Details
| Original language | English |
|---|---|
| Pages (from-to) | 21585-21594 |
| Number of pages | 10 |
| Journal | ACS NANO |
| Volume | 17 |
| Issue number | 21 |
| Early online date | 3 Nov 2023 |
| Publication status | Published - 14 Nov 2023 |
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.
Keywords
- click-chemistry, cucurbiturils, host−guest complexes, nanoparticles, quantum dots
ASJC Scopus subject areas
- Materials Science(all)
- General Materials Science
- Engineering(all)
- General Engineering
- Physics and Astronomy(all)
- General Physics and Astronomy
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In: ACS NANO, Vol. 17, No. 21, 14.11.2023, p. 21585-21594.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Supramolecular Click Chemistry for Surface Modification of Quantum Dots Mediated by Cucurbit[7]uril
AU - McGuire, Katie
AU - He, Suhang
AU - Gracie, Jennifer
AU - Bryson, Charlotte
AU - Zheng, Dazhong
AU - Clark, Alasdair W.
AU - Koehnke, Jesko
AU - France, David J.
AU - Nau, Werner M.
AU - Lee, Tung Chun
AU - Peveler, William J.
N1 - Funding Information: The authors gratefully acknowledge M. Mullin and the Glasgow Imaging Facility for support and assistance with TEM; G. R. Ubbara for assistance with Mass Spectrometry; and B. Russell, Z. Liao, and K. Wynne for access to DLS. W.J.P. 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. K.M. and C.B. acknowledge the EPSRC for DTA studentship funding (EP/T517896/1). A.W.C. 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.). W.M.N. and S.H. thank the DFG for financial support (grant no. NA 681/8). For the purpose of open access, the authors have applied a Creative Commons Attribution (CC BY) licence to any Author Accepted Manuscript version arising from this submission
PY - 2023/11/14
Y1 - 2023/11/14
N2 - 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.
AB - 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.
KW - click-chemistry
KW - cucurbiturils
KW - host−guest complexes
KW - nanoparticles
KW - quantum dots
UR - http://www.scopus.com/inward/record.url?scp=85178447210&partnerID=8YFLogxK
U2 - 10.1021/acsnano.3c06601
DO - 10.1021/acsnano.3c06601
M3 - Article
C2 - 37922402
AN - SCOPUS:85178447210
VL - 17
SP - 21585
EP - 21594
JO - ACS NANO
JF - ACS NANO
SN - 1936-0851
IS - 21
ER -