Betulinic Acid Hydroxamate is Neuroprotective and Induces Protein Phosphatase 2A-Dependent HIF-1α Stabilization and Post-transcriptional Dephosphorylation of Prolyl Hydrolase 2.


Journal

Neurotherapeutics : the journal of the American Society for Experimental NeuroTherapeutics
ISSN: 1878-7479
Titre abrégé: Neurotherapeutics
Pays: United States
ID NLM: 101290381

Informations de publication

Date de publication:
07 2021
Historique:
accepted: 07 07 2021
pubmed: 3 8 2021
medline: 4 3 2022
entrez: 2 8 2021
Statut: ppublish

Résumé

Huntington's disease (HD) is a neurodegenerative disorder characterized by unwanted choreatic movements, behavioral and psychiatric disturbances, and dementia. The activation of the hypoxic response pathway through the pharmacological inhibition of hypoxia-inducing factor (HIF) prolyl-hydroxylases (PHDs) is a promising approach for neurodegenerative diseases, including HD. Herein, we have studied the mechanism of action of the compound Betulinic acid hydroxamate (BAH), a hypoximimetic derivative of betulinic acid, and its efficacy against striatal neurodegeneration using complementary approaches. Firstly, we showed the molecular mechanisms through which BAH modifies the activity of the PHD2 prolyl hydroxylase, thus directly affecting HIF-1α stability. BAH treatment reduces PHD2 phosphorylation on Ser-125 residue, responsible for the control of its hydrolase activity. HIF activation by BAH is inhibited by okadaic acid and LB-100 indicating that a protein phosphatase 2A (PP2A) is implicated in the mechanism of action of BAH. Furthermore, in striatal cells bearing a mutated form of the huntingtin protein, BAH stabilized HIF-1α protein, induced Vegf and Bnip3 gene expression and protected against mitochondrial toxin-induced cytotoxicity. Pharmacokinetic analyses showed that BAH has a good brain penetrability and experiments performed in a mouse model of striatal neurodegeneration induced by 3-nitropropionic acid showed that BAH improved the clinical symptoms. In addition, BAH also prevented neuronal loss, decreased reactive astrogliosis and microglial activation, inhibited the upregulation of proinflammatory markers, and improved antioxidant defenses in the brain. Taken together, our results show BAH's ability to activate the PP2A/PHD2/HIF pathway, which may have important implications in the treatment of HD and perhaps other neurodegenerative diseases.

Identifiants

pubmed: 34339019
doi: 10.1007/s13311-021-01089-4
pii: 10.1007/s13311-021-01089-4
pmc: PMC8608974
doi:

Substances chimiques

Hif1a protein, mouse 0
Hypoxia-Inducible Factor 1, alpha Subunit 0
Neuroprotective Agents 0
Nitro Compounds 0
Pentacyclic Triterpenes 0
Propionates 0
Egln1 protein, mouse EC 1.14.11.29
Hypoxia-Inducible Factor-Proline Dioxygenases EC 1.14.11.29
Protein Phosphatase 2 EC 3.1.3.16
3-nitropropionic acid QY4L0FOX0D
Betulinic Acid 4G6A18707N

Types de publication

Journal Article Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Pagination

1849-1861

Informations de copyright

© 2021. The Author(s).

