Journal of Ethnopharmacology ] (]]]]) ]]]–]]] Contents lists available at SciVerse ScienceDirect Journal of Ethnopharmacology journal homepage: www.elsevier.com/locate/jep Anti-inflammatory and anti-nociceptive properties of Prunus padus Jae Hyuk Choi, Dong Seok Cha, Hoon Jeon n College of Pharmacy, Woosuk University, Jeonbuk 565-701, Republic of Korea a r t i c l e i n f o abstract Article history: Received 27 April 2012 Received in revised form 12 September 2012 Accepted 16 September 2012 Ethnopharmacological relevance: Prunus padus Linne has been widely used as a traditional medicine, with beneficial effects in numerous diseases, including stroke, neuralgia and hepatitis. In this study, we demonstrated anti-inflammatory and anti-nociceptive activities of the methylene chloride fraction of P. padus (MPP). Materials and methods: In vitro studies, the anti-inflammatory effects of MPP were examined using IFN-g/LPS-activated murine peritoneal macrophage model. To confirm the anti-inflammatory effects of MPP in vivo, trypsin-induced paw edema test was also conducted. The anti-nociceptive activities of MPP were measured using various experimental pain models including thermal nociception methods such as the tail immersion test and the hot plate test as well as chemical nociception methods like acetic acid-induced writhing test and formalin test. To determine whether analgesic activity of MPP is connected with the opioid receptor, we carried out combination test with naloxone, a nonselective opioid receptor antagonist. Results: In the current study, MPP showed potent inhibitory effect on IFN-g/LPS-induced NO production. MPP also suppressed not only iNOS enzyme activity but also iNOS expression. Moreover, MPP inhibited COX-2 expression dose dependently. IFN-g/LPS stimulation induced the translocation of NF-kB to nucleus but it was attenuated in the presence of MPP. In vivo study revealed that MPP could reduce paw volume after subplantar injection of trypsin. In addition, MPP showed potent analgesic activities both thermal and chemical nociception compared to tramadol and indomethacin. Furthermore, pre-treatment of naloxone slightly suppress the analgesic activity of MPP indicating that MPP acts as a partial opioid receptor agonist. Conclusions: In the present study, MPP showed potent anti-inflammatory properties through not only by suppressing various inflammatory mediators in vitro, but reducing the inflammatory edema in vivo. MPP also exhibited strong anti-nociceptive activities via both central and peripheral mechanism by acting as a partial opioid agonist. Based on these results we suggest that P. padus has the potential to provide a therapeutic approach to inflammation-mediated chronic diseases as an effective antiinflammatory agent and painkiller. & 2012 Elsevier Ireland Ltd. All rights reserved. Keywords: Prunus padus Anti-inflammatory Anti-nociceptive 1. Introduction Inflammation is an important host defense mechanism and can be characterized by redness, swelling, pain, heat and dysfunction of the tissue and organs (Lawrence et al., 2002). Against outer stimuli or tissue injury, the host activates cellular immune responses that increase production of pro-inflammatory mediators including nitric oxide (NO) and prostaglandins (PGs). Previous studies have demonstrated that excessive production of NO and PGs participates in inflammatory diseases including rheumatoid arthritis, asthma and cancer as well as nociceptive events (Holthusen and Arndt, 1994; Rakel and Rindfleisch, 2005). High levels of NO and PGs are n Corresponding author. Tel.: þ82 63 290 1577; fax: þ82 63 290 1576. E-mail address: hoonj6343@hanmail.net (H. Jeon). produced by inducible enzymes such as inducible nitric oxide synthase (iNOS) and cyclooxygenase-2 (COX-2), respectively (Kimura et al., 1998; Jeong and Jeong, 2010). Therefore, inhibition of iNOS and COX-2 expression can be an attractive therapeutic target for treating inflammatory diseases (Bogdan, 2001). Pain is an