Food Chemistry 129 (2011) 171–174

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Food Chemistry
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Antioxidant effect of essential oils of rosemary, clove and cinnamon on hazelnut and poppy oils
Mehmet Musa Özcan ⇑, Derya Arslan
Department of Food Engineering, Faculty of Agriculture, Selcuk University, 42031 Konya, Turkey

a r t i c l e

i n f o

a b s t r a c t
Antioxidant effects of essential oils from rosemary (Rosmarinus officinalis), clove (Syzygium aromaticum) and cinnamon (Cinnamomum zeylanicum) were determined on hazelnut and poppy oils. These essential oils were added to the oils at concentrations of 0.25% and 0.5%. Butylated hydroxyanisole (BHA) at 0.02% level served as standard besides the control groups for comparison. The samples were stored 50 °C in darkness for 14 days. The antioxidant activity of the essential oils was determined by measuring peroxide values (meq O2/kg oil) at regular intervals. On the basis of peroxide value assay, the essential oils showed stronger antioxidant effect when compared to control groups. BHA was more effective than the essential oils, whilst it exhibited no antioxidative effect on the first few days of storage. Amongst the investigated essential oils, the cinnamon oil was the most effective on retarding lipid oxidation of crude oils, which was followed by clove and rosemary oils. Ó 2011 Published by Elsevier Ltd.

Article history: Received 26 September 2009 Received in revised form 4 October 2010 Accepted 1 January 2011 Available online 22 January 2011 Keywords: Antioxidant effect Spice Essential oil Hazelnut oil Poppy oil

1. Introduction Antioxidants commonly used in food products today are butylated hydroxyanisole (BHA) and butylated hydroxytoluene (BHT). In recent years the safety of synthetic food additives, including the possible toxicity of these chemicals used as antioxidants has received increasing attention. So, there is need for other components to act as antioxidants and to render food products safer for mankind (Branen, 1975; Kahl & Kappus, 1993). As it is known, mainly the edible oils, fats and fatty foods can undergo deterioration in the course of the time depending on external factors such as heat, light, enzyme and trace metals. As a result of autoxidation especially which occurs with the effect of oxygen in the air, unpleasant taste and smell that are known as the signs of rancidity in oil occur. Autoxidation is an irreversible reaction which goes on spontaneously when it begins, and its rate is directly related to the oil’s unsaturation degree. The breakdown products formed after oxidation process such as peroxides, aldehydes and ketones shorten the shelf life of oils and turn products unacceptable for consumption (Akgül, 1989; Shahidi & Nazck, 1995). As a conclusion of these researches, in order to overcome the stability problems of oils and fats synthetic antioxidants, most of which have phenolic characteristic, such as BHA, BHT, ter-butyl hydroquinone (TBHQ) and gallates have been used as food additives for many years (Akgül, 1989; De Man, 1980). But recent reports reveal that these compounds may be implicated in many
⇑ Corresponding author. Tel.: +90 332 2232933; fax: +90 332 2410108.
E-mail address: (M.M. Özcan). 0308-8146/$ - see front matter Ó 2011 Published by Elsevier Ltd. doi:10.1016/j.foodchem.2011.01.055

health risks (Özcan & Akgül, 1995). For example, BHT causes liver expansion (Akgül, 1989). Also, it is well known that these compounds cause unpleasant taste and smells as they easily vaporise and degrade (Akgül, 1989; Özcan & Akgül, 1995). To prevent these harmful effects of synthetic antioxidants, the use of antioxidants which are found in foods and various natural materials is recommended (Özcan & Akgül, 1995). Researches on rosemary show that compounds which have antioxidant characteristic have phenol character and flavonoids occupy an important part in them (Decker, 1997). On the other hand, it was reported that eugenol which is found in clove and cinnamon essential oils is an effective antioxidant compound in the researches (Farag, Badei, Hewedi, & ElBaroty, 1989a). It is doubtless, this effect is the result of eugenol’s phenolic structure (Weidenbörner, Hindrof, & Tsotsonos, 1990). The antioxidative effects of natural antioxidants on lipids were studied in recent years as a popular research area. Some of the effective factors on the antioxidative mechanism of natural compounds on lipids were expressed as the emulsion type of the system (Frankel, Huang, & Aeschbach, 1997; Hopia, Huang, Schwarz, German, & Frankel 1996), antagonistic and synergistic effects (Medina, Tombo, Satuè-Gracia, German, & Frankel, 2002; Özcan, 1999; Özcan, 2000), temperature (Sature, Huang, & Frankel, 1995), concentration, hydrophilic or the lipophilic tendency of the system (Frankel, Huang, Aeschbach, & Prior, 1996; Schwarz et al., 2000) and the number and the place of connection of the hydroxyl groups in aromatic cycle (Chen, Chan, Ho, Fung, & Wang, 1996; Das & Pereira, 1990). Overall strongest activity of rosemary was not surprising because of various findings reported on its stabilising effect (Chang,