Références

Piotr, R. and B.-K. Teresa, Natural Triterpenoids and their Derivatives with Pharmacological Activity Against Neurodegenerative Disorders. Mini Rev Org Chem, 2014. 11(3): p. 307-315.
doi: 10.2174/1570193X1103140915111559
Anna Hordyjewska, A.O., Anna Horecka & Jacek Kurzepa Betulin and betulinic acid: triterpenoids derivatives with a powerful biological potential. Phytochemistry Reviews, 2019. 18: p. 929–951.
doi: 10.1007/s11101-019-09623-1
McMillin, M., et al., TGR5 signaling reduces neuroinflammation during hepatic encephalopathy. J Neurochem, 2015. 135(3): p. 565-76.
pubmed: 26179031 pmcid: 5031412 doi: 10.1111/jnc.13243
Jiao, S., et al., Betulinic acid protects against cerebral ischemia/reperfusion injury by activating the PI3K/Akt signaling pathway. Biomed Pharmacother, 2016. 84: p. 1533-1537.
pubmed: 27876208 doi: 10.1016/j.biopha.2016.11.028
Wang, D., et al., Betulinic acid protects the neuronal damage in new born rats from isoflurane-induced apoptosis in the developing brain by blocking FASL-FAS signaling pathway. Biomed Pharmacother, 2017. 95: p. 1631-1635.
pubmed: 28950663 doi: 10.1016/j.biopha.2017.09.028
Kaundal, M., et al., Betulinic acid, a natural PDE inhibitor restores hippocampal cAMP/cGMP and BDNF, improve cerebral blood flow and recover memory deficits in permanent BCCAO induced vascular dementia in rats. Eur J Pharmacol, 2018. 832: p. 56-66.
pubmed: 29778746 doi: 10.1016/j.ejphar.2018.05.015
Kaundal, M., R. Deshmukh, and M. Akhtar, Protective effect of betulinic acid against intracerebroventricular streptozotocin induced cognitive impairment and neuronal damage in rats: Possible neurotransmitters and neuroinflammatory mechanism. Pharmacol Rep, 2018. 70(3): p. 540-548.
pubmed: 29674241 doi: 10.1016/j.pharep.2017.11.020
Li, C., et al., Inhibitory Effects of Betulinic Acid on LPS-Induced Neuroinflammation Involve M2 Microglial Polarization via CaMKKbeta-Dependent AMPK Activation. Front Mol Neurosci, 2018. 11: p. 98.
pubmed: 29666569 pmcid: 5891622 doi: 10.3389/fnmol.2018.00098
Xu, S.H., et al., New 30-norlupane derivatives through chemical-microbial semi-synthesis of betulinic acid and their neuroprotective effect. Bioorg Med Chem Lett, 2020. 30(17): p. 127407.
Minassi, A., et al., Triterpenoid Hydroxamates as HIF Prolyl Hydrolase Inhibitors. J Nat Prod, 2018. 81(10): p. 2235-2243.
pubmed: 30350996 doi: 10.1021/acs.jnatprod.8b00514
Prados, M.E., et al., Betulinic acid hydroxamate prevents colonic inflammation and fibrosis in murine models of inflammatory bowel disease. Acta Pharmacol Sin, 2020.
Choudhry, H. and A.L. Harris, Advances in Hypoxia-Inducible Factor Biology. Cell Metab, 2018. 27(2): p. 281-298.
pubmed: 29129785 doi: 10.1016/j.cmet.2017.10.005
Di Conza, G., et al., The mTOR and PP2A Pathways Regulate PHD2 Phosphorylation to Fine-Tune HIF1alpha Levels and Colorectal Cancer Cell Survival under Hypoxia. Cell Rep, 2017. 18(7): p. 1699-1712.
pubmed: 28199842 pmcid: 5318657 doi: 10.1016/j.celrep.2017.01.051
Ehling, M., et al., B55alpha/PP2A Limits Endothelial Cell Apoptosis During Vascular Remodeling: A Complementary Approach To Disrupt Pathological Vessels? Circ Res, 2020. 127(6): p. 707-723.
pubmed: 32527198 doi: 10.1161/CIRCRESAHA.119.316071
Caterino, M., et al., Huntingtin protein: A new option for fixing the Huntington's disease countdown clock. Neuropharmacology, 2018. 135: p. 126-138.
pubmed: 29526547 doi: 10.1016/j.neuropharm.2018.03.009
Rebec, G.V., Corticostriatal network dysfunction in Huntington's disease: Deficits in neural processing, glutamate transport, and ascorbate release. CNS Neurosci Ther, 2018. 24(4): p. 281-291.
pubmed: 29464896 pmcid: 6489880 doi: 10.1111/cns.12828
Benarroch, E.E., Hypoxia-induced mediators and neurologic disease. Neurology, 2009. 73(7): p. 560-5.
