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Facet-resolved electrochemistry of polycrystalline boron-doped diamond electrodes : microscopic factors determining the aqueous solvent window in aqueous potassium chloride solutions
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Liu, Danqing, Chen, Chang-Hui, Perry, David, West, Geoffrey D., Cobb, Sam, Macpherson, Julie V. and Unwin, Patrick R. (2018) Facet-resolved electrochemistry of polycrystalline boron-doped diamond electrodes : microscopic factors determining the aqueous solvent window in aqueous potassium chloride solutions. ChemElectroChem . doi:10.1002/celc.201800770 (In Press)
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Official URL: https://doi.org/10.1002/celc.201800770
Abstract
A systematic examination of the microscopic factors affecting the aqueous solvent (electrolyte) window of polycrystalline (p) boron-doped diamond (BDD) electrodes in chloride-containing salt solutions is undertaken using scanning electrochemical cell microscopy (SECCM), in conjunction with electron backscatter diffraction (EBSD) and Raman microscopy. A major focus is to determine the effect of local boron doping level, within the same orientation grains, on the solvent window response. EBSD is used to select the predominant (110) orientated areas of the surface with different boron-doped facets, thereby eliminating crystallographic effects from the electrochemical response. Voltammetric SECCM is employed, whereby a cyclic voltammogram (CV) is recorded at each pixel mapped by the meniscus-contact SECCM cell. The data obtained can be played as an electrochemical movie of potential-resolved current maps of the surface to reveal spatial variations of electroactivity, over a wide potential range, including the solvent (electrolyte) window. Local heterogeneities are observed, indicating that the solvent window is mainly linked to local dopant levels, with lower dopant levels leading to a wider window, i.e. slower electrode kinetics for solvent/electrolyte electrolysis. Furthermore, the effects of O- and H-surface termination of the BDD surface are investigated, for the same electrode (in the same area). The surface termination is a particularly important factor: the solvent window of an H-terminated surface is wider than for O-termination for similar boron dopant levels. Further, the anodic potential window of the O-terminated surface is greatly diminished due to chloride electro-oxidation. These studies provide new perspectives on the local electrochemical properties of BDD and highlight the importance of probing the electrochemistry of BDD at the level of a single crystalline grain (facet) in order to unravel the factors that control the solvent (aqueous) window of these complex heterogeneous electrodes.
| Item Type: | Journal Article | ||||||||||||||||||||||||
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| Subjects: | Q Science > QD Chemistry | ||||||||||||||||||||||||
| Divisions: | Faculty of Science > Chemistry | ||||||||||||||||||||||||
| Library of Congress Subject Headings (LCSH): | Electrodes -- Materials, Electrochemistry, Diamonds -- Electric properties, Boron -- Electric properties, Doped semiconductors, Potassium chloride, Scanning electrochemical microscopy, Electrons -- Backscattering | ||||||||||||||||||||||||
| Journal or Publication Title: | ChemElectroChem | ||||||||||||||||||||||||
| Publisher: | Wiley - V C H Verlag GmbH & Co. KGaA | ||||||||||||||||||||||||
| ISSN: | 2196-0216 | ||||||||||||||||||||||||
| Official Date: | 6 August 2018 | ||||||||||||||||||||||||
| Dates: |
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| Date of first compliant deposit: | 8 October 2018 | ||||||||||||||||||||||||
| DOI: | 10.1002/celc.201800770 | ||||||||||||||||||||||||
| Status: | Peer Reviewed | ||||||||||||||||||||||||
| Publication Status: | In Press | ||||||||||||||||||||||||
| Publisher Statement: | This is the peer reviewed version of the following article: Liu, D. , Chen, C. , Perry, D. , West, G. , Cobb, S. J., Macpherson, J. V. and Unwin, P. R. (2018), Facet‐Resolved Electrochemistry of Polycrystalline Boron‐Doped Diamond Electrodes: Microscopic Factors Determining the Solvent Window in Aqueous Potassium Chloride Solutions. ChemElectroChem. . doi:10.1002/celc.201800770, which has been published in final form at https://doi.org/10.1002/celc.201800770. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. | ||||||||||||||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||||||||||||||||||
| RIOXX Funder/Project Grant: |
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