Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis

Leishmaniasis is a neglected tropical disease caused by <i>Leishmania</i> sp. The therapeutic arsenal is reduced and limited. In this context, acridine derivatives present themselves as promising leishmanicidal compounds. This paper involved synthesizing and evaluating the antileishmania...

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Main Authors: Sonaly Albino, Michelangela Nobre, Jamire da Silva, Malu dos Reis, Maria Nascimento, Mayara de Oliveira, Tatiana Borges, Lucas Albuquerque, Selma Kuckelhaus, Luis Alves, Fábio dos Santos, Maria de Lima, Igor Nascimento, Teresinha da Silva, Ricardo de Moura
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Language:English
Published: MDPI AG 2025-06-01
Series:Microorganisms
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Online Access:https://www.mdpi.com/2076-2607/13/6/1297
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author Sonaly Albino
Michelangela Nobre
Jamire da Silva
Malu dos Reis
Maria Nascimento
Mayara de Oliveira
Tatiana Borges
Lucas Albuquerque
Selma Kuckelhaus
Luis Alves
Fábio dos Santos
Maria de Lima
Igor Nascimento
Teresinha da Silva
Ricardo de Moura
author_facet Sonaly Albino
Michelangela Nobre
Jamire da Silva
Malu dos Reis
Maria Nascimento
Mayara de Oliveira
Tatiana Borges
Lucas Albuquerque
Selma Kuckelhaus
Luis Alves
Fábio dos Santos
Maria de Lima
Igor Nascimento
Teresinha da Silva
Ricardo de Moura
author_sort Sonaly Albino
collection DOAJ
description Leishmaniasis is a neglected tropical disease caused by <i>Leishmania</i> sp. The therapeutic arsenal is reduced and limited. In this context, acridine derivatives present themselves as promising leishmanicidal compounds. This paper involved synthesizing and evaluating the antileishmanial and immunomodulatory potential of spiro-acridine derivatives. Six spiro-acridine derivatives were obtained through nucleophilic substitution reactions between the acetohydrazide/acetamide intermediates and 9-carbaldehydeacridine, followed by spontaneous cyclization. IR, NMR, and HRMS confirmed the structures. These were analyzed in vitro against <i>L. infantum</i> and <i>L. amazonensis</i> to determine anti-promastigote, anti-amastigote, and cytotoxicity effects. Immunomodulatory activity was evaluated using CBA, DCF-DA, and DAF-FM diacetate. In silico evaluation included molecular docking and dynamics. The spiro-acridines showed a wide range of anti-promastigote activities (IC<sub>50</sub> = 0.73–234.95 µM) and non-toxicity to red blood cells. AMTAC-02 and ACMD-03 demonstrated satisfactory anti-amastigote effect (IC<sub>50</sub> = 10.47–13.50 µM), low toxicity to macrophages (CC<sub>50</sub> = 27.22–569.50 µM), and cytokine and reactive species modulation. Molecular docking proposed cysteine protease B of <i>L. amazonensis</i> as a target, and molecular dynamics analysis highlighted the complex’s stability using RMSD, R<sub>g</sub>, SASA, DCCM, PCA, and MM-PBSA (ΔG = −65.225 kJ/mol). Furthermore, QM-MM calculation provided the best energy for ACMD-03 (−199.30 au). Hence, AMTAC-02 and ACMD-03 demonstrated antileishmanial potential, making them promising entities for the development of leishmanicidal drug candidates.
