Literature DB >> 22734650

Allyl m-trifluoromethyldiazirine mephobarbital: an unusually potent enantioselective and photoreactive barbiturate general anesthetic.

Pavel Y Savechenkov1, Xi Zhang, David C Chiara, Deirdre S Stewart, Rile Ge, Xiaojuan Zhou, Douglas E Raines, Jonathan B Cohen, Stuart A Forman, Keith W Miller, Karol S Bruzik.   

Abstract

We synthesized 5-allyl-1-methyl-5-(m-trifluoromethyl-diazirynylphenyl)barbituric acid (14), a trifluoromethyldiazirine-containing derivative of general anesthetic mephobarbital, separated the racemic mixture into enantiomers by chiral chromatography, and determined the configuration of the (+)-enantiomer as S by X-ray crystallography. Additionally, we obtained the (3)H-labeled ligand with high specific radioactivity. R-(-)-14 is an order of magnitude more potent than the most potent clinically used barbiturate, thiopental, and its general anesthetic EC(50) approaches those for propofol and etomidate, whereas S-(+)-14 is 10-fold less potent. Furthermore, at concentrations close to its anesthetic potency, R-(-)-14 both potentiated GABA-induced currents and increased the affinity for the agonist muscimol in human α1β2/3γ2L GABA(A) receptors. Finally, R-(-)-14 was found to be an exceptionally efficient photolabeling reagent, incorporating into both α1 and β3 subunits of human α1β3 GABA(A) receptors. These results indicate R-(-)-14 is a functional general anesthetic that is well-suited for identifying barbiturate binding sites on Cys-loop receptors.

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Year:  2012        PMID: 22734650      PMCID: PMC3717557          DOI: 10.1021/jm300631e

Source DB:  PubMed          Journal:  J Med Chem        ISSN: 0022-2623            Impact factor:   7.446


  51 in total

1.  Tryptophan mutations at azi-etomidate photo-incorporation sites on alpha1 or beta2 subunits enhance GABAA receptor gating and reduce etomidate modulation.

Authors:  Deirdre Stewart; Rooma Desai; Qi Cheng; Aiping Liu; Stuart A Forman
Journal:  Mol Pharmacol       Date:  2008-09-19       Impact factor: 4.436

2.  Mapping general anesthetic binding site(s) in human α1β3 γ-aminobutyric acid type A receptors with [³H]TDBzl-etomidate, a photoreactive etomidate analogue.

Authors:  David C Chiara; Zuzana Dostalova; Selwyn S Jayakar; Xiaojuan Zhou; Keith W Miller; Jonathan B Cohen
Journal:  Biochemistry       Date:  2012-01-23       Impact factor: 3.162

3.  Stereoselective interaction of thiopentone enantiomers with the GABA(A) receptor.

Authors:  D J Cordato; M Chebib; L E Mather; G K Herkes; G A Johnston
Journal:  Br J Pharmacol       Date:  1999-09       Impact factor: 8.739

4.  Interaction of barbiturate analogs with the Torpedo californica nicotinic acetylcholine receptor ion channel.

Authors:  H R Arias; E A McCardy; M J Gallagher; M P Blanton
Journal:  Mol Pharmacol       Date:  2001-09       Impact factor: 4.436

5.  p-(4-Azipentyl)propofol: a potent photoreactive general anesthetic derivative of propofol.

Authors:  Deirdre S Stewart; Pavel Y Savechenkov; Zuzana Dostalova; David C Chiara; Rile Ge; Douglas E Raines; Jonathan B Cohen; Stuart A Forman; Karol S Bruzik; Keith W Miller
Journal:  J Med Chem       Date:  2011-11-10       Impact factor: 7.446

6.  A general and convenient preparation of [bis(trifluoroacetoxy)iodo]perfluoroalkanes and [bis(trifluoroacetoxy)iodo]arenes by oxidation of organic iodides using oxone and trifluoroacetic acid.

Authors:  Aleksandra A Zagulyaeva; Mekhman S Yusubov; Viktor V Zhdankin
Journal:  J Org Chem       Date:  2010-03-19       Impact factor: 4.354

7.  Numerous classes of general anesthetics inhibit etomidate binding to gamma-aminobutyric acid type A (GABAA) receptors.