unpleasant sensory and emotional experience associated with actual or potential tissue damage (IASP, 1979). Since pain enables immediate awareness of actual or threatening injuries, it is essential for the survival of an organism (Bromm and Lorenz, 1998). However, continuous nociception in the absence of a detectable stimulus needs a proper pain management. In this regards, many studies have attempted to find effective analgesic agent originating from traditional plant-derived medicines with high efficiency and low toxicity (Calixto et al., 2000). Prunus padus Linne is a plant in a family of Rosaceae and sometimes referred as ‘bird cherry’, distributed in Korea, Japan 0378-8741/$ - see front matter & 2012 Elsevier Ireland Ltd. All rights reserved. http://dx.doi.org/10.1016/j.jep.2012.09.023 Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 2 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] and China. This plant has been used as a traditional medicine for the treatment of edema, stroke, neuralgia and hepatitis. Previous phytochemical analysis revealed that P. padus has anthocyanins, cyanogenic glycosides, flavonoids, and chlorogenic acid (ISI database, 2003; Olszewska and Kwapisz, 2011). This plant has been found to possess anti-oxidant (Olszewska and Kwapisz, 2011), and anti-bacterial (Kumarasamy et al., 2004) properties. However, pharmacological activities of P. padus are extremely limited. Therefore, this study was undertaken to validate the antiinflammatory and anti-nociceptive effects of P. padus. 2. Materials and methods 2.1. Plant material The plant materials were purchased from Hainyakupsa (Jeonbuk, Korea) in May 2011. The plant was identified by Dr. Dae Keun Kim, College of Pharmacy, Woosuk University, Republic of Korea. A voucher specimen (WH078) has been deposited at the Department of Oriental Pharmacy, College of Pharmacy, Woosuk University. 2.2. Extraction and solvent fractionation of plant material We extracted the dried stem of the plant (3000 g) using 12,000 ml of MeOH with 2 h sonication. The resultant methanolic extract was concentrated into 113 g (yield: 5.1%) using a rotary evaporator. Then, the extract was subjected to successive solvent partitioning to give n-hexane (8.9 g), CH2Cl2 (7.2 g), EtOAc (8.76 g) and n-BuOH (22.7 g) soluble fractions. Each fraction were lyophilized and then stored at 20 1C for further use. Because the preliminary experiments for anti-inflammatory and antinociceptive activity of the fractions showed that among the four fractions, the CH2Cl2 fraction (MPP) have the most potent pharmacological potential. Therefore, further studies were conducted using MPP. 2.3. Animals ICR mice (6 weeks old) weighing 20–25 g and C57BL/6 mice (5 weeks old) weighing 18–22 g were supplied by Damul science (Daejeon, Korea). All animals were housed at 2271 1C with a 12 h light/dark cycle and fed a standard pellet diet with tap water ad libitum. For the purpose of isolating peritoneal macrophages, the C57BL/6 mice were given intraperitoneal (i.p.) injections 3 days earlier with 2.5 ml of thioglycollate (TG) solution. The experimental protocols complied with the recommendations of the International Association for the Study of Pain (Zimmermann, 1983). 2.4. Anti-inflammatory study 2.4.1. Isolation and culture of mouse macrophages TG-elicited macrophages were harvested 3 days after i.p. injection of TG and isolated. Using 8 ml of PBS containing 10 U/ml heparin, peritoneal lavage was performed. Then, the cells were distributed in FBS-free DMEM and maintained at 37 1C in a humidified atmosphere of 5% CO2. After 3 h, the cells were washed three times with PBS to remove non-adherent cells and equilibrated with DMEM that contained 10% heat-inactivated FBS before treatment. 2.4.2. Determination of cell viability Cell respiration, an indicator of cell viability, was measured by the mitochondrial dependent reduction of 3-(3,4-dimethylthiazol2-yl)-2,5-diphenyl tetrazolium bromide (MTT) to formazan, as described previously (Mosmann, 1983). The extent of the reduction of MTT to formazan within cells was quantified by measuring the optical density (OD) at 570 nm using an automated microplate reader (GENios, Tecan, Austria). 