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Enhanced Voltammetric Anion Sensing at Halogen and Hydrogen Bonding Ferrocenyl SAMs

preprint
submitted on 10.11.2020, 22:25 and posted on 12.11.2020, 12:53 by Robert Hein, Xiaoxiong Li, Paul D. Beer, Jason J Davis
Halogen bonding mediated electrochemical anion sensing has very recently been established as a potent platform for the selective and sensitive detection of anions, although the principles that govern binding and subsequent signal transduction remain poorly understood. Herein we address this challenge by providing a comprehensive study of novel redox-active halogen bonding (XB) and hydrogen bonding (HB) ferrocene-isophthalamide-(iodo)triazole receptors in solution and at self-assembled monolayers (SAMs). Under diffusive conditions the sensory performance of the XB sensor was significantly superior. In molecular films the XB and HB binding motifs both display a notably enhanced, but similar, response to specific anions. Importantly, the enhanced response of these films is rationalised by a consideration of the (interfacial) dielectric microenvironment. These effects, and the resolved relationship between anion binding and signal transduction, underpin an improved fundamental understanding of anion sensing at redox-active interfaces which will benefit not just the development of more potent, real-life relevant sensors, but also new tools to study host-guest interactions at interfaces.

History

Email Address of Submitting Author

robert.hein@chem.ox.ac.uk

Institution

University of Oxford

Country

United Kingdom

ORCID For Submitting Author

0000-0001-8567-0924

Declaration of Conflict of Interest

No conflicts of interest

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