Mcguire, K. et al. (2023) Supramolecular click chemistry for surface modification of quantum dots mediated by Cucurbit[7]uril. ACS Nano, 17(21), pp. 21585-21594. (doi: 10.1021/acsnano.3c06601) (PMID:37922402)
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Abstract
Cucurbiturils (CBs), barrel-shaped macrocyclic molecules, are capable of self-assembling at the surface of nanomaterials in their native state, via their carbonyl-ringed portals. However, the symmetrical two-portal structure typically leads to aggregated nanomaterials. We demonstrate that fluorescent quantum dot (QD) aggregates linked with CBs can be broken-up, retaining CBs adsorbed at their surface, via inclusion of guests in the CB cavity. Simultaneously, the QD surface is modified by a functional tail on the guest, thus the high affinity host–guest binding (logKa > 9) enables a non-covalent, click-like modification of the nanoparticles in aqueous solution. We achieved excellent modification efficiency in several functional QD conjugates as protein labels. Inclusion of weaker-binding guests (logKa = 4–6) enables subsequent displacement with stronger binders, realising modular switchable surface chemistries. Our general “hook-and-eye” approach to host–guest chemistry at nanomaterial interfaces will lead to divergent routes for nano-architectures with rich functionalities for theranostics and photonics in aqueous systems.
| Item Type: | Articles |
|---|---|
| Additional Information: | WJP acknowledges the University of Glasgow for a Lord Kelvin Adam Smith Fellowship, the Royal Society for funding (RGS\R2\192190), and the EPSRC ECR Capital Award Scheme (EP/S017984/1) and Academy of Medical Research Springboard Grant (SBF005\1008) for supporting instrumentation. KM and CB acknowledge the EPSRC for DTA studentship funding (EP/T517896/1). AWC acknowledges The Leverhulme Trust (RPG-2018-149), the BBSRC (BB/T000627/1, BB/N016734/1), and the EPSRC (EP/V030515/1) for financial support. This work was in part supported by the European Research Council (Consolidator Grant 101002326 to J.K.) WMN and SH thank the DFG for financial support (grant no. NA 681/8). |
| Keywords: | Quantum dots, cucurbiturils, host-guest complexes, click-chemistry, nanoparticles. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Bryson, Miss Charlotte and Zheng, Mr Dazhong and Mcguire, Miss Katie Jane and Peveler, Dr William and Clark, Professor Alasdair and France, Dr David and Koehnke, Professor Jesko |
| Authors: | Mcguire, K., He, S., Gracie, J., Bryson, C., Zheng, D., Clark, A. W., Koehnke, J., France, D. J., Nau, W. M., Lee, T.-C., and Peveler, W. J. |
| College/School: | College of Science and Engineering > School of Chemistry College of Science and Engineering > School of Engineering > Biomedical Engineering |
| Journal Name: | ACS Nano |
| Publisher: | American Chemical Society |
| ISSN: | 1936-0851 |
| ISSN (Online): | 1936-086X |
| Published Online: | 03 November 2023 |
| Copyright Holders: | Copyright: © 2023 The Authors |
| First Published: | First published in ACS Nano 17(21): 21585−21594 |
| Publisher Policy: | Reproduced under a Creative Commons licence |
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