Doping as a means to probe the potential dependence of dopamine adsorption on carbon-based surfaces

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dc.contributor Aalto-yliopisto fi
dc.contributor Aalto University en Aarva, Anja Laurila, Tomi Caro, Miguel A. 2018-08-01T12:37:51Z 2018-08-01T12:37:51Z 2017-06-21
dc.identifier.citation Aarva , A , Laurila , T & Caro , M A 2017 , ' Doping as a means to probe the potential dependence of dopamine adsorption on carbon-based surfaces : A first-principles study ' Journal of Chemical Physics , vol 146 , no. 23 , 234704 . DOI: 10.1063/1.4986521 en
dc.identifier.issn 0021-9606
dc.identifier.issn 1089-7690
dc.identifier.other PURE UUID: 09a8f389-fb27-4c3d-bdd9-2bb371557e1d
dc.identifier.other PURE ITEMURL:
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dc.description.abstract In this work, we study the adsorption characteristics of dopamine (DA), ascorbic acid (AA), and dopaminequinone (DAox) on carbonaceous electrodes. Our goal is to obtain a better understanding of the adsorption behavior of these analytes in order to promote the development of new carbon-based electrode materials for sensitive and selective detection of dopamine in vivo. Here we employ density functional theory-based simulations to reach a level of detail that cannot be achieved experimentally. To get a broader understanding of carbonaceous surfaces with different morphological characteristics, we compare three materials: graphene, diamond, and amorphous carbon (a-C). Effects of solvation on adsorption characteristics are taken into account via a continuum solvent model. Potential changes that take place during electrochemical measurements, such as cyclic voltammetry, can also alter the adsorption behavior. In this study, we have utilized doping as an indirect method to simulate these changes by shifting the work function of the electrode material. We demonstrate that sp2- and sp3-rich materials, as well as a-C, respond markedly different to doping. Also the adsorption behavior of the molecules studied here differs depending on the surface material and the change in the surface potential. In all cases, adsorption is spontaneous, but covalent bonding is not detected in vacuum. The aqueous medium has a large effect on the adsorption behavior of DAox, which reaches its highest adsorption energy on diamond when the potential is shifted to more negative values. In all cases, inclusion of the solvent enhances the charge transfer between the slab and DAox. Largest differences in adsorption energy between DA and AA are obtained on graphene. Gaining better understanding of the behavior of the different forms of carbon when used as electrode materials provides a means to rationalize the observed complex phenomena taking place at the electrodes during electrochemical oxidation/reduction of these biomolecules. en
dc.format.mimetype application/pdf
dc.language.iso en en
dc.relation.ispartofseries Journal of Chemical Physics en
dc.relation.ispartofseries Volume 146, issue 23 en
dc.rights openAccess en
dc.subject.other Physics and Astronomy(all) en
dc.subject.other Physical and Theoretical Chemistry en
dc.subject.other 113 Computer and information sciences en
dc.subject.other 114 Physical sciences en
dc.title Doping as a means to probe the potential dependence of dopamine adsorption on carbon-based surfaces en
dc.type A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä fi
dc.description.version Peer reviewed en
dc.contributor.department Department of Electrical Engineering and Automation
dc.contributor.department Department of Applied Physics en
dc.subject.keyword Physics and Astronomy(all)
dc.subject.keyword Physical and Theoretical Chemistry
dc.subject.keyword 113 Computer and information sciences
dc.subject.keyword 114 Physical sciences
dc.identifier.urn URN:NBN:fi:aalto-201808014069
dc.identifier.doi 10.1063/1.4986521
dc.type.version publishedVersion

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