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spelling doaj-art-dc40d24776ba4bf2a21728a4eb640a782025-08-20T02:21:07ZengMDPI AGMicroorganisms2076-26072025-06-01136129710.3390/microorganisms13061297Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against LeishmaniasisSonaly Albino0Michelangela Nobre1Jamire da Silva2Malu dos Reis3Maria Nascimento4Mayara de Oliveira5Tatiana Borges6Lucas Albuquerque7Selma Kuckelhaus8Luis Alves9Fábio dos Santos10Maria de Lima11Igor Nascimento12Teresinha da Silva13Ricardo de Moura14Postgraduate Program in Therapeutic Innovation, Federal University of Pernambuco, Recife 50740-570, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilMorphology Area, Faculty of Medicine-UnB, University of Brasília, Darcy Ribeiro Campus, Brasília 70910-900, BrazilCellular Immunology Laboratory, Pathology Area, Faculty of Medicine, University of Brasília, Darcy Ribeiro Campus, Brasília 70910-900, BrazilCellular Immunology Laboratory, Pathology Area, Faculty of Medicine, University of Brasília, Darcy Ribeiro Campus, Brasília 70910-900, BrazilMorphology Area, Faculty of Medicine-UnB, University of Brasília, Darcy Ribeiro Campus, Brasília 70910-900, BrazilDepartment of Parasitology, Aggeu Magalhães Institute (FIOCRUZ/PE), Recife 50740-465, BrazilDepartment of Parasitology, Aggeu Magalhães Institute (FIOCRUZ/PE), Recife 50740-465, BrazilDepartment of Antibiotics, Federal University of Pernambuco, Biosciences Center, Recife 50740-570, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilPostgraduate Program in Therapeutic Innovation, Federal University of Pernambuco, Recife 50740-570, BrazilDrug Development and Synthesis Laboratory, Department of Pharmacy, State University of Paraíba, Campina Grande 58429-500, BrazilLeishmaniasis is a neglected tropical disease caused by <i>Leishmania</i> sp. The therapeutic arsenal is reduced and limited. In this context, acridine derivatives present themselves as promising leishmanicidal compounds. This paper involved synthesizing and evaluating the antileishmanial and immunomodulatory potential of spiro-acridine derivatives. Six spiro-acridine derivatives were obtained through nucleophilic substitution reactions between the acetohydrazide/acetamide intermediates and 9-carbaldehydeacridine, followed by spontaneous cyclization. IR, NMR, and HRMS confirmed the structures. These were analyzed in vitro against <i>L. infantum</i> and <i>L. amazonensis</i> to determine anti-promastigote, anti-amastigote, and cytotoxicity effects. Immunomodulatory activity was evaluated using CBA, DCF-DA, and DAF-FM diacetate. In silico evaluation included molecular docking and dynamics. The spiro-acridines showed a wide range of anti-promastigote activities (IC<sub>50</sub> = 0.73–234.95 µM) and non-toxicity to red blood cells. AMTAC-02 and ACMD-03 demonstrated satisfactory anti-amastigote effect (IC<sub>50</sub> = 10.47–13.50 µM), low toxicity to macrophages (CC<sub>50</sub> = 27.22–569.50 µM), and cytokine and reactive species modulation. Molecular docking proposed cysteine protease B of <i>L. amazonensis</i> as a target, and molecular dynamics analysis highlighted the complex’s stability using RMSD, R<sub>g</sub>, SASA, DCCM, PCA, and MM-PBSA (ΔG = −65.225 kJ/mol). Furthermore, QM-MM calculation provided the best energy for ACMD-03 (−199.30 au). Hence, AMTAC-02 and ACMD-03 demonstrated antileishmanial potential, making them promising entities for the development of leishmanicidal drug candidates.https://www.mdpi.com/2076-2607/13/6/1297spontaneous cyclizationmolecular simplificationleishmaniasisimmunomodulationstructure–activity relationshipQM-MM
spellingShingle Sonaly Albino
Michelangela Nobre
Jamire da Silva
Malu dos Reis
Maria Nascimento
Mayara de Oliveira
Tatiana Borges
Lucas Albuquerque
Selma Kuckelhaus
Luis Alves
Fábio dos Santos
Maria de Lima
Igor Nascimento
Teresinha da Silva
Ricardo de Moura
Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
Microorganisms
spontaneous cyclization
molecular simplification
leishmaniasis
immunomodulation
structure–activity relationship
QM-MM
title Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
title_full Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
title_fullStr Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
title_full_unstemmed Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
title_short Synthesis, Biological Evaluation, Molecular Dynamics, and QM-MM Calculation of Spiro-Acridine Derivatives Against Leishmaniasis
title_sort synthesis biological evaluation molecular dynamics and qm mm calculation of spiro acridine derivatives against leishmaniasis
topic spontaneous cyclization
molecular simplification
leishmaniasis
immunomodulation
structure–activity relationship
QM-MM
url https://www.mdpi.com/2076-2607/13/6/1297
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