Electrochemical sensor for arsenite detection using graphene oxide assisted generation of prussian blue nanoparticles as enhanced signal label

• Published in: Analytica chimica acta 2018-03, Vol.1002, p.82-89
• Main Authors: Wen, Shao-Hua, Wang, Yi, Yuan, Yan-Hong, Liang, Ru-Ping, Qiu, Jian-Ding
• Format: Article
• Language: English
• Subjects: Adsorption; Arsenite; Biosensors; Chemical sensors; Conformational change; Electrochemical sensor; Electrochemistry; Electrodes; Gold; Graphene; Graphene oxide; Heavy metals; Hydrogen bonding; Hydrogen bonds; Metal ions; Nanoparticles; Pigments; Prussian blue; Self-assembly; ssDNA; Water analysis; Water sampling
• ISSN: 0003-2670; 1873-4324
• DOI: 10.1016/j.aca.2017.11.057

An electrochemical sensor was fabricated for arsenite detection using graphene oxide-assisted generation of prussian blue nanoparticles as enhanced redox signal label. The 5′-thiolate-labeled (GT)21-ssDNA was first self-assembled on a gold electrode surface via Au-S bond. Graphene oxide can interact with ssDNA through π-π stacking interaction and facilitate the generation of prussian blue nanoparticles on its surface as an electrochemically active indicator. In the absence of arsenite, plenty of graphene oxide/prussian blue nanoparticles can be adsorbed on the electrode surface to produce a stronger redox signal of prussian blue nanoparticles. While in the presence of arsenite, (GT)21-ssDNA can recognize and combine with arsenite via hydrogen bonds to form (GT)21-ssDNA/arsenite complex with a frizzy structure. The conformational change of (GT)21-ssDNA led to less adsorption of graphene oxide/prussian blue nanoparticles on the electrode surface, resulting in a reduced redox response. The arsenite-induced (GT)21-ssDNA structure switching can be used for sensitive detection of arsenite with a linear range from 0.2 to 500 ppb and a detection limit down to 0.058 ppb. Benefiting from (GT)21-ssDNA containing arsenite recognition sequence, the proposed sensor exhibited excellent specificity against other heavy metal ions. The applicability of the electrochemical biosensor for arsenite assay in real water samples demonstrated the great potential of this strategy for trace arsenite detection in environment. [Display omitted] Schematic illustration of the sensor fabrication process and the generation of prussian blue nanoparticles on graphene oxide sheets used as electrochemical signal label for As(III) detection. •Graphene oxide was used as supporting matrix for the in-situ generation of PB NPs.•Adsorption of GO on ssDNA can be regulated by As(III)-induced conformational change of (GT)21-ssDNA.•A sensor for As(III) detection was designed using GO-assisted generation of PB NPs as enhanced signal label.•The sensor showed high sensitivity for As(III) with a detection limit of 0.058 ppb.•The biosensor can be used for selective detection of As(III) in real water samples.