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Revisiting the factors influencing gold electrodes prepared using cyclic voltammetry
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.ORCID-id: 0000-0003-3843-7198
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.ORCID-id: 0000-0003-4764-1246
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.ORCID-id: 0000-0003-2417-274X
Vise andre og tillknytning
2019 (engelsk)Inngår i: Sensors and actuators. B, Chemical, ISSN 0925-4005, E-ISSN 1873-3077, Vol. 283, s. 146-153Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

Gold is widely used as the electrode material in different chemi- and biosensing applications while cyclic voltammetry (CV) in sulfuric acid solutions is a commonly employed method for gold surface preparation and characterization. However, as shown herein, chloride leakage from the Ag/AgCl/sat. KCl reference electrode and platinum dissolution from the platinum counter electrode can severely compromise the reproducibility and hence the reliability of the prepared gold electrodes. The aim of this work is to obtain a comprehensive understanding of the separate and interdependent effects of the aforementioned factors on the voltammetric behavior of microfabricated polycrystalline gold electrodes. It is shown that the leakage of chloride gives rise to etching of both the gold working and the platinum counter electrodes and that the chloride concentration has a strong influence on the ratio between the obtained gold and platinum concentrations in the electrolyte. The dissolved gold and platinum are then re-deposited on the gold electrode on the cathodic voltammetric scan, changing the structure and properties of the electrode. It is also demonstrated that the changes in the properties of the gold electrode are determined by the ratio between the co-deposited platinum and gold rather than the absolute amount of platinum deposited on the gold electrode. In addition, the chloride and sulfate adsorption behavior on the gold electrode is carefully investigated. It is proposed that redox peaks due to the formation ofthe corresponding Au(I) complexes can be seen in the double layer region of the voltammogram. The results show that the chloride leakage from the reference electrode needs to be carefully controlled and that platinum counter electrodes should be avoided when developing gold sensing electrodes. The present comprehensive understanding of the electrochemical performance of gold electrodes prepared using CV should be of significant importance in conjunction with both fundamental investigations and practical applications.

sted, utgiver, år, opplag, sider
2019. Vol. 283, s. 146-153
Emneord [en]
gold electrode, cyclic voltammetry, platinum, electrde etching, chloride leakage, Au(I) complexes
HSV kategori
Forskningsprogram
Kemi med inriktning mot oorganisk kemi; Teknisk fysik med inriktning mot fasta tillståndets fysik
Identifikatorer
URN: urn:nbn:se:uu:diva-372135DOI: 10.1016/j.snb.2018.12.008ISI: 000455854000018OAI: oai:DiVA.org:uu-372135DiVA, id: diva2:1275405
Forskningsfinansiär
Swedish Foundation for Strategic Research , ICA 12-0047Swedish Foundation for Strategic Research , FFL15-0174Swedish Research Council, 2014-5588Wallenberg Foundations, Academy FellowTilgjengelig fra: 2019-01-06 Laget: 2019-01-06 Sist oppdatert: 2020-01-08bibliografisk kontrollert
Inngår i avhandling
1. Interface Studies for Gold-based Electrochemical DNA Sensors
Åpne denne publikasjonen i ny fane eller vindu >>Interface Studies for Gold-based Electrochemical DNA Sensors
2019 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

Gold based label-free electrochemical DNA sensors have been widely studied for biomarker diagnostics. The sensitivity and reproducibility of these sensors are determined by the sensing interface: the DNA modified gold surfaces. This thesis systematically studies the preparation processes of the DNA sensor interfaces as well as their effects on the sensor performance. First, three pretreatment methods to clean the gold electrode surface and their influence on the subsequent binding of thiolated molecules were carefully investigated. As we found that the surface pretreatment method involving cyclic voltammetry (CV) in H2SO4 may induce structural changes to the gold surface, thus greatly impacting the thiolated molecule binding, the factors influencing this pretreatment method were studied. Practical guidelines were summarized for preparing a clean and reproducible gold surface prior to functionalization. Afterwards, the effects of the surface coverage density of probe DNA and the salt concentration on the probe-target DNA hybridization on a gold sensing surface were systematically investigated using surface plasmon resonance (SPR) analysis. Based on the SPR results, the maximum potentiometric signal that could be generated by the DNA hybridization on the surface, and the detection limits, were estimated for different experimental conditions. These estimations were further compared with experimental results obtained using silicon nanowire field effect transistors (SiNW FET) with DNA modified gold on the gate oxide. Practical limitations for the potentiometric DNA sensor were analysed and discussed. Finally, the stability and reproducibility issues on the electrochemical impedance spectroscopy (EIS) analyses of DNA hybridization were also studied on the aptamer/mercaptohexanol (MCH)-modified gold surface. The root cause for the drift problems in this type of sensor and the temperature effects on the aptamer/MCH modified surface were identified. This thesis could serve as a practical reference for the preparation and understanding of the sensing interface of gold-based electrochemical DNA sensors.

sted, utgiver, år, opplag, sider
Uppsala: Acta Universitatis Upsaliensis, 2019. s. 83
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1882
HSV kategori
Identifikatorer
urn:nbn:se:uu:diva-397807 (URN)978-91-513-0824-1 (ISBN)
Disputas
2020-01-20, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2019-12-18 Laget: 2019-11-25 Sist oppdatert: 2020-01-14

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