A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor

Recently, a novel negative allosteric modulator (NAM) of the D 2-like dopamine receptors 1 was identified through virtual ligand screening. This ligand comprises a thieno[2,3-d]pyrimidine scaffold that does not feature in known dopaminergic ligands. Herein, we provide pharmacological validation of a...

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Main Authors: Fyfe, Tim J., Zarzycka, Barbara, Lim, Herman D., Kellam, Barrie, Mistry, Shailesh N., Katrich, Vsevolod, Scammells, Peter J., Lane, J. Robert, Capuano, Ben
Format: Article
Language:English
Published: American Chemical Society 2018
Online Access:https://eprints.nottingham.ac.uk/51343/
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author Fyfe, Tim J.
Zarzycka, Barbara
Lim, Herman D.
Kellam, Barrie
Mistry, Shailesh N.
Katrich, Vsevolod
Scammells, Peter J.
Lane, J. Robert
Capuano, Ben
author_facet Fyfe, Tim J.
Zarzycka, Barbara
Lim, Herman D.
Kellam, Barrie
Mistry, Shailesh N.
Katrich, Vsevolod
Scammells, Peter J.
Lane, J. Robert
Capuano, Ben
author_sort Fyfe, Tim J.
building Nottingham Research Data Repository
collection Online Access
description Recently, a novel negative allosteric modulator (NAM) of the D 2-like dopamine receptors 1 was identified through virtual ligand screening. This ligand comprises a thieno[2,3-d]pyrimidine scaffold that does not feature in known dopaminergic ligands. Herein, we provide pharmacological validation of an allosteric mode of action for 1, revealing that it is a NAM of dopamine efficacy and identify the structural determinants of this allostery. We find that key structural moieties are important for functional affinity and negative cooperativity, whilst functionalization of the thienopyrimidine at the 5- and 6-positions results in analogues with divergent cooperativity profiles. Successive compound iterations have yielded analogues exhibiting a 10-fold improvement in functional affinity, as well as enhanced negative cooperativity with dopamine affinity and efficacy. Furthermore, our study reveals a fragment-like core that maintains low μM affinity and robust negative cooperativity with markedly improved ligand efficiency.
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spelling nottingham-513432019-04-23T04:30:14Z https://eprints.nottingham.ac.uk/51343/ A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor Fyfe, Tim J. Zarzycka, Barbara Lim, Herman D. Kellam, Barrie Mistry, Shailesh N. Katrich, Vsevolod Scammells, Peter J. Lane, J. Robert Capuano, Ben Recently, a novel negative allosteric modulator (NAM) of the D 2-like dopamine receptors 1 was identified through virtual ligand screening. This ligand comprises a thieno[2,3-d]pyrimidine scaffold that does not feature in known dopaminergic ligands. Herein, we provide pharmacological validation of an allosteric mode of action for 1, revealing that it is a NAM of dopamine efficacy and identify the structural determinants of this allostery. We find that key structural moieties are important for functional affinity and negative cooperativity, whilst functionalization of the thienopyrimidine at the 5- and 6-positions results in analogues with divergent cooperativity profiles. Successive compound iterations have yielded analogues exhibiting a 10-fold improvement in functional affinity, as well as enhanced negative cooperativity with dopamine affinity and efficacy. Furthermore, our study reveals a fragment-like core that maintains low μM affinity and robust negative cooperativity with markedly improved ligand efficiency. American Chemical Society 2018-04-23 Article PeerReviewed application/pdf en https://eprints.nottingham.ac.uk/51343/1/A%20Thieno23-dpyrimidine%20Scaffold%20is%20a%20Novel%20Negative%20Allosteric%20Modulator%20of%20the%20Dopamine%20D2%20Receptor%20%28J%20Med%20Chem%20accepted%20230418%29.pdf Fyfe, Tim J., Zarzycka, Barbara, Lim, Herman D., Kellam, Barrie, Mistry, Shailesh N., Katrich, Vsevolod, Scammells, Peter J., Lane, J. Robert and Capuano, Ben (2018) A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor. Journal of Medicinal Chemistry . ISSN 1520-4804 https://pubs.acs.org/doi/10.1021/acs.jmedchem.7b01565 doi:10.1021/acs.jmedchem.7b01565 doi:10.1021/acs.jmedchem.7b01565
spellingShingle Fyfe, Tim J.
Zarzycka, Barbara
Lim, Herman D.
Kellam, Barrie
Mistry, Shailesh N.
Katrich, Vsevolod
Scammells, Peter J.
Lane, J. Robert
Capuano, Ben
A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title_full A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title_fullStr A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title_full_unstemmed A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title_short A thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine D2 receptor
title_sort thieno[2,3-d]pyrimidine scaffold is a novel negative allosteric modulator of the dopamine d2 receptor
url https://eprints.nottingham.ac.uk/51343/
https://eprints.nottingham.ac.uk/51343/
https://eprints.nottingham.ac.uk/51343/