4 12.7 23 ± 1.9 20. Lee. Ho.3 19.5 ± 1.5 and 1. 1993).5 ± 1. cinnamon.M.9 11.8 24 ± 1. A lot of studies were carried out on antioxidants characteristics of several plants and corresponding derivatives such as essential oil and extracts. Wu. & Chang. The extracted oil was dried over anhydrous sodium sulphate.3 22 ± 2.25 0.4.2 9 ± 0. Preparation of essential oil Essential oils of the samples were obtained by hydrodistillation method. The plant materials (about 100 g) were ground into small pieces and were placed in a flask (2 L) together with double distilled water (1. It is believed that detection of natural antioxidant sources and proper consumption of them in daily diet or use of isolated compounds in clinical practices would be beneficial for healthy life (Farag.). Ho.3 10.6 25 ± 1. Material and methods 2.5 ± 1.5 ± 1. Fifteen grams of each sample were stored in 10 Â 100 mm open beakers at 50 °C in the dark.5 ± 1.2 19 ± 1. The liberated iodine was titrated with sodium thiosulphate solution (0.4 6 ± 0.5 ± 2. and El-Baroty (1989b) reported that clove and thyme essential oils exhibited antioxidant activity in refined cotton seed oil.5 ± 0. Butylated hydroxyanisole Synthetic antioxidant (Sigma) was preferred because of its common usage at vegetable oil producing companies to retard the oxidation.7 25 ± 0.8 14.02%.4 85 ± 4.1 50 ± 3. Sui. although they have been extensively examined for their medicinal. carnosic and ursolic acids etc.2 0. 1982).50 0.1 12 ± 1.1a 11.9 11 ± 0. and saturated solution of KI (1 mL) was then added.5 11 ± 1. Statistical analyses 2. Özcan. 2.50 0.5 ± 2. cinnamon and clove essential oils on the peroxide value (meq O2/kg oil) of hazelnut oil stored at 50 °C in darkness. Nakatani.8 60 ± 3. 1990).50% and dissolution was obtained by manual homogenisation for about 5 minutes. After the 10th day.5. Statistical analyses were performed using a one-way analysis of variance. Plant material The samples [rosemary (Rosmarinus officinalis) leaves.3 75 ± 4. 3. 2.4 35 ± 4. 1989). Hewedi. On the third day of the assay. Recently.1. Kramer (1985) has identified eugenol as one of the major antioxidants present in clove.6. Badei. The samples were transported in polypropylene bags. The mixture was boiled for 4 h. culinary and antimicrobial properties (Akgül. with clove oil being superior to thyme oil.2 15 ± 1.5 ± 0.5% level of all essential oils on hazelnut oil maintained their antioxidant activity. A control sample was prepared under the same conditions without addition of any antioxidant. and related active components such as carnosol. All essential oils were kept at freezing temperature (À18 °C) until used for the analysis. Results and discussion 2. Badei. 1985. Antioxidant activities of rosemary. clove and cinnamon oils were slightly weaker when compared to BHA added samples. After 10 days. respectively. & Fuwa.025% and 0. 0. Antioxidants are the most effective compounds against free radicals. A clear antioxidant effect of the essential oils was not observed on both hazelnut and poppy oils until the 10th day of storage when it is compared to control samples (Tables 1 and 2). 1983. The extract was condensed in cooling vapour to collect the essential oil of each material. rosmanol.3 14 ± 1.8 Mean ± standard deviation.5 ± 1.5 ± 0.8 47 ± 3. Hazelnut and poppy oils Natural hazelnut and poppy oils without adding any antioxidant were kindly supplied by cool press processing.4 11.7 40 ± 2.5 ± 1.8 26 ± 2.6 11.9 38.5 ± 0. D.50 0.1 38.5 ± 1. 1989a). & Ho 1992. Inatoni. Arslan / Food Chemistry 129 (2011) 171–174 Ostric-Matijasvic. and were dried to constant weight in room temperature for analyses.05 was considered significant _ (Püskülcü & Ikiz. & El-Baroty.5 L).8. pollution. antioxidant effect increased together with essential oil concentration.1 22.5 ± 2. stress and industrial food consumption increased the existence of free radicals. For the determination of peroxide number.25 0. & Hsieh.7 10 57. 2. On the other hand. clove essential oils’ antioxidant effects on hazelnut and poppy oil stored at 50 °C in darkness.2 7 18. exhibiting a marked effect in comparison with BHA (Table Table 1 The effect of rosemary. . Little is known about the extent to which the spice essential oils may contribute to the antioxidant activity.2. 2.2 14 80 ± 4.172 M. Farag.25 0.3. all the oils showed antioxidant effect in varying degrees on hazelnut oil.5 ± 1. Concentrations (%) Days 3 Rosemary Cinnamon Clove BHA Control a 5 12. clove (Syzygium aromaticum) buds and cinnamon (Cinnamomum zeylanicum) barks] were purchased from local market in Konya in Turkey. 1977). Peroxide values (meq O2/kg oil) of poppy and hazelnut oils were 1. essential oil showed antioxidant effect at various degrees (Fig 1. A calculated quantity of the BHA and essential oils were added directly to the hazelnut and poppy oils at room temperature with the concentrations of 0.v/v). a given weight of hazelnut and poppy oils were dissolved in a mixture of acetic acid:chloroform (CH3COOH:CHCl3) (3:2. 0. at the beginning of experiment. The purpose of this work was to determine rosemary. & Chang. A probability value of P < 0. Antioxidant activity measurement The rate of oxidation was monitored by periodic determination of peroxide values of the oil stored at 50 °C by using essential oils.2 10 ± 0. Antioxidant effects of the spice essential oils on hazelnut and poppy oils were given in Tables 1 and 2. (Chen. Houlihan.2 15.01 N) in the presence of starch as an indicator (AOCS.02 14.7 ± 2.

