Voltammetric kinetic discrimination of two sequential proton-coupled electron transfers in serotonin oxidation: Electrochemical interrogation of a serotonin intermediate
- Authors
- Yeo, Jeongmin; Chang, Jinho
- Issue Date
- Mar-2022
- Publisher
- Elsevier Ltd
- Keywords
- A serotonin radical intermediate; Proton coupled electron transfer; Serotonin; Voltammetric kinetic discrimination
- Citation
- Electrochimica Acta, v.409, pp.1 - 15
- Indexed
- SCIE
SCOPUS
- Journal Title
- Electrochimica Acta
- Volume
- 409
- Start Page
- 1
- End Page
- 15
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/139352
- DOI
- 10.1016/j.electacta.2022.139973
- ISSN
- 0013-4686
- Abstract
- An understanding of the electrochemical mechanism involved in serotonin oxidation is critical to the development of accurate sensing applications. Electrochemical signals of a reactive serotonin intermediate can reveal detailed mechanistic information. Here, oxidation of a serotonin radical intermediate, SH∙, is electrochemically interrogated in a buffered system at a neutral pH by voltammetric kinetic discrimination (VKD). At a low scan rate of 0.02 V/s, the voltammogram showed one oxidation peak that can be attributed to electro-oxidation of serotonin with two proton-coupled electron transfers (PCETs) in the absence of voltammetric resolution. This corresponds to the inherent thermodynamic instability of a reactive serotonin intermediate, leading to potential inversion in two sequential PCETs. However, at a scan rate of 1 V/s, the single voltammetric peak gradually resolved into two, each of which are associated with sequential electro-oxidation of serotonin via 1e−-1H+. The peak resolution originated from kinetic discrimination between the first and second PCET in serotonin oxidation; the first PCET step is Nernstian, while the second is electrochemically irreversible. The observed VKD in electro-oxidation of serotonin can be explained by voltammetric simulations.
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