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Synthesis of R-GABA Derivatives via Pd(II) Catalyzed Enantioselective C(sp3)-H Arylation and Virtual Validation with GABAB1 Receptor for Potential leads

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논문

Synthesis of R-GABA Derivatives via Pd(II) Catalyzed Enantioselective C(sp3)-H Arylation and Virtual Validation with GABAB1 Receptor for Potential leads

학술지

Chemistry, an Asian journal

저자명

Mohanlal, Smitha; Saha, Diprupa; Pandey, Shubhant; Acharya, Rudresh; Sharma, Nagendra K.

초록

<P><B>Abstract</B><P>GABA (&gamma;-amino butyric acid) analogues like baclofen, tolibut, phenibut, etc., are well-known GABAB1 inhibitors and pharmaceutically important drugs. However, there is a huge demand for more chiral GABA aryl analogues with promising pharmacological actions. Here, we demonstrate the chiral ligand acetyl-protected amino quinoline (APAQ) mediated enantioselective synthesis of GABAB1 inhibitor drug scaffolds from easily accessible GABA via Pd-catalyzed C(sp<SUP>3</SUP>)&#x2212;H activation. The synthetic methodology shows moderate to good yields, up to 74% of <I>ee</I>. We have successfully demonstrated the deprotection and removal of the directing group to synthesize <I>R</I>-tolibut in 86% yield. Further, we employed computation to probe the binding of <I>R</I>-GABA analogues to the extracellular domain of the human GABAB1 receptor. Our Rosetta-based molecular docking calculations show better binding for four <I>R</I>-enantiomers of GABA analogues than <I>R</I>-baclofen and <I>R</I>-phenibut. In addition, we employed GROMACS MD simulations and MMPB(GB)SA calculations to identify per-residue contribution to binding free energy. Our computational results suggest analogues (3<I>R</I>)&#x2010;4&#x2010;amino&#x2010;3&#x2010;(3,4&#x2010;dimethylphenyl) butanoic acid, (3<I>R</I>)&#x2010;4&#x2010;amino&#x2010;3&#x2010;(3&#x2010;fluorophenyl) butanoic acid, (3<I>R</I>)&#x2010;3&#x2010;(4&#x2010;acetylphenyl)&#x2010;4&#x2010;aminobutanoic acid, (3<I>R</I>)&#x2010;4&#x2010;amino&#x2010;3&#x2010;(4&#x2010;methoxyphenyl) butanoic acid, and (3<I>R</I>)&#x2010;4&#x2010;amino&#x2010;3&#x2010;phenylbutanoic acid are potential leads which could be synthesized from our methodology reported here.</P></P>

발행연도

2024

발행기관

Wiley (John WileySons)

ISSN

1861-4728

ISSN

1861-471x

19

11

페이지

pp.e202400064

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1 2023-12-11

논문; 2024-06-03

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