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1.
Anal Chem ; 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38848224

RESUMO

Numerous high-performance nanotechnologies have been developed, but their practical applications are largely restricted by the nanomaterials' low stabilities and high operation complexity in aqueous substrates. Herein, we develop a simple and high-reliability hydrogel-based nanotechnology based on the in situ formation of Au nanoparticles in molybdenum disulfide (MoS2)-doped agarose (MoS2/AG) hydrogels for electrophoresis-integrated microplate protein recognition. After the incubation of MoS2/AG hydrogels in HAuCl4 solutions, MoS2 nanosheets spontaneously reduce Au ions, and the hydrogels are remarkably stained with the color of as-synthetic plasmonic Au hybrid nanomaterials (Au staining). Proteins can precisely mediate the morphologies and optical properties of Au/MoS2 heterostructures in the hydrogels. Consequently, Au staining-based protein recognition is exhibited, and hydrogels ensure the comparable stabilities and sensitivities of protein analysis. In comparison to the fluorescence imaging and dye staining, enhanced sensitivity and recognition performances of proteins are implemented by Au staining. In Au staining, exfoliated MoS2 semiconductors directly guide the oriented growth of plasmonic Au nanostructures in the presence of formaldehyde, showing environment-friendly features. The Au-stained hydrogels merge the synthesis and recognition applications of plasmonic Au nanomaterials. Significantly, the one-step incubation of the electrophoretic hydrogels leads to high simplicity of operation, largely challenging those multiple-step Ag staining routes which were performed with high complexity and formaldehyde toxicity. Due to its toxic-free, simple, and sensitive merits, the Au staining integrated with electrophoresis-based separation and microplate-based high-throughput measurements exhibits highly promising and improved practicality of those developing nanotechnologies and largely facilitates in-depth understanding of biological information.

2.
Anal Chem ; 95(51): 18859-18870, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38096265

RESUMO

Trivalent Au ions are easily reduced to be zerovalent atoms by coexisting reductant reagents, resulting in the subsequent accumulation of Au atoms and formation of plasmonic nanostructures. In the absence of stabilizers or presence of weak stabilizers, aggregative growth of Au nanoparticles (NPs) always occurs, and unregular multidimensional Au materials are consequently constructed. Herein, the addition of nanomole-level mercury ions can efficiently prevent the epitaxial accumulation of Au atoms, and separated Au NPs with mediated morphologies and superior plasmonic characteristics are obtained. Experimental results and theoretical simulation demonstrate the Hg-concentration-reliant formation of plasmonic nanostructures with their mediated sizes and shapes in the presence of weak reductants. Moreover, the sensitive plasmonic responses of reaction systems exhibit selectivity comparable to that of Hg species. As a concept of proof, polymeric carbon dots (CDs) were used as the initial reductant, and the reactions between trivalent Au and CDs were studies. Significantly, Hg atoms prevent the epitaxial accumulation of Au atoms, and plasmonic NPs with decreased sizes were in situ synthesized, corresponding to varied surface plasmonic resonance absorption performance of the CD-induced hybrids. Moreover, with the integration of sensing substrates of CD-doped hydrogels, superior response stabilities, analysis selectivity, and sensitivity of Hg2+ ions were achieved on the basis of the mercury-mediated in situ chemical reactions between trivalent Au ions and reductant CDs. Consequently, a high-performance sensing strategy with the use of Au NP-staining hydrogels (nanostaining hydrogels) was exhibited. In addition to Hg sensing, the nanostaining hydrogels facilitated by doping of emerging materials and advanced chem/biostrategies can be developed as high-performance on-site monitoring routes to various pollutant species.

3.
Langmuir ; 39(8): 3052-3061, 2023 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-36787386

RESUMO

The way of accurately regulating the growth of chiral plasmonics is of great importance for exploring the chirality information and improving its potential values. Herein, cysteine enantiomers modulate the anisotropic and epitaxial growth of gold nanoplasmonics on seeds of exfoliated MoS2 nanosheets. The heterostructural Au and MoS2 hybrids induced by enantiomeric cysteine are presented with chiroptical characteristics, dendritic morphologies, and plasmonic performances. Moreover, the synthesis, condition optimization, formation mechanism, and plasmonic properties of Au and MoS2 dendritic nanostructures are studied. The chirality characteristics are identified using the circular dichroism spectra and scanning electron microscopy. Time-resolved transmission electron microscopy and UV-vis spectra of the intermediate products captured are analyzed to confirm the formation mechanism of dendritic plasmonic nanostructures at heterostructural surfaces. The specific dendritic morphologies originate from the synergistic impacts of heterostructural MoS2 interfaces and enantiomeric cysteine-induced anisotropic manipulation. Significantly, the developed synthesis strategy of chiral nanostructures at heterostructural interfaces is highly promising in promoting the understanding of the plasmonic function and crucial chirality bioinformation.

4.
Nat Commun ; 13(1): 7289, 2022 11 26.
Artigo em Inglês | MEDLINE | ID: mdl-36435865

RESUMO

The transfer of the concept of chirality from molecules to synthesized nanomaterials has attracted attention amongst multidisciplinary teams. Here we demonstrate heterogeneous nucleation and anisotropic accumulation of Au nanoparticles on multilayer MoS2 planes to form chiroptically functional nanomaterials. Thiol amino acids with chiral conformations modulate asymmetric growth of gold nanoarchitectures on seeds of highly faceted Au/MoS2 heterostructures. Consequently, dendritic plasmonic nanocrystals with partial chiral morphologies are synthesized. The chirality of dendritic nanocrystals inherited from cysteine molecules refers to the structural characteristics and includes specific recognition of enantiomeric molecules. With integration of the intrinsic photothermal properties and inherited enantioselective characteristics, dendritic Au/MoS2 heterostructures exhibit chirality-dependent release of antimicrobial drugs from hydrogel substrates when activated by exogenous infrared irradiation. A three-in-one strategy involving synthesis of chiral dendritic heterostructures, enantioselective recognition, and controlled drug release system is presented, which improves nanomaterial synthetic technology and enhances our understanding of crucial chirality information.


Assuntos
Anti-Infecciosos , Nanopartículas Metálicas , Ouro/química , Estereoisomerismo , Nanopartículas Metálicas/química , Molibdênio , Anti-Infecciosos/farmacologia
5.
Anal Methods ; 13(45): 5436-5440, 2021 11 25.
Artigo em Inglês | MEDLINE | ID: mdl-34763345

RESUMO

Semiconducting MoS2 layers offer the electrons, reducing conjugated Au(I) to Au atoms, and sebsequently serve as desirable substrates for supporting the interfacial growths of gold nanostructures. Au-covering MoS2 heterostructures perform morphology-varied optical characteristics, and the surface engineering of MoS2 involved by Hg2+ ions results in the differential growths of nanostructures and morphological diversities. Naked-eye colorimetric responses to mercury ions, with a low limit of detection of 1.27 nM, are achieved based on the in situ grown heterostructures.


Assuntos
Mercúrio , Nanopartículas Metálicas , Ouro/química , Íons , Mercúrio/química , Nanopartículas Metálicas/química , Molibdênio/química
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