H<sub>2</sub>O<sub>2</sub> Detection at Carbon Nanotubes
and Nitrogen-Doped Carbon Nanotubes: Oxidation, Reduction, or Disproportionation?
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Abstract
The electrochemical behavior of hydrogen
peroxide (H<sub>2</sub>O<sub>2</sub>) at carbon nanotubes (CNTs) and
nitrogen-doped carbon
nanotubes (N-CNTs) was investigated over a wide potential window.
At CNTs, H<sub>2</sub>O<sub>2</sub> will be oxidized or reduced at
large overpotentials, with a large potential region between these
two processes where electrochemical activity is negligible. At N-CNTs,
the overpotential for both H<sub>2</sub>O<sub>2</sub> oxidation and
reduction is significantly reduced; however, the reduction current
from H<sub>2</sub>O<sub>2</sub>, especially at low overpotentials,
is attributed to increased oxygen reduction rather than the direct
reduction of H<sub>2</sub>O<sub>2</sub>, due to a fast chemical disproportionation
of H<sub>2</sub>O<sub>2</sub> at the N-CNT surface. Additionally,
N-CNTs do not display separation between observable oxidation and
reduction currents from H<sub>2</sub>O<sub>2</sub>. Overall, the analytical
sensitivity of N-CNTs to H<sub>2</sub>O<sub>2</sub>, either by oxidation
or reduction, is considerably higher than CNTs, and obtained at significantly
lower overpotentials. N-CNTs display an anodic sensitivity and limit
of detection of 830 mA M<sup>–1</sup> cm<sup>–2</sup> and 0.5 μM at 0.05 V, and a cathodic sensitivity and limit
of detection of 270 mA M<sup>–1</sup> cm<sup>–2</sup> and 10 μM at −0.25 V (V vs Hg/Hg<sub>2</sub>SO<sub>4</sub>). N-CNTs are also a superior platform for the creation of
bioelectrodes from the spontaneous adsorption of enzyme, compared
to CNTs. Glucose oxidase (GOx) was allowed to adsorb onto N-CNTs,
producing a bioelectrode with a sensitivity and limit of detection
to glucose of 80 mA M<sup>–1</sup> cm<sup>–2</sup> and
7 μM after only 30 s of adsorption time from a 81.3 μM
GOx solution