Interaction of the Antibiotic Rifampicin with Lipid Membranes

Rifampicin is a broad-spectrum antibiotic, active against several bacterial infections such as tuberculosis. It is a relatively large and structurally complex molecule, including numerous polar groups. Although violating several of Lipinski’s rules for efficient intestinal absorption, rifampicin sho...

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Main Authors: Rui M. S. Santos, Jaime Samelo, Alexandre C. Oliveira, Margarida M. Cordeiro, Maria Julia Mora, Gladys E. Granero, Hugo A. L. Filipe, Luís M. S. Loura, Maria João Moreno
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Language:English
Published: MDPI AG 2025-02-01
Series:Biomolecules
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Online Access:https://www.mdpi.com/2218-273X/15/3/320
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author Rui M. S. Santos
Jaime Samelo
Alexandre C. Oliveira
Margarida M. Cordeiro
Maria Julia Mora
Gladys E. Granero
Hugo A. L. Filipe
Luís M. S. Loura
Maria João Moreno
author_facet Rui M. S. Santos
Jaime Samelo
Alexandre C. Oliveira
Margarida M. Cordeiro
Maria Julia Mora
Gladys E. Granero
Hugo A. L. Filipe
Luís M. S. Loura
Maria João Moreno
author_sort Rui M. S. Santos
collection DOAJ
description Rifampicin is a broad-spectrum antibiotic, active against several bacterial infections such as tuberculosis. It is a relatively large and structurally complex molecule, including numerous polar groups. Although violating several of Lipinski’s rules for efficient intestinal absorption, rifampicin shows good oral bioavailability, permeating through cell membranes in the absorption pathway and those of the target organisms. Some hypotheses have been proposed for its efficient membrane permeation, but the details are mostly unknown. In this work, the interaction of rifampicin with POPC lipid bilayers is studied using experimental biophysics methodologies and atomistic molecular dynamics simulations considering the two most prevalent ionic species at physiological pH, the anionic and the zwitterionic forms. The results show that both ionization forms of rifampicin establish favorable interactions with the membrane lipids, in agreement with the relatively high partition coefficient obtained experimentally. The results from MD simulations and isothermal titration calorimetry using different pH buffers show that the piperazine group inserts deeply in the membrane and is accompanied by a stabilization of its neutral form. The bulky nature of rifampicin and its deep insertion in the membrane lead to a strong perturbation in the lipids local order, decreasing the membrane barrier properties as evaluated from the rate of carboxyfluorescein leaching. Altogether, the comparison between the experimental and MD simulations results provides important insight regarding the rifampicin molecular features responsible for its relatively fast membrane permeation. The lipid POPC used in this study was selected as a simple membrane with relevance for different organisms across all kingdoms. Further studies using more complex lipid compositions will provide details on eventual specificities for rifampicin interaction with the membranes of distinct organisms.
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spelling doaj-art-601232f26ee04e48942dd725a5aa373e2025-08-20T03:43:26ZengMDPI AGBiomolecules2218-273X2025-02-0115332010.3390/biom15030320Interaction of the Antibiotic Rifampicin with Lipid MembranesRui M. S. Santos0Jaime Samelo1Alexandre C. Oliveira2Margarida M. Cordeiro3Maria Julia Mora4Gladys E. Granero5Hugo A. L. Filipe6Luís M. S. Loura7Maria João Moreno8Coimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalUnidad de Investigación y Desarrollo en Tecnología Farmacéutica (UNITEFA, CONICET) and Departamento de Ciencias Farmacéuticas, Facultad de Ciencias Químicas, Universidad Nacional de Córdoba, Ciudad Universitaria, Córdoba 5000, ArgentinaCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalCoimbra Chemistry Center, Institute of Molecular Sciences (CQC-IMS), University of Coimbra, 3004-535 Coimbra, PortugalRifampicin is a broad-spectrum antibiotic, active against several bacterial infections such as tuberculosis. It is a relatively large and structurally complex molecule, including numerous polar groups. Although violating several of Lipinski’s rules for efficient intestinal absorption, rifampicin shows good oral bioavailability, permeating through cell membranes in the absorption pathway and those of the target organisms. Some hypotheses have been proposed for its efficient membrane permeation, but the details are mostly unknown. In this work, the interaction of rifampicin with POPC lipid bilayers is studied using experimental biophysics methodologies and atomistic molecular dynamics simulations considering the two most prevalent ionic species at physiological pH, the anionic and the zwitterionic forms. The results show that both ionization forms of rifampicin establish favorable interactions with the membrane lipids, in agreement with the relatively high partition coefficient obtained experimentally. The results from MD simulations and isothermal titration calorimetry using different pH buffers show that the piperazine group inserts deeply in the membrane and is accompanied by a stabilization of its neutral form. The bulky nature of rifampicin and its deep insertion in the membrane lead to a strong perturbation in the lipids local order, decreasing the membrane barrier properties as evaluated from the rate of carboxyfluorescein leaching. Altogether, the comparison between the experimental and MD simulations results provides important insight regarding the rifampicin molecular features responsible for its relatively fast membrane permeation. The lipid POPC used in this study was selected as a simple membrane with relevance for different organisms across all kingdoms. Further studies using more complex lipid compositions will provide details on eventual specificities for rifampicin interaction with the membranes of distinct organisms.https://www.mdpi.com/2218-273X/15/3/320drug–membrane associationmembrane perturbationdrug bioavailability
spellingShingle Rui M. S. Santos
Jaime Samelo
Alexandre C. Oliveira
Margarida M. Cordeiro
Maria Julia Mora
Gladys E. Granero
Hugo A. L. Filipe
Luís M. S. Loura
Maria João Moreno
Interaction of the Antibiotic Rifampicin with Lipid Membranes
Biomolecules
drug–membrane association
membrane perturbation
drug bioavailability
title Interaction of the Antibiotic Rifampicin with Lipid Membranes
title_full Interaction of the Antibiotic Rifampicin with Lipid Membranes
title_fullStr Interaction of the Antibiotic Rifampicin with Lipid Membranes
title_full_unstemmed Interaction of the Antibiotic Rifampicin with Lipid Membranes
title_short Interaction of the Antibiotic Rifampicin with Lipid Membranes
title_sort interaction of the antibiotic rifampicin with lipid membranes
topic drug–membrane association
membrane perturbation
drug bioavailability
url https://www.mdpi.com/2218-273X/15/3/320
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