2.4.3. Measurement of nitrite concentration The peritoneal macrophages (3 105 cells/well) were cultured with various concentrations of MPP. The cells were then stimulated with rIFN-g (20 U/ml) and LPS (10 mg/ml) and further incubated for 48 h. NO synthesis in cell cultures was measured with a microplate assay method. To measure nitrite, 100 ml aliquots were removed from conditioned medium and incubated with an equal volume of Griess reagent at room temperature for 10 min. The absorbance at 540 nm was determined by a microplate reader. The quantity of NO2 was calculated by using sodium nitrite as a standard. Nitro-L-arginine methyl ester (L-NAME) was used as a reference drug. 2.4.4. Measurement of iNOS enzyme activity iNOS enzyme activity was determined according to Israf et al. (2007) with minor modification (Israf et al., 2007). The cells were induced to produce iNOS enzyme with rIFN-g (20 U/ml) and LPS (10 mg/ml) stimulation. After 12 h incubation, the medium was discarded and the cells were treated with various concentrations of MPP, and incubated for another 12 h. Nitrite levels were determined using the Griess reagent as described in Section 2.4.3. 2.4.5. Preparation of nuclear extracts Nuclear extracts were prepared essentially as described previously (Baek et al., 2002). Briefly, the cells were allowed to swell by adding lysis buffer (10 mM HEPES pH 7.9, 10 mM KCl, 0.1 mM EDTA, 1 mM dithiothreitol and 0.5 mM phenylmethylsulfonyl fluoride). Pellets containing crude nuclei were resuspended in extraction buffer (20 mM HEPES pH 7.9, 400 mM NaCl, 1 mM EDTA, 1 mM dithiothreitol and 1 mM phenylmethylsulfonyl fluoride) and incubated for 30 min on ice. The samples were centrifuged at 12,000 rpm for 10 min to obtain the supernatant containing nuclear extracts. 2.4.6. Western blot analysis Whole cell lysates were made by boiling peritoneal macrophages in sample buffer (62.5 mM Tris–HCl pH 6.8, 2% sodium dodecyl sulfate (SDS), 20% glycerol and 10% 2-mercaptoethanol). Proteins in the cell lysates were then separated by 10% SDSpolyacrylamide gel electrophoresis and transferred to nitrocellulose paper. The membrane was then blocked with 5% skim milk for 2 h at room temperature and then incubated with anti-iNOS, anti-NF-kB (Santa Cruz Biotechnology, CA, USA) and anti-COX-2 (Pierce Biotechnology, IL, USA). After washing the membrane in phosphate buffered saline (PBS) containing 0.05% tween 20 three times, the blot was incubated with HRP-conjugated anti-rabbit and anti-mouse (Amersham Biosciences, Little Chalfont, UK) and the target proteins were visualized by an enhanced chemiluminesence detection system (Millipore Corporation. MI, USA). 2.4.7. Trypsin-induced paw edema Edema was induced in the right-hind paw by a 30 ml intraplantar (i.pl.) injection of saline containing trypsin (30 mg/paw) after oral administration of MPP (250, 500 mg/kg) or indomethacin (10 mg/kg). The left paw received the same volume of saline and it was used as the control. Edema was measured by a plethysmometer (LE7500, Panlab, Spain), at different periods of time (0, 15, 30, 60, 120, 240) after injection of trypsin. Edema was recorded as the difference between the volume of right and left paws. Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] 2.5. Anti-nociceptive study 2.5.1. Grouping and drug administration Animals were randomly assigned into several groups, each consisting of eight or ten mice for analgesic tests. Mice were fasted for 12 h prior to experiments. Negative controls were treated with the same volume of distilled water which was used for reconstituting the drug. Positive controls were treated with standard drugs: tramadol (i.p.) or indomethacin (p.o.). Treatment groups in each test were treated orally with different doses of MPP. 2.5.2. Acute toxicity test To evaluate possible toxicity, the acute toxicity test was carried out. Mice (n ¼6) were tested by administering different doses of MPP and the doses were increased or decreased according to the response of the animal (Bruce, 1985). The control group received only the equal volume of distilled water. All the groups were observed for any gross effect or mortality for a 24 h period. 