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Assembly of dithiocarbamate-anchored monolayers on gold surfaces in aqueous solutions.

ABSTRACT: Dithiocarbamates (DTCs) can be formed by the in situ condensation of polar alkylamines with CS 2, and assembled into dithiocarbamate-anchored monolayers (DAMs) on Au substrates in aqueous solutions. Primary and secondary amines can both be used to prepare DTCs, but have significant differences in their reactivities and product stabilities. Ultraviolet absorption spectroscopy provides a convenient method for monitoring in situ DTC formation as well as the formation of potential byproducts. The kinetics of DAM assembly on Au substrates as measured by second harmonic generation (SHG) indicated first-order rate processes and saturation coverages similar to those of alkanethiols on Au. However, the rate of adsorption did not change with DTC concentration in a manner expected of Langmuir kinetics, and is attributed to the competitive adsorption of alkylammonium counterions to the freshly oxidized Au substrate. These analyses establish a practical range of conditions for preparing DAMs from polar amines using in situ DTC formation.

SUBMITTER: Zhu H

PROVIDER: S-EPMC2585038 | biostudies-literature | 2008 Aug

REPOSITORIES: biostudies-literature

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Assembly of dithiocarbamate-anchored monolayers on gold surfaces in aqueous solutions.

Zhu Heng H Coleman Donna M DM Dehen Christopher J CJ Geisler Iris M IM Zemlyanov Dmitry D Chmielewski Jean J Simpson Garth J GJ Wei Alexander A

Langmuir : the ACS journal of surfaces and colloids 20080711 16

Dithiocarbamates (DTCs) can be formed by the in situ condensation of polar alkylamines with CS 2, and assembled into dithiocarbamate-anchored monolayers (DAMs) on Au substrates in aqueous solutions. Primary and secondary amines can both be used to prepare DTCs, but have significant differences in their reactivities and product stabilities. Ultraviolet absorption spectroscopy provides a convenient method for monitoring in situ DTC formation as well as the formation of potential byproducts. The ki ...[more]

PMID: 18616309

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Project description:The development of electrochemical multisensor systems is driven by the need for fast, miniature, inexpensive, analytical devices, and advanced interdisciplinary based on both chemometric and (nano)material approaches. A multicomponent analysis of complex mixtures in environmental and technological monitoring, biological samples, and cell culture requires chip-based multisensor systems with high-stability sensors. In this paper, we describe the development, characterization, and applications of chip-based nanoelectrochemical sensor arrays prepared by the directed electrochemical nanowire assembly (DENA) of noble metals and metal alloys to analyze aqueous solutions. A synergic action of the electrode transducer function and electrocatalytic activity of the nanostructured surface toward analytes is achieved in the assembled metal nanowire (NW) sensors. Various sensor nanomaterials (Pd, Ni, Au, and their multicomponent compositions) can be electrochemically assembled on a single chip without employing multiple cycles of photolithography process to realize multi-analyte sensing applications as well as spatial resolution of sensor analysis by this single-chip multisensor system. For multi-analyte electrochemical sensing, individual amperometric signals of two or more nanowires can be acquired, making use of the specific electrocatalytic surface properties of the individual nanowire sensors of the array toward analytes. To demonstrate the application of a new electrochemical multisensor platform, Pd-Au, Pd-Ni, Pd, and Au NW electrode arrays on a single chip were employed for the non-enzymatic analysis of hydrogen peroxide, glucose, and ethanol. The analytes are determined at low absolute values of the detection potentials with linear concentration ranges of 1.0 × 10-6 - 1.0 × 10-3 M (H2O2), 1.5 × 10-7 - 2.0 × 10-3 M (glucose), and 0.7 × 10-3 - 3.0 × 10-2 M (ethanol), detection limits of 2 × 10-7 M (H2O2), 4 × 10-8 M (glucose), and 5.2 × 10-4 M (ethanol), and sensitivities of 18 ?A M-1 (H2O2), 178 ?A M-1 (glucose), and 28 ?A M-1 (ethanol), respectively. The sensors demonstrate a high level of stability due to the non-enzymatic detection mode. Based on the DENA-assembled nanowire electrodes of a compositional diversity, we propose a novel single-chip electrochemical multisensor platform, which is promising for acquiring complex analytical signals for advanced data processing with chemometric techniques aimed at the development of electronic tongue-type multisensor systems for flexible multi-analyte monitoring and healthcare applications.

Dataset Information

Assembly of dithiocarbamate-anchored monolayers on gold surfaces in aqueous solutions.

Publications

Assembly of dithiocarbamate-anchored monolayers on gold surfaces in aqueous solutions.

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