Anion-Binding-Induced Electrochemical Signal Transduction in Ferrocenylimidazolium: Combined Electrochemical Experimental and Theoretical Investigation.

Tan-Qing Weng,Shan Jin,Lou-Sha Xue,Jie Cheng,Sheng-Hua Liu,De-Yin Wu,Yi-Fan Huang,George Chen

doi:10.3390/molecules24020238

Abstract

Five ferrocene alkymethylimidazolium cations 1a–1d and 2 with different alkyl spacer lengths were reinvestigated using voltammetry and density functional theory (DFT) calculations. The voltammetric responses of ligand 2 toward various anions are described in detail. An interesting and unprecedented finding from both experimental and theoretical studies is that coupled electron and intramolecular anion (F−) transfer may be present in these molecules. In addition, it was also observed that, in these studied molecules, the electrostatic attraction interaction toward F− would effectively vanish beyond 1 nm, which was previously reported only for cations.

Highlights

Non-covalent interactions are present in various modified and finely tuned forms in nature.As a primary example, electrostatic interactions play the decisive role in a range of intra- and intermolecular phenomena in the biological world [1,2,3]
To focus the research effort on the understanding of electrostatic communications involving anionic guests, we propose to use a series of host molecules in which the ferrocene is linked to the anionic guests, we propose to use a series of host molecules in which the ferrocene is linked to the imidazolium receptor via an alkyl chain of various lengths
An interesting derivation is that the electrochemical oxidation of the Fc center is coupled with an intramolecular F− transfer from the imidazolium cation toward the Fc+ center in short alkyl-linked mono-ferrocene imidazolium cations

Summary

Introduction

Electrostatic interactions play the decisive role in a range of intra- and intermolecular phenomena in the biological world [1,2,3]. Such interactions, depending on their strength and direction, could direct protein folding, binding, flexibility, stability, and functions. They are the main driving forces for signaling in biomacromolecules and supramolecules. Existing techniques and devices are not yet able to effectively and accurately detect such antigen-antibody recognition signals, hindering high-quality healthcare

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Conclusion