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Chiral probes for α1-AGP reporting by species-specific induced circularly polarised luminescence

Chiral probes for α1-AGP reporting by species-specific induced circularly polarised luminescence
Chiral probes for α1-AGP reporting by species-specific induced circularly polarised luminescence

Luminescence spectroscopy has been used to monitor the selective and reversible binding of pH sensitive, macrocyclic lanthanide complexes, [LnL1], to the serum protein α1-AGP, whose concentration can vary significantly in response to inflammatory processes. On binding α1-AGP, a very strong induced circularly-polarised europium luminescence signal was observed that was of opposite sign for human and bovine variants of α1-AGP-reflecting the differences in the chiral environment of their drug-binding pockets. A mixture of [EuL1] and [TbL1] complexes allowed the ratiometric monitoring of α1-AGP levels in serum. Moreover, competitive displacement of [EuL1] from the protein by certain prescription drugs could be monitored, allowing the determination of drug binding constants. Reversible binding of the sulphonamide arm as a function of pH, led to a change of the coordination environment around the lanthanide ion, from twisted square antiprism (TSAP) to a square antiprismatic geometry (SAP), signalled by emission spectral changes and verified by detailed computations and the fitting of NMR pseudocontact shift data in the sulphonamide bound TSAP structure for the Dy and Eu examples. Such analyses allowed a full definition of the magnetic susceptibility tensor for [DyL1].

2041-6520
2996-3003
Shuvaev, Sergey
c34c5544-9339-4437-b3ff-66ba5083ba19
Suturina, Elizaveta A.
24dd007d-949a-4852-99d1-ea42b00103ef
Mason, Kevin
b44d68df-9067-4812-a742-ff17df162f4b
Parker, David
31bfb567-907a-4490-af57-411089ae0e73
Shuvaev, Sergey
c34c5544-9339-4437-b3ff-66ba5083ba19
Suturina, Elizaveta A.
24dd007d-949a-4852-99d1-ea42b00103ef
Mason, Kevin
b44d68df-9067-4812-a742-ff17df162f4b
Parker, David
31bfb567-907a-4490-af57-411089ae0e73

Shuvaev, Sergey, Suturina, Elizaveta A., Mason, Kevin and Parker, David (2018) Chiral probes for α1-AGP reporting by species-specific induced circularly polarised luminescence. Chemical Science, 9 (11), 2996-3003. (doi:10.1039/c8sc00482j).

Record type: Article

Abstract

Luminescence spectroscopy has been used to monitor the selective and reversible binding of pH sensitive, macrocyclic lanthanide complexes, [LnL1], to the serum protein α1-AGP, whose concentration can vary significantly in response to inflammatory processes. On binding α1-AGP, a very strong induced circularly-polarised europium luminescence signal was observed that was of opposite sign for human and bovine variants of α1-AGP-reflecting the differences in the chiral environment of their drug-binding pockets. A mixture of [EuL1] and [TbL1] complexes allowed the ratiometric monitoring of α1-AGP levels in serum. Moreover, competitive displacement of [EuL1] from the protein by certain prescription drugs could be monitored, allowing the determination of drug binding constants. Reversible binding of the sulphonamide arm as a function of pH, led to a change of the coordination environment around the lanthanide ion, from twisted square antiprism (TSAP) to a square antiprismatic geometry (SAP), signalled by emission spectral changes and verified by detailed computations and the fitting of NMR pseudocontact shift data in the sulphonamide bound TSAP structure for the Dy and Eu examples. Such analyses allowed a full definition of the magnetic susceptibility tensor for [DyL1].

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Accepted/In Press date: 18 February 2018
e-pub ahead of print date: 19 February 2018
Published date: 21 March 2018

Identifiers

Local EPrints ID: 419132
URI: http://eprints.soton.ac.uk/id/eprint/419132
ISSN: 2041-6520
PURE UUID: ce46606c-095e-4219-8b7c-65a3ce3f8a87

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Date deposited: 06 Apr 2018 16:30
Last modified: 17 Mar 2024 12:01

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Contributors

Author: Sergey Shuvaev
Author: Elizaveta A. Suturina
Author: Kevin Mason
Author: David Parker

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