2.5.3. Tail immersion test The tail immersion test was performed according to the procedures used by Wang et al. (2000) with minor modification. Briefly, the lower two-third of mouse’s tail was immersed on a water bath set at temperature of 50 70.2 1C. The reaction time, i.e. the amount of time it takes the animal to withdraw its tail, was measured 0, 30, 60, 90 and 120 min after the administration of MPP (250, 500 mg/kg; p.o.), tramadol (15 mg/kg; i.p.) and vehicle (D.W). To avoid tissue injury, the cut-off time was 20 s. 2.5.4. Hot plate test The hot plate test was carried out using a hot plate apparatus (model JD-A-10A, Jungdo BNP, Korea), maintained at 5571 1C. Only mice that showed initial nociceptive responses (licking of the forepaws or jumping) between 7 and 15 s were used for additional experiments. The chosen mice were pre-treated with MPP (250, 500 mg/kg; p.o.) or vehicle (D.W), and 30 min later the measurements were taken. A tramadol (15 mg/kg; i.p.) treated animal group was included as a positive control. The cut-off time was set at 30 s to minimize skin damages. The reaction time was calculated as described for the tail immersion test. 2.5.5. Acetic acid-induced writhing test Acetic acid-induced writhing test was performed as previously described (Olajide et al., 2000). The response to an intraperitoneal injection of acetic acid solution (1% in 0.9% saline), which consisted of abdominal constrictions and hind limb stretching, was measured for each mouse starting 5 min after the acetic acid injection and was measured for an additional 20 min. Each experimental group was treated orally with vehicle (D.W), MPP (250, 500 mg/kg) or indomethacin (10 mg/kg) 1 h prior to the acetic acid injection. 2.5.6. Formalin test In the formalin test (Santos and Calixto, 1997), group of mice were treated orally with MPP (250 and 500 mg/kg; p.o.) or vehicle (D.W). After 1 h, each mouse was treated with 20 ml of 5% formalin (in 0.9% saline, subplantar) into the right hind paw. The duration of paw licking (s) was used as an index to measure the pain response during the 0–5 min period (first phase, neurogenic) and the 20–35 min period (second phase, inflammatory) after formalin injection. Tramadol and indomethacin were used as positive control drugs and were administrated 30 min before the test at a dose of 10 mg/kg, i.p. and p.o. respectively. To examine 3 the possible connection of endogenous opioids to the antinociceptive activity, the tramadol, indomethacin and MPP groups were treated with naloxone (5 mg/kg; i.p.) 15 min prior to drug administration. 2.6. Statistical analysis The results are expressed as the mean 7S.D. or mean 7S.E.M. depending on the experiments. One-way ANOVA was used to determine statistical significance. P-values less than 0.01 were considered significant. The intensity of the bands obtained from western blotting studies was estimated with ImageQuantTL (GE Healthcare, Sweden) and the values were expressed as mean7 standard error. 3. Results 3.1. Effects of MPP on nitrite production Various concentration (125, 250 and 500 mg/ml) of MPP were used on murine peritoneal macrophages to test whether MPP can suppress rIFN-g/LPS-induced NO production. As seen in Fig. 1A, unstimulated cells secreted nitrite approximately 3.61 70.09 mM, while rIFN-g/LPS-stimulated cells produced about 30 folds of nitrite (93.770.97 mM). This increased nitrite levels were markedly inhibited in a dose dependent manner by pre-treatment of MPP. Interestingly, MPP showed similar inhibitory activity at maximum concentration (80.6% inhibition, p o0.001) compared to L-NAME (78.2% inhibition, po0.001), a synthetic NOS inhibitor. When the cells were incubated with MPP alone, the nitrite levels was not significantly different to vehicle (data not shown). To exclude the possibility that the inhibitory effect of MPP on NO production was due to cytotoxcity, we carried out MTT colorimetric assay. When the cells were treated with MPP, there was no change in cell viability (data not shown). 