pubmed: 19687457 doi: 10.1212/WNL.0b013e3181b2a719
Speer, R.E., et al., Hypoxia-inducible factor prolyl hydroxylases as targets for neuroprotection by "antioxidant" metal chelators: From ferroptosis to stroke. Free Radic Biol Med, 2013. 62: p. 26-36.
pubmed: 23376032 pmcid: 4327984 doi: 10.1016/j.freeradbiomed.2013.01.026
Yang, Y.T., T.C. Ju, and D.I. Yang, Induction of hypoxia inducible factor-1 attenuates metabolic insults induced by 3-nitropropionic acid in rat C6 glioma cells. J Neurochem, 2005. 93(3): p. 513-25.
pubmed: 15836611 doi: 10.1111/j.1471-4159.2005.03032.x
Niatsetskaya, Z., et al., HIF prolyl hydroxylase inhibitors prevent neuronal death induced by mitochondrial toxins: therapeutic implications for Huntington's disease and Alzheimer's disease. Antioxid Redox Signal, 2010. 12(4): p. 435-43.
pubmed: 19659431 pmcid: 2821149 doi: 10.1089/ars.2009.2800
Li, H.S., et al., HIF-1alpha protects against oxidative stress by directly targeting mitochondria. Redox Biol, 2019. 25: p. 101109.
Chi, O.Z., et al., Effects of erythropoietin on blood-brain barrier disruption in focal cerebral ischemia. Pharmacology, 2008. 82(1): p. 38-42.
pubmed: 18434762 doi: 10.1159/000127839
Bhattarai, D., X. Xu, and K. Lee, Hypoxia-inducible factor-1 (HIF-1) inhibitors from the last decade (2007 to 2016): A "structure-activity relationship" perspective. Med Res Rev, 2018. 38(4): p. 1404-1442.
pubmed: 29278273 doi: 10.1002/med.21477
Trettel, F., et al., Dominant phenotypes produced by the HD mutation in STHdh(Q111) striatal cells. Hum Mol Genet, 2000. 9(19): p. 2799-809.
pubmed: 11092756 doi: 10.1093/hmg/9.19.2799
Morrugares, R., et al., Phosphorylation-dependent regulation of the NOTCH1 intracellular domain by dual-specificity tyrosine-regulated kinase 2. Cell Mol Life Sci, 2020. 77(13): p. 2621-2639.
pubmed: 31605148 doi: 10.1007/s00018-019-03309-9
Chiva, C., et al., QCloud: A cloud-based quality control system for mass spectrometry-based proteomics laboratories. PLoS One, 2018. 13(1): p. e0189209.
Perkins, D.N., et al., Probability-based protein identification by searching sequence databases using mass spectrometry data. Electrophoresis, 1999. 20(18): p. 3551-67.
pubmed: 10612281 doi: 10.1002/(SICI)1522-2683(19991201)20:18<3551::AID-ELPS3551>3.0.CO;2-2
Beer, L.A., et al., Efficient Quantitative Comparisons of Plasma Proteomes Using Label-Free Analysis with MaxQuant. Methods Mol Biol, 2017. 1619: p. 339-352.
pubmed: 28674895 pmcid: 5575765 doi: 10.1007/978-1-4939-7057-5_23
Teo, G., et al., SAINTexpress: improvements and additional features in Significance Analysis of INTeractome software. J Proteomics, 2014. 100: p. 37-43.
pubmed: 24513533 doi: 10.1016/j.jprot.2013.10.023
Calzado, M.A., et al., An inducible autoregulatory loop between HIPK2 and Siah2 at the apex of the hypoxic response. Nat Cell Biol, 2009. 11(1): p. 85-91.
pubmed: 19043406 doi: 10.1038/ncb1816
Brouillet, E., et al., Partial inhibition of brain succinate dehydrogenase by 3-nitropropionic acid is sufficient to initiate striatal degeneration in rat. J Neurochem, 1998. 70(2): p. 794-805.
pubmed: 9453576 doi: 10.1046/j.1471-4159.1998.70020794.x
Fernagut, P.O., et al., Subacute systemic 3-nitropropionic acid intoxication induces a distinct motor disorder in adult C57Bl/6 mice: behavioural and histopathological characterisation. Neuroscience, 2002. 114(4): p. 1005-17.
pubmed: 12379255 doi: 10.1016/S0306-4522(02)00205-1
Ito, D., et al., Enhanced expression of Iba1, ionized calcium-binding adapter molecule 1, after transient focal cerebral ischemia in rat brain. Stroke, 2001. 32(5): p. 1208-15.
pubmed: 11340235 doi: 10.1161/01.STR.32.5.1208
Chen, S.D., et al., More Insight into BDNF against Neurodegeneration: Anti-Apoptosis, Anti-Oxidation, and Suppression of Autophagy. Int J Mol Sci, 2017. 18(3).
