Electrocatalytic Mechanism for Improving Sensitivity and Specificity of Electrochemical Nucleic Acid-Based Sensors with Covalent Redox Tags - Part i

Yao Wu, Sufyaan Ali, Ryan J. White

Research output: Contribution to journalArticlepeer-review

Abstract

The design and development of advanced electrocatalysis have been extensively explored for efficient energy conversion and electrochemical biosensing. Both ferricyanide (Fe(CN)63-) and methylene blue (MB) have been widely used in the development of electrochemical biosensing strategies. However, the electrocatalytic mechanism between nucleic acid-tethered MB and Fe(CN)63- remains unexplored. In this manuscript, we aim to provide readers in our community molecular insights into the electrocatalytic mechanism. The exploration of the electrocatalytic mechanism starts with a kinetic zone diagram for a one-electron homogeneous electrocatalytic reaction. Two factors - the excess factor γand the kinetic parameter λ - are important for a homogeneous electrocatalytic reaction; as such, we studied both. The excess factor parameter was controlled by applying Fe(CN)63- with various concentrations (50, 100, and 200 μM), and the kinetic parameter effect on the electrocatalytic process was examined by varying scan rates of cyclic voltammetry (CV) or frequencies of square-wave voltammetry (SWV). Moreover, we discovered that the probe dynamics of the nucleic acid tether is the third rate-limiting factor for the electrocatalytic reaction. As the probe dynamics switch of electrode-bound nucleic acid is often utilized as a mechanism in electrochemical nucleic acid-based sensors, we believe the electrocatalysis between nucleic acid-tethered MB and Fe(CN)63- is capable of enhancing sensitivity and specificity of electrochemical nucleic acid-based sensors with covalent redox tags.

Original languageEnglish (US)
Pages (from-to)3833-3841
Number of pages9
JournalACS sensors
Volume5
Issue number12
DOIs
StatePublished - Dec 24 2020
Externally publishedYes

Keywords

  • electrocatalysis
  • electrochemical nucleic acid-based sensors
  • ferricyanide
  • methylene blue
  • probe dynamics

ASJC Scopus subject areas

  • Bioengineering
  • Instrumentation
  • Process Chemistry and Technology
  • Fluid Flow and Transfer Processes

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