3.2. Effects of MPP on iNOS enzyme activity To assess whether MPP directly inhibit the catalytic activity of iNOS, we treated MPP after stimulation and checked the nitrite levels. Since we removed supernatant and added fresh media 12 h after stimulation, rIFN-g/LPS-stimulated macrophages generated less amount of nitrite compared to continuous stimulated cells for 48 h. Fig. 1B showed that 500 mg/ml of MPP slightly suppress NO accumulation (23.8% inhibition, p o0.01) by rIFN-g/LPSinduced iNOS enzyme activity, while another concentrations did not affect the increased nitrite level. Only L-NAME, a reference drug, exhibited relative strong inhibitory effect (59.4% inhibition, po0.001) upon iNOS catalytic activity. 3.3. Effects of MPP on iNOS and COX-2 expression Next, we investigated the effect of MPP on the iNOS and COX-2 at a translational level using western blotting. Fig. 2 showed that iNOS protein expression was strongly increased after rIFN-g and LPS stimulation. Compared to the control, iNOS expression was potently blocked in the presence of MPP. We also tested the expression of COX-2, another pro-inflammatory mediator. The enhanced expression of COX-2 protein from rIFN-g/LPS stimulation was attenuated by MPP dose-dependently. The downregulated protein levels were most noticeable at the maximum concentration in both iNOS and COX-2, demonstrating that MPP could play an important role in the blocking iNOS and COX-2 expression. Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 4 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] Fig. 1. Effects of MPP on NO production and iNOS enzyme activity in rIFN-g/LPS-activated mouse peritoneal macrophages. (A) Peritoneal macrophages (3 105 cells/well) were cultured with various concentration of MPP or 0.05% DMSO, a vehicle. After 30 min, macrophages were stimulated with rIFN-g (20 U/ml) for 6 h and then stimulated with LPS (10 mg/ml). After 48 h of culture, NO release was measured by the Griess method (nitrite). (B) Peritoneal macrophages (3 105 cells/well) were stimulated with rIFN-g (20 U/ml) for 6 h and then stimulated with LPS (10 mg/ml). After 12 h incubation, the medium was changed with fresh medium and the cells were incubated for another 12 h with various concentrations of MPP. Then NO release was measured by the Griess method described previously. The amount of NO (nitrite) released into the medium is presented as the mean 7S.D. of three independent experiments with duplicates in each run. The nitrite volume was determined by using a sodium nitrite (NaNO2) standard curve; *p o0.01 and **p o 0.001 compared to the rIFN-g/LPS-treated control group. 3.4. Effects of MPP on NF-kB activation It is well known that NF-kB is involved in the expression of various inflammatory mediators (Ghosh et al., 1998; Henkel et al., 1993). Thus, we also investigated the effect of MPP on the activation of NF-kB. To evaluate the inhibitory effect of MPP on activation of NF-kB, western blotting was performed using cytosolic and nuclear extracts. As shown in Fig. 3, MPP treatment attenuated translocation of NF-kB protein from cytosol to nucleus after rIFN-g/LPS stimulation, suggesting MPP inhibited the transcriptional activity of NF-kB. reduction of the edema formation induced by trypsin in the mouse paw. 3.6. Acute toxicity To test possible toxicity of MPP in animals, acute toxicity test was conducted. Various concentrations of MPP (up to 2000 mg/kg; p.o.) were administered to the mice. In this study, they did not present any abnormal behavior or death during the assessment period (24 h) (data not shown). These results suggest that MPP was safe to use in mice at the treatment concentration (250 and 500 mg/kg; p.o.). 