Sharp, F.R., et al., Hypoxic preconditioning protects against ischemic brain injury. NeuroRx, 2004. 1(1): p. 26-35.
pubmed: 15717005 pmcid: 534910 doi: 10.1602/neurorx.1.1.26
Kim, J.W., et al., HIF-1-mediated expression of pyruvate dehydrogenase kinase: a metabolic switch required for cellular adaptation to hypoxia. Cell Metab, 2006. 3(3): p. 177-85.
pubmed: 16517405 doi: 10.1016/j.cmet.2006.02.002
Deepak Bhatia, M.S.A., Qiwen Shi and Shahrzad Movafagh, Hypoxia and its Emerging Therapeutics in Neurodegenerative, Inflammatory and Renal Diseases, in Hypoxia and Human Diseases, C.Z. Jing Zheng, Editor 2017: Intechopen.
Awan, M.U., et al., Neuroprotective role of BNIP3 under oxidative stress through autophagy in neuroblastoma cells. Mol Biol Rep, 2014. 41(9): p. 5729-34.
pubmed: 24928088 doi: 10.1007/s11033-014-3444-7
Clark, A.R. and M. Ohlmeyer, Protein phosphatase 2A as a therapeutic target in inflammation and neurodegeneration. Pharmacol Ther, 2019. 201: p. 181-201.
pubmed: 31158394 pmcid: 6700395 doi: 10.1016/j.pharmthera.2019.05.016
Chang, K.H., et al., Plasma inflammatory biomarkers for Huntington's disease patients and mouse model. Brain Behav Immun, 2015. 44: p. 121-7.
pubmed: 25266150 doi: 10.1016/j.bbi.2014.09.011
Dobrogowska, D.H., et al., Increased blood-brain barrier permeability and endothelial abnormalities induced by vascular endothelial growth factor. J Neurocytol, 1998. 27(3): p. 163-73.
pubmed: 10640176 doi: 10.1023/A:1006907608230
Sondell, M., G. Lundborg, and M. Kanje, Vascular endothelial growth factor has neurotrophic activity and stimulates axonal outgrowth, enhancing cell survival and Schwann cell proliferation in the peripheral nervous system. J Neurosci, 1999. 19(14): p. 5731-40.
pubmed: 10407014 pmcid: 6783109 doi: 10.1523/JNEUROSCI.19-14-05731.1999
Jin, K.L., X.O. Mao, and D.A. Greenberg, Vascular endothelial growth factor rescues HN33 neural cells from death induced by serum withdrawal. J Mol Neurosci, 2000. 14(3): p. 197-203.
pubmed: 10984196 doi: 10.1385/JMN:14:3:197
Ellison, S.M., et al., Dose-dependent neuroprotection of VEGF(1)(6)(5) in Huntington's disease striatum. Mol Ther, 2013. 21(10): p. 1862-75.
pubmed: 23799534 pmcid: 4059596 doi: 10.1038/mt.2013.132
Bjorkqvist, M., et al., A novel pathogenic pathway of immune activation detectable before clinical onset in Huntington's disease. J Exp Med, 2008. 205(8): p. 1869-77.
pubmed: 18625748 pmcid: 2525598 doi: 10.1084/jem.20080178
Palpagama, T.H., et al., The Role of Microglia and Astrocytes in Huntington's Disease. Front Mol Neurosci, 2019. 12: p. 258.
pubmed: 31708741 pmcid: 6824292 doi: 10.3389/fnmol.2019.00258
Ben Haim, L., et al., Elusive roles for reactive astrocytes in neurodegenerative diseases. Front Cell Neurosci, 2015. 9: p. 278.
pubmed: 26283915 pmcid: 4522610 doi: 10.3389/fncel.2015.00278
Franco, R. and D. Fernandez-Suarez, Alternatively activated microglia and macrophages in the central nervous system. Prog Neurobiol, 2015. 131: p. 65-86.
pubmed: 26067058 doi: 10.1016/j.pneurobio.2015.05.003
Zuccato, C. and E. Cattaneo, Role of brain-derived neurotrophic factor in Huntington's disease. Prog Neurobiol, 2007. 81(5-6): p. 294-330.
pubmed: 17379385 doi: 10.1016/j.pneurobio.2007.01.003
Ciammola, A., et al., Low brain-derived neurotrophic factor (BDNF) levels in serum of Huntington's disease patients. Am J Med Genet B Neuropsychiatr Genet, 2007. 144B(4): p. 574-7.
pubmed: 17427191 doi: 10.1002/ajmg.b.30501
Islam, M.T., Oxidative stress and mitochondrial dysfunction-linked neurodegenerative disorders. Neurol Res, 2017. 39(1): p. 73-82.
pubmed: 27809706 doi: 10.1080/01616412.2016.1251711
Damiano, M., et al., Mitochondria in Huntington's disease. Biochim Biophys Acta, 2010. 1802(1): p. 52-61.
pubmed: 19682570 doi: 10.1016/j.bbadis.2009.07.012

