed from two peaks to one peak as the amount of gold increased. Ag-Au core/shell and alloy nanostructures were utilized as surface enhanced Raman scattering (SERS) substrates to detect methylene blue (MB) (10-7 M concentration). Our experimental observations indicated that the highest enhancement factor (EF) of about 1.2 × 107 was obtained with Ag-Au alloy. Our detailed investigations revealed that the Ag-Au alloy exhibited significant EF compared to pure metal Ag and Ag-Au core/shell nanostructures. Moreover, the analysis of the data revealed a linear dependence between the logarithm of concentration (log C) and the logarithm of SERS signal intensity (log I) in the range of 10-7-10-4 M with a correlation coefficient (R 2) of 0.994. This research helps us understand better the SERS mechanism and the application of Raman spectroscopy on a bimetallic surface.

Dataset Information

DNA-Encoded Morphological Evolution of Bimetallic Pd@Au Core-shell Nanoparticles from a High-indexed Core.

Publications

DNA-Encoded Morphological Evolution of Bimetallic Pd@Au Core-shell Nanoparticles from a High-indexed Core.

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