3.5. Effects of MPP on trypsin-induced paw edema 3.7. Anti-nociceptive activity of MPP in the tail immersion test The trypsin-induced paw edema model was performed to evaluate the in vivo anti-inflammatory activity of MPP. Subplantar injection of trypsin induced a marked and time-dependent edema of paw tissues and this response peaked from 30 to 60 min and then decreased gradually. Oral treatment of MPP effectively reduced edema volume in a dose dependent manner (Fig. 4). Indomethacin, a common clinical NSAID, also produced a marked In the tail immersion test, MPP showed significant antinociceptive effect in a dose-dependent manner. Table 1 demonstrated that MPP delayed reaction times to a nociceptive stimulus 60 min after oral administration (38.61% at 250 mg/kg and 68.51% at 500 mg/kg, p o0.001). Tramadol, the reference drug, also exhibited strong analgesic activity (70.47%, po0.001) which was recorded 30 min after drug treatment. Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] 5 Nuclear p65 level (%) 120 100 80 60 40 20 0 IFN-¥ã/LPS - + + + + MPP (¥ìg/mL) - - 125 250 500 0 IFN-¥ã/LPS - + + + + MPP (¥ìg/mL) - - 250 500 Cytosolic p65 level (%) 300 Fig. 2. Effect of MPP on the expression of iNOS and COX-2 in the rIFN-g/LPSactivated peritoneal macrophages. Peritoneal macrophages (5 106 cells/well) were pretreated with MPP or 0.05% DMSO, 30 min prior to rIFN-g (20 U/ml) stimulation. After 6 h, macrophages were then stimulated with LPS (10 mg/ml) for 24 h. The protein extracts were prepared and samples were analyzed for iNOS and COX-2 expression by Western blotting as described in Section 2. The expression of iNOS and COX-2 was quantified by densitometric analysis. The expression levels of the rIFN-g/ LPS treated control cells were considered to be 100% for the percentage calculations. 3.8. Anti-nociceptive activity of MPP in the hot plate test MPP also generated potent increases in analgesia in the hot plate test. The anti-nociceptive effects of MPP (250, 500 mg/kg) occurred between 30 and 90 min and maximum analgesia was reached at 60 min (37.98%, po0.01 and 62.18%, po0.001 respectively) (Table 2). Tramadol also caused significant anti-nociception (62.05%, po0.001) 30 min after drug treatment. 3.9. Anti-nociceptive activity of MPP in the acetic acid-induced writhing test Intraperitoneal injection of 1% acetic acid into mice caused 47.86 72.03 writhings in a 20 min interval. As shown in Table 3, 250 200 150 100 50 125 Fig. 3. Effects of MPP on NF-kB translocation by rIFN-g/LPS-stimulated peritoneal macrophages. Peritoneal macrophages (5 106 cells/well) were pretreated with MPP or 0.05% DMSO for 30 min and then stimulated with rIFN-g (20 U/ml) for 2 h. After 1 h stimulation with LPS (10 mg/ml), the nuclear extracts were prepared and samples were analyzed by Western blotting as described in Section 2 and quantified by densitometry. the treatment with MPP induced a significant decrease in the number of writhing motions dose dependently (52.5% at 250 mg/kg, po0.001 and 72.8% at 500 mg/kg, po0.001). The reference drug, indomethacin, also caused strong anti-nociception (74.3%, po0.001) which is similar with the inhibition observed for the high concentration of MPP. 3.10. Anti-nociceptive activity of MPP in the formalin test In the formalin test, the vehicle group produced nociceptive response of licking total duration (s) of 124.8076.90 in the first phase (0–5 min) and 140.3678.81 in the second phase (20–35 min). Table 4 revealed that MPP has a potent analgesic activity both first phase (32.37%, 38.40%) and second phase (30.58%, 56.64%) for the 250 and 500 mg/kg doses, respectively. Tramadol significantly blocked the pain responses in both phases (first phase, 54.85% and second phase, 62.68%). However indomethacin suppressed second phase (54.92%) nociception only. In combination studies using naloxone, an opioid receptor antagonist, the analgesic Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 6 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] activity of tramadol was reduced about 18.01% and 11.34% in first phase and second phase pain responses, respectively. However, naloxone did not alter the second phase anti-nociception of indomethacin. Interestingly, MPP’s analgesic activity was slightly antagonized by naloxone ( 11.39%). 