They reported the results as 0.5 ± 4. and Tikkanen (2003) determined the free radical scavenging activities of the aqueous extracts of O. officinalis obtained from Finland. officinalis and S.M. Hewedi. Lagouri.5 ± 25.5 332. Özcan.50 0.3 19 ± 2.6 34 ± 3.3 78.5 ± 3. Özcan and Akgül (1995) re- ported the antioxidant effects of the same spice volatile oils in sun flower oil in their study with an order like: summer savory > rosemary > sage > marjoram > oregano > anise > tarragon.335.236 and 0.5 ± 28.7 11. The effect of rosemary.4 62 ± 3. 1).2 34 ± 3. cinnamon essential oil showed the highest effect. the effect was at a very limited level.1 575 ± 17. and they reported that the essential oils and their main components showed much higher antioxidant effect than BHA.25% Clove 0.5 35 ± 3. Hiltunen.5 ± 12. vulgare L. Tsimidou. carnosic acid. cinnamon and clove essential oils on the peroxide value (meq O2/kg oil) of poppy oil stored at 50 °C in darkness.3 413 ± 28. and Boskou (1993) tested four Labiatae plant essential oils and carvacrol and thymol as the main components of the essential oils from this plant species in lard which was stored at 35 °C. The same level of this essential oil was effective on control group.7 30 ± 4.5 ± 33.2 10 207.7 231. As it is seen on Table 1. Blekas.6 14 537. Kokkini.6 234 ± 21.M.25 0. peroxide value (meq O2/kg oil) 90 80 70 60 50 40 30 20 10 0 1 (a) 2 3 4 5 6 7 8 days 9 10 11 12 13 14 15 Rosemary 0.1 33.6 19. Concentrations (%) Days 3 Rosemary Cinnamon Clove BHA Control a 173 5 31. Farag..1 36 ± 3. In contrast.8 523. respectively. and a-tocopherol were significantly more active than carnosol.3 18.25 0.50% Cinnamon 0.50 0. the rosemary extract.6 87.25% BHA 0.4 552.5 ± 5.7 71.2 85 ± 4.50 0.2 240 ± 23.1 76 ± 4.8 812. and El-Baroty (1989a) found the antioxidant effects of some spice essential oil in linoleic acid which emulsified in aqueous phase following the order like.1 34 ± 2. 0. The highest antioxidant activity was exhibited by 0.5 ± 2.4 138 ± 15.02 18.6 472 ± 22.5 ± 1. D.5 ± 1. the rosemary .2 7 88 ± 6.25% 900 800 700 600 500 400 300 200 100 0 1 2 3 4 Rosemary 0. too.4a 20 ± 2.5 ± 3. cinnamon and clove essential oils on the peroxide value (meq O2/kg oil) of hazelnut (a) and poppy (b) oils stored at 50 °C in darkness.5 ± 13. R.5% concentration of clove oil (Fig 1). All of spice essential oils were effective at 50 °C in comparison with control.5 ± 4. Antioxidant effect of 0.4 0.50% Control peroxide value (meq O2/kg oil) (b) 5 6 7 8 days 9 10 11 12 13 14 15 Fig.3 ± 2.3 565 ± 24. When antioxidant effect of essential oils were compared for hazelnut and poppy oils. Arslan / Food Chemistry 129 (2011) 171–174 Table 2 The effect of rosemary. clove > thyme > rosemary > cumin > sage > frenk cumin.4 20.02% Cinnamon 0. Peltoketo. In bulk corn oil.5 ± 32. their effect was more remarkable for poppy oils (Table 2). Badei.5 ± 27.5% level of clove oil was found higher compared to that of other essential oils (Table 2). Dorman. rosmarinic acid. 1.6 Mean ± standard deviation.5 ± 21.2 305 ± 26. But when it was compared to BHA.6 19 ± 3.50% Clove 0.4 287.1 22 ± 4.25 0.5 ± 1. in corn oil-in-water emulsion.265 (IC50 [mg/ml]).

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