Authors:  Guo-Dong Li; David C Chiara; Jonathan B Cohen; Richard W Olsen
Journal:  J Biol Chem       Date:  2010-01-18       Impact factor: 5.157

8.  Barbiturate action is dependent on the conformational state of the acetylcholine receptor.

Authors:  A J de Armendi; P H Tonner; B Bugge; K W Miller
Journal:  Anesthesiology       Date:  1993-11       Impact factor: 7.892

9.  A comparison of the potencies of a series of barbiturates at the neuromuscular junction and on the central nervous system.

Authors:  S Lee-Son; B E Waud; D R Waud
Journal:  J Pharmacol Exp Ther       Date:  1975-11       Impact factor: 4.030

10.  Structure validation in chemical crystallography.

Authors:  Anthony L Spek
Journal:  Acta Crystallogr D Biol Crystallogr       Date:  2009-01-20
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  29 in total

Review 1.  Mapping General Anesthetic Sites in Heteromeric γ-Aminobutyric Acid Type A Receptors Reveals a Potential For Targeting Receptor Subtypes.

Authors:  Stuart A Forman; Keith W Miller
Journal:  Anesth Analg       Date:  2016-11       Impact factor: 5.108

2.  Identifying barbiturate binding sites in a nicotinic acetylcholine receptor with [3H]allyl m-trifluoromethyldiazirine mephobarbital, a photoreactive barbiturate.

Authors:  Ayman K Hamouda; Deirdre S Stewart; David C Chiara; Pavel Y Savechenkov; Karol S Bruzik; Jonathan B Cohen
Journal:  Mol Pharmacol       Date:  2014-02-21       Impact factor: 4.436

3.  Mechanisms revealed through general anesthetic photolabeling.

Authors:  Brian P Weiser; Kellie A Woll; William P Dailey; Roderic G Eckenhoff
Journal:  Curr Anesthesiol Rep       Date:  2014-03-01

4.  Dodecyl maltopyranoside enabled purification of active human GABA type A receptors for deep and direct proteomic sequencing.

Authors:  Xi Zhang; Keith W Miller
Journal:  Mol Cell Proteomics       Date:  2014-12-03       Impact factor: 5.911

5.  Binding site location on GABAA receptors determines whether mixtures of intravenous general anaesthetics interact synergistically or additively in vivo.

Authors:  Daniel E Kent; Pavel Y Savechenkov; Karol S Bruzik; Keith W Miller
Journal:  Br J Pharmacol       Date:  2019-12-11       Impact factor: 8.739

6.  Alphaxalone Binds in Inner Transmembrane β+-α- Interfaces of α1β3γ2 γ-Aminobutyric Acid Type A Receptors.

Authors:  Alexis M Ziemba; Andrea Szabo; David W Pierce; Marian Haburcak; Alex T Stern; Anahita Nourmahnad; Elizabeth S Halpin; Stuart A Forman
Journal:  Anesthesiology       Date:  2018-02       Impact factor: 7.892

7.  Tryptophan and Cysteine Mutations in M1 Helices of α1β3γ2L γ-Aminobutyric Acid Type A Receptors Indicate Distinct Intersubunit Sites for Four Intravenous Anesthetics and One Orphan Site.

Authors:  Anahita Nourmahnad; Alex T Stern; Mayo Hotta; Deirdre S Stewart; Alexis M Ziemba; Andrea Szabo; Stuart A Forman
Journal:  Anesthesiology       Date:  2016-12       Impact factor: 7.892

8.  Discovery of allosteric modulators for GABAA receptors by ligand-directed chemistry.

Authors:  Kei Yamaura; Shigeki Kiyonaka; Tomohiro Numata; Ryuji Inoue; Itaru Hamachi
Journal:  Nat Chem Biol       Date:  2016-08-15       Impact factor: 15.040

9.  A potent photoreactive general anesthetic with novel binding site selectivity for GABAA receptors.

Authors:  Abdelrahman R Shalabi; Zhiyi Yu; Xiaojuan Zhou; Youssef Jounaidi; Hanwen Chen; Jiajia Dai; Daniel E Kent; Hua-Jun Feng; Stuart A Forman; Jonathan B Cohen; Karol S Bruzik; Keith W Miller
Journal:  Eur J Med Chem       Date:  2020-03-23       Impact factor: 6.514

Review 10.  Shedding Light on Anesthetic Mechanisms: Application of Photoaffinity Ligands.

Authors:  Kellie A Woll; William P Dailey; Grace Brannigan; Roderic G Eckenhoff
Journal:  Anesth Analg       Date:  2016-11       Impact factor: 5.108

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