A Comparative Study between Different Tunisian Propolis Essential Oils and Their Antioxidant Activities

Document Type : Research Article


Laboratoire Matériaux Molécules et Applications, Institut Préparatoire des Etudes Scientifiques et Techniques, IPEST, BP 51, 2070 La Marsa, TUNISIA


Propolis is a resinous substance collected by bees from plants with a complex and variable chemical composition. Propolis and its fractions possess multiple biological activities. This study focused on a chemical and statistical comparison between four Tunisian Propolis Essential Oils (PEO) and its antioxidant activities. Volatile oils were extracted by hydrodistillation and analyzed by GC-MS. Essential oil yield varied from 0.095% to 0.324%. A total of 59 volatile components were identified mainly dominated by sesquiterpenes and diterpenes hydrocarbons. Six major components were found in all samples collected from the four different locations α-Cedrol, Manoyl Oxide, Manool, Totarol, Tricosane, and Eicosane. The antioxidant activities of Tunisian propolis essential oils have been evaluated using two methods: β-carotene-linoleic acid bleaching and DPPH radical scavenging assays and the results were compared with the standard antioxidant (Triolox). PEO from Bizerte region presented a lower IC50 value (30.5 mg/mL) than that of the standard antioxidant Trolox (IC50 = 40.05 mg/mL) indicating high antioxidant capacity using DPPH assay but for the b-carotene-linoleic acid bleaching assay, PEO from Zouarine region had the lowest value of (IC50 = 26.5 mg/mL) compared to standard (IC50 = 31.25 mg/mL). Our findings demonstrated that Propolis Essential Oil (PEO) possess high antioxidant activities and may be suggested as a new potential source of natural antioxidant.


