Immune cell targeted fumaric esters support a role of GPR109A as a primary target of monomethyl fumarate in vivo.


Journal

Inflammopharmacology
ISSN: 1568-5608
Titre abrégé: Inflammopharmacology
Pays: Switzerland
ID NLM: 9112626

Informations de publication

Date de publication:
Jun 2023
Historique:
received: 02 12 2022
accepted: 19 02 2023
medline: 1 6 2023
pubmed: 3 4 2023
entrez: 2 4 2023
Statut: ppublish

Résumé

Dimethyl fumarate (DMF) is approved as a treatment for multiple sclerosis (MS), however, its mode of action remains unclear. One hypothesis proposes that Michael addition to thiols by DMF, notably glutathione is immunomodulatory. The alternative proposes that monomethyl fumarate (MMF), the hydrolysis product of DMF, is a ligand to the fatty acid receptor GPR109A found in the lysosomes of immune cells. We prepared esters of MMF and macrolides derived from azithromycin, which were tropic to immune cells by virtue of lysosomal trapping. We tested the effects of these substances in an assay of response to Lipopolysaccharide (LPS) in freshly isolated human peripheral blood mononuclear cells (PBMCs). In this system, we observed that the 4'' ester of MMF (compound 2 and 3) reduced levels of Interleukins (IL)-1β, IL-12 and tumor necrosis factor alpha (TNFα) significantly at a concentration of 1 µM, while DMF required about 25 µM for the same effect. The 2' esters of MMF (compound 1 and 2) were, like MMF itself, inactive in vitro. The 4'' ester formed glutathione conjugates rapidly while the 2' conjugates did not react with thiols but did hydrolyze slowly to release MMF in these cells. We then tested the substances in vivo using the imiquimod/isostearate model of psoriasis where the 2' ester was the most active at 0.06-0.12 mg/kg (approximately 0.1 µmol/kg), improving skin score, body weight and cytokine levels (TNFα, IL-17A, IL-17F, IL-6, IL-1β, NLRP3 and IL-23A). In contrast, the thiol reactive 4'' ester was less active than the 2' ester while DMF was ca. 300-fold less active. The thiol reactive 4'' ester was not easily recovered from either plasma or organs while the 2' ester exhibited conventional uptake and elimination. The 2' ester also reduced levels of IL-6 in acute monosodium urate (MSU) induced inflammation. These data suggest that mechanisms that are relevant in vivo center on the release of MMF. Given that GPR109A is localized to the lysosome, and that lysosomal trapping increases 2' ester activity by > 300 fold, these data suggest that GPR109A may be the main target in vivo. In contrast, the effects associated with glutathione (GSH) conjugation in vitro are unlikely to be as effective in vivo due to the much lower dose in use which cannot titrate the more concentrated thiols. These data support the case for GPR109A modulation in autoimmune diseases.

Identifiants

pubmed: 37004600
doi: 10.1007/s10787-023-01186-0
pii: 10.1007/s10787-023-01186-0
doi:

Substances chimiques

monomethyl fumarate 45IUB1PX8R
Esters 0
Interleukin-6 0
Tumor Necrosis Factor-alpha 0
citraconic acid 0RQ6CXO9KD
Dimethyl Fumarate FO2303MNI2
Glutathione GAN16C9B8O

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

1223-1239

Informations de copyright

© 2023. The Author(s), under exclusive licence to Springer Nature Switzerland AG.

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Auteurs

Simon Straß (S)

Pharmaceutical Chemistry, Institute for Pharmaceutical Sciences, Eberhard Karls University Tübingen, Tübingen, Germany.
Synovo GmbH, Tübingen, Germany.

Johanna Geiger (J)

Synovo GmbH, Tübingen, Germany.

Natascha Cloos (N)

Synovo GmbH, Tübingen, Germany.

Nadja Späth (N)

Synovo GmbH, Tübingen, Germany.

Sophia Geiger (S)

Synovo GmbH, Tübingen, Germany.

Anna Schwamborn (A)

Synovo GmbH, Tübingen, Germany.

Luciano De Oliveira da Cunha (L)

Synovo GmbH, Tübingen, Germany.

Mariella Martorelli (M)

Pharmaceutical Chemistry, Institute for Pharmaceutical Sciences, Eberhard Karls University Tübingen, Tübingen, Germany.
Synovo GmbH, Tübingen, Germany.

Jan-Hinrich Guse (JH)

Synovo GmbH, Tübingen, Germany.

Thaisa Lucas Sandri (TL)

Synovo GmbH, Tübingen, Germany.
Institute of Tropical Medicine, Eberhard Karls University Tübingen, Tübingen, Germany.

Michael Burnet (M)

Synovo GmbH, Tübingen, Germany. michael.burnet@synovo.com.

Stefan Laufer (S)

Pharmaceutical Chemistry, Institute for Pharmaceutical Sciences, Eberhard Karls University Tübingen, Tübingen, Germany.

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