Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics

The duration of action of adenosine A2A receptor (A2A) agonists is critical for their clinical efficacy, and we sought to better understand how this can be optimized. The in vitro temporal response profiles of a panel of A2A agonists were studied using cAMP assays in recombinantly (CHO) and endogeno...

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Main Authors: Hothersall, J. Daniel, Guo, Dong, Sarda, Sunil, Sheppard, Robert J., Chen, Hongming, Keur, Wesley, Waring, Michael J., IJzerman, Adriaan P., Hill, Stephen J., Dale, Ian L., Rawlins, Philip B.
Format: Article
Published: ASPET 2017
Online Access:https://eprints.nottingham.ac.uk/40520/
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author Hothersall, J. Daniel
Guo, Dong
Sarda, Sunil
Sheppard, Robert J.
Chen, Hongming
Keur, Wesley
Waring, Michael J.
IJzerman, Adriaan P.
Hill, Stephen J.
Dale, Ian L.
Rawlins, Philip B.
author_facet Hothersall, J. Daniel
Guo, Dong
Sarda, Sunil
Sheppard, Robert J.
Chen, Hongming
Keur, Wesley
Waring, Michael J.
IJzerman, Adriaan P.
Hill, Stephen J.
Dale, Ian L.
Rawlins, Philip B.
author_sort Hothersall, J. Daniel
building Nottingham Research Data Repository
collection Online Access
description The duration of action of adenosine A2A receptor (A2A) agonists is critical for their clinical efficacy, and we sought to better understand how this can be optimized. The in vitro temporal response profiles of a panel of A2A agonists were studied using cAMP assays in recombinantly (CHO) and endogenously (SH-SY5Y) expressing cells. Some agonists (e.g., 3cd; UK-432,097) but not others (e.g., 3ac; CGS-21680) demonstrated sustained wash-resistant agonism, where residual receptor activation continued after washout. The ability of an antagonist to reverse pre-established agonist responses was used as a surrogate read-out for agonist dissociation kinetics, and together with radioligand binding studies suggested a role for slow off-rate in driving sustained effects. One compound, 3ch, showed particularly marked sustained effects, with a reversal t1/2 > 6 hours and close to maximal effects that remained for at least 5 hours after washing. Based on the structure-activity relationship of these compounds, we suggest that lipophilic N6 and bulky C2 substituents can promote stable and long-lived binding events leading to sustained agonist responses, although a high compound logD is not necessary. This provides new insight into the binding interactions of these ligands and we anticipate that this information could facilitate the rational design of novel long-acting A2A agonists with improved clinical efficacy.
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spelling nottingham-405202020-05-04T18:23:01Z https://eprints.nottingham.ac.uk/40520/ Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics Hothersall, J. Daniel Guo, Dong Sarda, Sunil Sheppard, Robert J. Chen, Hongming Keur, Wesley Waring, Michael J. IJzerman, Adriaan P. Hill, Stephen J. Dale, Ian L. Rawlins, Philip B. The duration of action of adenosine A2A receptor (A2A) agonists is critical for their clinical efficacy, and we sought to better understand how this can be optimized. The in vitro temporal response profiles of a panel of A2A agonists were studied using cAMP assays in recombinantly (CHO) and endogenously (SH-SY5Y) expressing cells. Some agonists (e.g., 3cd; UK-432,097) but not others (e.g., 3ac; CGS-21680) demonstrated sustained wash-resistant agonism, where residual receptor activation continued after washout. The ability of an antagonist to reverse pre-established agonist responses was used as a surrogate read-out for agonist dissociation kinetics, and together with radioligand binding studies suggested a role for slow off-rate in driving sustained effects. One compound, 3ch, showed particularly marked sustained effects, with a reversal t1/2 > 6 hours and close to maximal effects that remained for at least 5 hours after washing. Based on the structure-activity relationship of these compounds, we suggest that lipophilic N6 and bulky C2 substituents can promote stable and long-lived binding events leading to sustained agonist responses, although a high compound logD is not necessary. This provides new insight into the binding interactions of these ligands and we anticipate that this information could facilitate the rational design of novel long-acting A2A agonists with improved clinical efficacy. ASPET 2017-01-01 Article PeerReviewed Hothersall, J. Daniel, Guo, Dong, Sarda, Sunil, Sheppard, Robert J., Chen, Hongming, Keur, Wesley, Waring, Michael J., IJzerman, Adriaan P., Hill, Stephen J., Dale, Ian L. and Rawlins, Philip B. (2017) Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics. Molecular Pharmacology, 91 (1). pp. 25-38. ISSN 1521-0111 http://molpharm.aspetjournals.org/content/91/1/25 doi:10.1124/mol.116.105551 doi:10.1124/mol.116.105551
spellingShingle Hothersall, J. Daniel
Guo, Dong
Sarda, Sunil
Sheppard, Robert J.
Chen, Hongming
Keur, Wesley
Waring, Michael J.
IJzerman, Adriaan P.
Hill, Stephen J.
Dale, Ian L.
Rawlins, Philip B.
Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title_full Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title_fullStr Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title_full_unstemmed Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title_short Structure-activity relationships of the sustained effects of adenosine A2A receptor agonists driven by slow dissociation kinetics
title_sort structure-activity relationships of the sustained effects of adenosine a2a receptor agonists driven by slow dissociation kinetics
url https://eprints.nottingham.ac.uk/40520/
https://eprints.nottingham.ac.uk/40520/
https://eprints.nottingham.ac.uk/40520/