Main Subjects

[1] Greenaway W., Scaysbrook T., Whatley F.R., The Composition and Plant Origins of Propolis:
A Report of Work at Oxford
, Bee World, 71: 107-118 (1990).
[2]Ghisalberti E.L.,Propolis: a Review, Bee World, 60: 59-84 (1979).
[3] Bankova.V., Christov R., Popov S., Pureb O., Bocari G., Volatile Constituents of Propolis, Zeitschrift Für Naturforschung C, 49c: 6 - 10 (1994).
[4] Bankova V., Christov R., Popov S., Marcucci M.C., Antibacterial Activity of Essential Oils from Brazilian Propolis, Fitoterapia, 70: 190-193 (1999).
[5] Toress R.N.S., Dantas Lopes J.A., Machado Moia Neto J.M., Dasgraças Lopes Cito A. M., The Volatile Constituents of Propolis from Piaui, Quimica.Nova, 31(3): 479-485 (2008).
[6] Borcic I., Radonic A., Grzunov K., Comparison of the Volatile Constituents of Propolis Gathered
in Different Regions of Croatia
, Flavour and Fragrance Journal, 11: 311-313(1998).
[7] Melliou E., Stratis E., Chinou I., Volatile Constituents of Propolis from Various Regions of Greece - Antimicrobial Activity, Food. Chem., 103: 375-380 (2007).
[8] Naik D.G., Vaidya H.S., Namjoshi T.P., Essential Oil Of Indian Propolis: Chemical Composition and Repellency Against the Honeybee Apisflorea, Chembiodiv, 10: 649–657 (2013).
[9] Segueni N., Khadraoui F., Moussaoui F., Zellagui A., Guerraf N., Lahouel M., Rhouati S., Volatiles Constituents of Algerian Propolis, Annal. of Biological Research, 103-107 (2010).
[10] Bankova V., De Castro S.L., Marcucci  M.C., Propolis: Recent Advances In Chemistry And Plant Origin, Apidologie, 31, 3-15 ( 2000).
[11] Danlami J., Arsad A., Ahmad Zaini M., A Comparative Study of Various Oil Extraction Techniques from Plants, Reviews In Chemical Engineering, 30(6): 605-626 (2014).
[12] Tuan D.Q., Ilangantileke S.G., Liquid CO2 Extraction of Essential Oil from Star Anise Fruits (Illicium Verum H.), Journal of Food Engineering, 31: 47–57 (1997). 
[13] Bimakr M., Rahman R.A., Ganjloo A., Taip F.S., Saleh L.M., Sarker Z.I., Optimization of Supercritical Carbon Dioxide Extraction of Bioactive Flavonoid Compounds from Spearmint (Mentha Spicata L.) Leaves by Using Response Surface Methodology, Food Bioprocess Technol., 5: 912–920 (2012).
[14] Sajfrtová M., Ličková I., Wimmerová M., Sovová H., Zdeněk W., Β-Sitosterol: Supercritical Carbon Dioxide Extraction from Sea Buckthorn (Hippophae Rhamnoides L.) Seeds, Int. J. Mol. Sci., 11: 1842–1850 (2010).
[15] Golmohamadi A., Möller G., Powers J., Nindo C., Effect of Ultrasound Frequency on Antioxidant Activity, Total Phenolic and Anthocyanin Content of Red Raspberry Puree, Ultrason Sonochem, 20: 1316–1323 (2013).
[16] Shah M.V., Rohit M.C., Novel Techniques for Isolation and Extraction of Phytoconstituents From Herbal Plants, Am. J. Phytomed. Clin. Ther., 1: 338–350 (2013).
[17] Bankova V., Dyulgerov A., Popov S., Evstatieva L., Kuleva L., Purb O., Zamjansan Z., Propolis Produced in Bulgaria and Mongolia: Phenolic Compounds and Plant Origin, Apidologie, 23: 79-85 (1992).
[18] Marcucc. M.C., Ferreres F., Garc´Ia-Vigueira C., Bankova V.S., De Castro S.L., Dantas A.P.,
Valente P.H.M., Paulino N., Phenolic Compounds from Brazilian Propolis with Pharmacological Activities, Journal of Ethnopharmacol, 74: 105-112 (2001).
[19] Zhao Q., Zhan B., Zhou W., Guo Z., Study of Essential Oils of Propolis by Microwave Assisted Extraction Coupled with GC/MS, Fine Chem, 12: 1129-1195 ( 2007).
[21] Emmons C.L., Peterson D.M., & Paul G. L., Antioxidant Capacity of Oat (Avena Sativa L.) Extracts. 2. in Vitro Antioxidant Activity and Content of Phenolic and Tocol Antioxidants, Journal of Agricultural and Food Chemistry, 47: 4894–4898 (1999).
[22] Hanato T., Kagawa H., Yasuhara T., Okuda T., Two New Flavonoids and Other Constituents in Licorice Root: their Relative Astringency and Radical Scavenging Effect, Chem Pharm Bull, 36:1090–1097 (1988).
[23]European Pharmacopoeia, Vol. 3, Pp. 68-71,  Maisonneuve SA, Sainte-Rufine (1975).
[25] Bankova V., Recent Trends and Important Developments in Propolis Research, Comprehensive Alternative Medicine, 2, 29–32 (2005).
[26] Barbouche N., “La Filière Apicole En Tunisie, Situation, Contraintes Et Perspectives”, Institut National D’agriculture, Barkane 15-17 Octobre, (2009)
