Selective detection of nitroexplosives using molecular recognition within self-assembled plasmonic nanojunctions

Chio, W.-I. K., Peveler, W. J. , Assaf, K. I., Moorthy, S., Nau, W. M., Parkin, I. P., Olivo, M. and Lee, T.-C. (2019) Selective detection of nitroexplosives using molecular recognition within self-assembled plasmonic nanojunctions. Journal of Physical Chemistry C, (doi:10.1021/acs.jpcc.9b02363) (Early Online Publication)

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Abstract

We demonstrate that the reproducibility of sensors for nitroaromatics based on surface-enhanced Raman spectroscopy (SERS) can be significantly improved via a hierarchical aqueous self-assembly approach mediated by the multifunctional macrocyclic molecule cucurbit[7]uril (CB[7]). Our approach is enabled by the novel host–guest complexation between CB[7] and an explosive marker 2,4-dinitrotoluene (DNT). Binding studies are performed using experimental and computation techniques to quantify key binding parameters for the first time. This supramolecular complexation allows DNT to be positioned in close proximity to the plasmonic hotspots within aggregates of CB[7] and gold nanoparticles, resulting in significant SERS signals with a detection limit of ∼1 μM. The supramolecular ensemble is selective against a structurally similar nitroaromatics owing to the molecular-recognition nature of the complexation as well as tolerant against the presence of model organic contaminants that bind strongly to the SERS substrates.

Item Type:Articles
Additional Information:SM and TCL are grateful to the Research Project Grant (RPG2016-393) funded by the Leverhulme Trust. WIKC, IPP, MO, and TCL are grateful to the Studentship funded by the A*STAR-UCL Research Attachment Programme through the EPSRC M3S CDT (EP/L015862/1). WJP acknowledges the University of Glasgow for a Lord Kelvin Adam Smith Fellowship. KIA and WMN thank the DFG for grant NA686/8 within the priority program SPP 1807 “Control of London Dispersion Interactions in Molecular Chemistry”.
Status:Early Online Publication
Refereed:Yes
Glasgow Author(s) Enlighten ID:Peveler, Dr William
Authors: Chio, W.-I. K., Peveler, W. J., Assaf, K. I., Moorthy, S., Nau, W. M., Parkin, I. P., Olivo, M., and Lee, T.-C.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Journal of Physical Chemistry C
Publisher:American Chemical Society
ISSN:1932-7447
ISSN (Online):1932-7455
Published Online:23 April 2019
Copyright Holders:Copyright © 2019 American Chemical Society
First Published:First published in Journal of Physical Chemistry C 2019
Publisher Policy:Reproduced under a Creative Commons License

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