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Tailoring the electrochemical properties of 2D-hBN via physical linear defects: physicochemical, computational and electrochemical characterisation

García-Miranda Ferrari, Alejandro, Brownson, Dale AC, Abo Dena, Ahmed S, Foster, Christopher W, Rowley-Neale, Samuel J ORCID logoORCID: https://orcid.org/0000-0002-3741-4050 and Banks, Craig E ORCID logoORCID: https://orcid.org/0000-0002-0756-9764 (2019) Tailoring the electrochemical properties of 2D-hBN via physical linear defects: physicochemical, computational and electrochemical characterisation. Nanoscale Advances, 2 (1). pp. 264-273.

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Abstract

Monolayer hexagonal-boron nitride films (2D-hBN) are typically reported within the literature to be electrochemically inactive due to their considerable band gap (ca. 5.2–5.8 eV). It is demonstrated herein that introducing physical linear defects (PLDs) upon the basal plane surface of 2D-hBN gives rise to electrochemically useful signatures. The reason for this transformation from insulator to semiconductor (inferred from physicochemical and computational characterisation) is likely due to full hydrogenation and oxygen passivation of the boron and/or nitrogen at edge sites. This results in a decrease in the band gap (from ca. 6.11 to 2.36/2.84 eV; theoretical calculated values, for the fully hydrogenated oxygen passivation at the N or B respectively). The 2D-hBN films are shown to be tailored through the introduction of PLDs, with the electrochemical behaviour dependent upon the surface coverage of edge plane-sites/defects, which is correlated with electrochemical performance towards redox probes (hexaammineruthenium(III) chloride and Fe2+/3+) and the hydrogen evolution reaction. This manuscript de-convolutes, for the first time, the fundamental electron transfer properties of 2D-hBN, demonstrating that through implementation of PLDs, one can beneficially tailor the electrochemical properties of this nanomaterial

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