[28] Loizzo M.R.,Ben Jemia M., Senatore F., Bruno M., Menichini F., Tundis R., Chemistry and Functional Properties in Prevention of Neurodegenerative Disorders of Five Cistus Species Essential Oils, Food Chem. Toxicol, 59, 586–594 (2013). 
[30] Hanana M., Bejia A., Amri I., Gargouri S., Jamoussi B., Hamrouni L., Activités Biologiques Des Huiles Essentielles De Pins, Journal of New Sciences, Volume 4(3) (2014).
[31] Zammita E.J., Theumab K.B., Darmaninb S., Muraglia M., Camilleri-Podesta M.T., Buhagiard J.A., Calleja-Agiusb J., Adamia M.Z., Micallefe M., Franchinic C., Schembri-Wismayerb P., Totarol Content and Cytotoxicity Varies Significantly In Different Types of Propolis, Research Journal of Pharmaceutical, Biological and Chemical Sciences, 4(3): 1047-1058 (2013).
[32] Chen C.W.,Ho C.T., Antioxidant Properties of Polyphenols Extracted From Green and Black Tea, Journal of Food Lipids, 2, 35-46 (1995).
[34] Monique R., Moreira Ariana B., Souza Maísa A., Moreira Thamires C., Bianchi Luiza J., Carneiro Fernanda T., Estrela Raquel A., Dos Santos Ana H., Januário Carlos H.G., Martins Sérgio R., Ambrosio, Rodrigo C.S., Veneziani, RP-HPLC Analysis of Manool-Rich Salvia Officinalis Extract Andits Antimicrobial Activity Against Bacteria Associated with Dental Caries, Rev Bras Farma, 23: 870-876 (2013).
[35] Pratsinis H., Kletsas D., Melliou E., Chinou I., Antiproliferative Activity of Greek Propolis, Journal Of Medicinal Food, 13:286-290 (2010).
[36] Janas K., Bumba V., Contribution To Composition of Beeswax Propolis, Pharmazie, 29: 544–545 (1974).
[37] Pellati F., Prencipe F.P., Benvenuti S., Headspace Solid-Phase Micro Extraction-Gas Chromatography–Mass Spectrometry Characterization of Propolis Volatile Compounds, Journal Pharmbiomed Anal, 84:103–111 (2013).
[38] Oliveira A.P., França H.S., Custeer R.M., Teixeira L.A., Rocha L.M., Chemical Composition And Antibacterial Activity of Brazilian Propolis Essential Oil, J Venomous Animals Toxins Include Trop Dis, 16:121–130 (2010).
[39] Kaškoniene V., Kaškonas P., Maruška A., Kubiliene L., Chemometric Analysis of Volatiles of Propolis from Different Regions Using Static GC-MS, Cent. Eur. J. Chem., 12: 736–746 (2014).
[40] Bankova V., Christov R., Delgado Tejera A., Lignans and other Constituents of Propolis From Canary Islands, Phytochemistry, 49:1411–1415 (1998).
[41] Singh R.P., Murthy K.N.C., Jayaprakasha G.K., Studies on Antioxidant Activity of Pomegranate (Punicagranatum) Peel and Seed Extracts Using in Vitro Models, J Agric Food Chem, 50:81-86 (2002).
[42] Tepe B., Sokmen M., Akpulat H.A., Daferera D., Polissiou M., And Sokmen A., Antioxidative Activity of the Essential Oils of Thymus Sipyleus Subsp. Sipyleus Var. Sipyleus and Thymussipyleussubsp. Sipyleus Var. RosulansJournal of Food Engineering, 66, No. 4, Pp. 447–454 (2005).
[43] Tepe B., Donmez E., Unlu M., Candan F., Daferera D., Vardar-Unlu G., Polissiou M., Sokmen A., Antimicrobial and Antioxidative Activities of the Essential Oils and Methanol Extracts of Salvia Cryptantha (Montbret Et Aucher Ex Benth.) and Salvia Multicaulis (Vahl), Food Chem, 84: 519-525 (2004).
[44] Dapkevicius A., Van Beek T.A., Lelyveld G.P., Van Veldhuizen A., De Groot A., Linssen JPH, Isolation and Structure Elucidation of Radical Scavengers from Thymus Vulgaris Leaves, Journal of Natural Products, 65(6): 892–896 (2002).
[46] Agüero M.B., Svetaz L., Sánchez M., Luna L., Lima B., López M.L., Zacchino S., Palermo J., Wunderlin D., Feresin G.E., Tapia A., Argentinean Andean Propolis Associated with the Medicinal Plant Larreanitida Cav. (Zygophyllaceae). HPLC–MS and GC–MS Characterization and Antifungal Activity, Food Chem. Toxicol., 49: 1970–1978 (2011).
[47] Miguel M.G., Nunes S., Cruz C., Duarte J., Antunes M.D., Cavaco A.M.M., Mendes D., Lima A.S., Pedro L.G., Barroso J.G., Figueiredo A.C., Propolis Volatiles Characterisation from Acaricide-Treated and Untreated Beehives Maintained at Algarve (Portugal), Natural Prod Research, 27: 743–749 (2013).
[48] Akrout A., Etude Des Huiles Essentielles De Quelques Plantes Pastorales De La Région De Matmata (Tunisie), Cahiers Options Méditerranéennes, 62: 289-292 (2001).
[49] Nixon D.,Hobbs D.C., The Use of Totarol to Treat Acne in an Adolescent: a Case Study, Case report NZFP, 33(4):253-256 (2006).