Design, synthesis and structural exploration of novel fluorinated dabigatran derivatives as direct thrombin inhibitors

Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their thrombin inhibitory activity in vitro. Among these compounds, 14h, 14m, 14s and 14t were potent and the activity was in the range of reference dru...

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Published in:European journal of medicinal chemistry Vol. 96; pp. 122 - 138
Main Authors: Li, Mei-Lin, Ren, Yu-Jie, Dong, Ming-Hui, Ren, Wei-Xin
Format: Journal Article
Language:English
Published: ISSY-LES-MOULINEAUX Elsevier Masson SAS 26.05.2015
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ISSN:0223-5234, 1768-3254
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Abstract Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their thrombin inhibitory activity in vitro. Among these compounds, 14h, 14m, 14s and 14t were potent and the activity was in the range of reference drug, dabigatran. Three structural changes were introduced in these 21 compounds to elucidate the structure–activity relationship of the drugs. In addition, prodrugs of compounds 14h and 14s were developed to investigate their anticoagulant activities in vivo. In these experiments, compound 16 showed a fairly strong inhibitory effect on thrombin-induced platelet aggregation, and demonstrated potent activity for inhibiting arteriovenous thrombosis with an inhibition rate of (73 ± 6) %, which was comparable to that of dabigatran etexilate (76 ± 2) %. Moreover, molecular docking studies were performed to understand the binding interactions of active compounds 14h, 14s and 14t with thrombin protein (PDB ID:1KTS). Contour maps obtained from the 3D-QSAR model are meaningful in designing more active molecules to act as direct inhibitors of thrombin. [Display omitted] •Twenty-one novel fluorinated dabigatran derivatives were designed and synthesized.•All compounds efficiently inhibited thrombin at nanomolar levels in vitro.•Compound 14s showed the best inhibitory activity against thrombin (IC50 = 3.23 nM).•Compound 16 exhibited a potent inhibition against arteriovenous thrombosis in vivo.•Computational studies were performed to explain the inhibitory mechanism and SAR.
AbstractList Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their thrombin inhibitory activity in vitro. Among these compounds, 14h, 14m, 14s and 14t were potent and the activity was in the range of reference drug, dabigatran. Three structural changes were introduced in these 21 compounds to elucidate the structure activity relationship of the drugs. In addition, prodrugs of compounds 14h and 14s were developed to investigate their anticoagulant activities in vivo. In these experiments, compound 16 showed a fairly strong inhibitory effect on thrombin-induced platelet aggregation, and demonstrated potent activity for inhibiting arteriovenous thrombosis with an inhibition rate of (73 +/- 6) %, which was comparable to that of dabigatran etexilate (76 +/- 2) %. Moreover, molecular docking studies were performed to understand the binding interactions of active compounds 14h, 14s and 14t with thrombin protein (PDB ID:1 KTS). Contour maps obtained from the 3D-QSAR model are meaningful in designing more active molecules to act as direct inhibitors of thrombin. (C) 2015 Elsevier Masson SAS. All rights reserved.
Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their thrombin inhibitory activity in vitro. Among these compounds, 14h, 14m, 14s and 14t were potent and the activity was in the range of reference drug, dabigatran. Three structural changes were introduced in these 21 compounds to elucidate the structure–activity relationship of the drugs. In addition, prodrugs of compounds 14h and 14s were developed to investigate their anticoagulant activities in vivo. In these experiments, compound 16 showed a fairly strong inhibitory effect on thrombin-induced platelet aggregation, and demonstrated potent activity for inhibiting arteriovenous thrombosis with an inhibition rate of (73 ± 6) %, which was comparable to that of dabigatran etexilate (76 ± 2) %. Moreover, molecular docking studies were performed to understand the binding interactions of active compounds 14h, 14s and 14t with thrombin protein (PDB ID:1KTS). Contour maps obtained from the 3D-QSAR model are meaningful in designing more active molecules to act as direct inhibitors of thrombin. [Display omitted] •Twenty-one novel fluorinated dabigatran derivatives were designed and synthesized.•All compounds efficiently inhibited thrombin at nanomolar levels in vitro.•Compound 14s showed the best inhibitory activity against thrombin (IC50 = 3.23 nM).•Compound 16 exhibited a potent inhibition against arteriovenous thrombosis in vivo.•Computational studies were performed to explain the inhibitory mechanism and SAR.
Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their thrombin inhibitory activity in vitro. Among these compounds, 14h, 14m, 14s and 14t were potent and the activity was in the range of reference drug, dabigatran. Three structural changes were introduced in these 21 compounds to elucidate the structure-activity relationship of the drugs. In addition, prodrugs of compounds 14h and 14s were developed to investigate their anticoagulant activities in vivo. In these experiments, compound 16 showed a fairly strong inhibitory effect on thrombin-induced platelet aggregation, and demonstrated potent activity for inhibiting arteriovenous thrombosis with an inhibition rate of (73 ± 6) %, which was comparable to that of dabigatran etexilate (76 ± 2) %. Moreover, molecular docking studies were performed to understand the binding interactions of active compounds 14h, 14s and 14t with thrombin protein (PDB ID:1KTS). Contour maps obtained from the 3D-QSAR model are meaningful in designing more active molecules to act as direct inhibitors of thrombin.
Author Ren, Wei-Xin
Dong, Ming-Hui
Li, Mei-Lin
Ren, Yu-Jie
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Keywords PCHLJHIZYCJIRV-UHFFFAOYSA-N
VOUZBDCMLRKPJO-UHFFFAOYSA-N
Fluorinated dabigatran derivatives
Anticoagulant activity
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Synthesis
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FKEYMTIYCZZRMZ-UHFFFAOYSA-N
IXZRETUOHYOMNR-UHFFFAOYSA-N
DIDZBBLRDSTKCE-UHFFFAOYSA-N
LWEUEDJYLBHXAZ-UHFFFAOYSA-N
Computer-aided simulation
BPSNCXSWJKHOLW-UHFFFAOYSA-N
MADJUFXLRYLAOT-UHFFFAOYSA-N
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ZLPRAKFLAXBDOM-UHFFFAOYSA-N
LYJLSFCGAWKCDC-UHFFFAOYSA-N
MEDICINAL CHEMISTRY
XIMELAGATRAN
IN-VITRO
POTENT
STROKE PREVENTION
ORAL ANTICOAGULANTS
ETEXILATE
Language English
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Snippet Twenty-one fluorinated dabigatran derivatives were designed based on the bioisosteric principle. All derivatives were synthesised and evaluated for their...
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StartPage 122
SubjectTerms Animals
Anticoagulant activity
Anticoagulants - chemical synthesis
Anticoagulants - chemistry
Anticoagulants - pharmacology
Antithrombins - chemical synthesis
Antithrombins - chemistry
Antithrombins - pharmacology
Blood Coagulation - drug effects
Chemistry, Medicinal
Computer-aided simulation
Dabigatran - chemistry
Dabigatran - pharmacology
Dose-Response Relationship, Drug
Drug Design
Fluorinated dabigatran derivatives
Humans
Hydrocarbons, Fluorinated - chemical synthesis
Hydrocarbons, Fluorinated - chemistry
Hydrocarbons, Fluorinated - pharmacology
Life Sciences & Biomedicine
Molecular Structure
Pharmacology & Pharmacy
Platelet Aggregation - drug effects
Rats
Rats, Sprague-Dawley
Science & Technology
Structure-Activity Relationship
Synthesis
Thrombin - antagonists & inhibitors
Thrombin - metabolism
Title Design, synthesis and structural exploration of novel fluorinated dabigatran derivatives as direct thrombin inhibitors
URI https://dx.doi.org/10.1016/j.ejmech.2015.04.012
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