Dynamic combinatorial chemistry on a monolayer protected gold nanoparticle

Abstract

Here, we show that the addition of Hg(2+) or Ag(+) metal ions to a dynamic system composed of monolayer protected gold nanoparticles (Au NPs) and a mixture of four nucleotides (dGMP, dAMP, TMP, and dCMP) leads to the self-selection of TMP or dGMP, respectively, on the monolayer surface.

A modular self-assembled sensing system for heavy metal ions with tunable sensitivity and selectivity

“…Previously, we exploited a dynamic combinatorial approach for the target driven self-selection of recognition units on the surface of Au NP 1. 28 In line with the approach described above, the ability of target metal ions to induce the clustering of receptor units led to an accumulation of only those receptor units on the monolayer surface that are able to complex the added analyte. Thus, the addition of Hg 2+ to a mixture of 4 nucleotides (dAMP, dGMP, TMP, and dCMP) resulted in the self-selection of TMP as the optimal recognition element for Hg 2+ metal ions.…”

“…The anionic probe A was selected because of the following reasons: i) the high quantum yield of coumarin343 (λ ex = 445 nm; λ em = 493 nm) is advantageous for creating a response even at low concentrations, ii) the carboxylate-probe is readily displaced by phosphate competitors, and iii) the fluorescence properties of the probe are not affected by the analytes. 28 The detection range for TDP and cTMP separately was determined by measuring the fluorescence intensity after the addition of increasing amounts of Hg 2+ to a buffered aqueous solution containing Au NP 1 ([TACN•Zn 2+ ] = 20 ± 1 μM), A (7.3 μM) and either TDP (16 μM) or cTMP (800 μM). A much higher concentration of cTMP was used compared to TDP, because a much higher concentration of the cTMP•Hg 2+ •cTMP complex is required to elicit a displacement of probe A from Au NP 1.…”

“…In addition, this work provides a relevant implementation of our recently developed protocol for dynamic combinatorial chemistry (DCC) on a multivalent nanoparticle surface. 28…”

Manipulating the Monolayer: Responsive and Reversible Control of Colloidal Inorganic Nanoparticle Properties

“…Switching betweent he sorted and unsorted states was achievedb yr emoval and addition of Zn 2 + ,w hile specific stimuli could trigger sequential release of the probes from their respective NP-hosts.I nr elated work, complexation to AuNP-6·Zn 2 + has been used for the dynamic combinatorial identification of metal-linked bis-nucleotide dimers from ap ool of lower-affinity monomers, which could be developed either as am etal sensing platform, or for identifying optimal metal-bindingn ucleotide ligands. [33] ChemNanoMat 2016, 2,87-98 www.chemnanomat.org Nonbiomolecular systemso ffer several advantages over oligonucleotides in terms of structural simplicity,a daptability of molecular design and synthetic routes, anda pplicability under aw ider range of environmental conditions. These pioneering designsa re slowly closing the gap on the exquisite specificity, selectivity and kinetic tunability exhibited by DNA-functionalized NPs, but in only ah andful of cases is binding strong enough that property changes can be achieved and maintained independento fa nu nbounde xcess of reagent.…”

Sequence Adaptive Peptide–Polysaccharide Nanostructures by Biocatalytic Self-Assembly

“…[11][12][13][14] In this approach, building blocks with exchangeable components are formed through reversible interactions to create a dynamic mixture. [15][16][17] Molecular recognition and assembly between these building blocks (or with externally added templates) then give rise to autonomous optimization of the noncovalent interactions, i.e.…”