Auteurs

María E Prados (ME)

Emerald Health Biotechnology, Cordoba, Spain.

Alejandro Correa-Sáez (A)

Instituto Maimónides de Investigación Biomédica de Córdoba (IMIBIC), Cordoba, Spain.
Department of Cellular Biology, Physiology and Immunology, University of Cordoba, Cordoba, Spain.
Hospital Universitario Hospital Reina Sofia, Cordoba, Spain.

Juan D Unciti-Broceta (JD)

Emerald Health Biotechnology, Cordoba, Spain.

Martín Garrido-Rodríguez (M)

Instituto Maimónides de Investigación Biomédica de Córdoba (IMIBIC), Cordoba, Spain.
Department of Cellular Biology, Physiology and Immunology, University of Cordoba, Cordoba, Spain.
Hospital Universitario Hospital Reina Sofia, Cordoba, Spain.

Carla Jimenez-Jimenez (C)

Instituto Maimónides de Investigación Biomédica de Córdoba (IMIBIC), Cordoba, Spain.
Department of Cellular Biology, Physiology and Immunology, University of Cordoba, Cordoba, Spain.
Hospital Universitario Hospital Reina Sofia, Cordoba, Spain.

Massimiliano Mazzone (M)

Laboratory of Tumor Inflammation and Angiogenesis, Center for Cancer Biology, VIB-KULeuven, 3000, Leuven, Belgium.

Alberto Minassi (A)

Department of Drug Science, University of Piemonte Orientale, Novara, Italy.

Giovanni Appendino (G)

Department of Drug Science, University of Piemonte Orientale, Novara, Italy.

Marco A Calzado (MA)

Instituto Maimónides de Investigación Biomédica de Córdoba (IMIBIC), Cordoba, Spain. mcalzado@uco.es.
Department of Cellular Biology, Physiology and Immunology, University of Cordoba, Cordoba, Spain. mcalzado@uco.es.
Hospital Universitario Hospital Reina Sofia, Cordoba, Spain. mcalzado@uco.es.

Eduardo Muñoz (E)

Instituto Maimónides de Investigación Biomédica de Córdoba (IMIBIC), Cordoba, Spain. fi1muble@uco.es.
Department of Cellular Biology, Physiology and Immunology, University of Cordoba, Cordoba, Spain. fi1muble@uco.es.
Hospital Universitario Hospital Reina Sofia, Cordoba, Spain. fi1muble@uco.es.

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