4. Discussion In this study, we investigated the anti-inflammatory and antinociceptive properties of MPP. First, we checked the effect of MPP on NO levels using rIFN-g/LPS-stimulated murine peritoneal macrophage model. Nitrite determination using Griess method revealed that MPP has potent inhibitory activity on the NO Vehicle Indomethacin MPP 250 MPP 500 Change of paw volume (ml) 0.16 0.14 0.12 0.10 0.08 0.06 production. Next, we asked whether this inhibition is due to alteration of iNOS catalytic activity. To do so, we stimulated the macrophages and let them synthesize iNOS with overnight incubation. Then, we treated MPP after changing the medium to remove both generated NO and stimulation agents. After 12 h incubation, MPP attenuated iNOS-mediated NO production about 23.8% at maximum concentration, which has relatively low effect compared to the MPP pre-treatment data (80.6%). Previous studies on this plant showed that P. padus possess anti-oxidant capacity with several phenolic compounds including quercetin and chlorogenic acid (Olszewska and Kwapisz, 2011). Indeed, we tested NO radical scavenging activity of MPP using sodium nitroprusside (SNP), an inorganic NO generator. The results showed that MPP has similar anti-radical capacity at 500 mg/ml concentration (17.3%, data not shown) compared to its effect on the iNOS-mediated NO production. Thus, it is quite reasonable to assume that MPP may inhibit NO production through either interfering iNOS catalytic activity or scavenging NO radical directly. Since MPP did not block the iNOS enzyme activity strongly, we further checked iNOS protein expression at the translational level and MPP suppressed the expression of iNOS significantly. Based on these results, we can conclude that the inhibitory effect of MPP on NO production depends mainly on the attenuation of iNOS expression. We also examined the expression level of COX-2, 0.04 0.02 Table 3 Effect of MPP on nociceptive responses in the acetic acid-induced writhing test. 0.00 0 20 40 60 80 100 120 140 160 180 200 220 240 Time (min) Fig. 4. Effect of MPP on the increase in hind paw volume induced by intraplantar (i.pl.) injection of trypsin (30 mg/paw) in mice. Edema was induced in the righthind paw by trypsin after oral administration of MPP. The left paw received 30 ml of saline as a control. Edema was measured at different periods of time (0, 15, 30, 60, 120, 240) after injection of trypsin using plethysmometer. Data shows the mean 7 S.E.M. (n¼ 14). Treatment Dose (mg/kg) Number of writhings (5–25 min) Inhibition (%) Vehicle Indomethacin MPP MPP – 10 250 500 47.86 7 2.03 12.25 7 1.96 22.70 7 2.27 13.007 1.91 – 74.39nn 52.56nn 72.83nn Values expressed as mean 7 S.E.M (n ¼10). nn po 0.001 to vehicle-treated group. Table 1 Effect of MPP on nociceptive responses in the tail immersion test. Treatment Vehicle Tramadol MPP MPP Dose (mg/kg) Latency time (s) – 15 250 500 0 30 60 90 120 3.807 0.12 3.74 7 0.12 3.65 7 0.13 4.037 0.13 3.96 70.14 6.74 70.26nn 4.71 70.14 5.21 70.23n 4.047 0.11 5.667 0.29nn 5.607 0.15nn 6.807 0.34nn 4.007 0.08 4.427 0.16 4.097 0.12 4.877 0.24 3.91 7 0.11 4.06 7 0.16 3.65 7 0.12 3.88 7 0.24 Values expressed as mean 7 S.E.M. and units are in seconds (n¼ 10). n po 0.01 compared to vehicle-treated group. p o 0.001 compared to vehicle-treated group. nn Table 2 Effect of MPP on nociceptive responses in the hot plate test. Treatment Vehicle Tramadol MPP MPP Dose (mg/kg) – 15 250 500 Latency time (s) 0 30 60 90 120 10.407 0.16 10.12 7 0.28 10.007 0.28 11.21 7 0.47 10.47 7 0.15 16.96 7 0.90nn 12.18 7 0.34 13.04 7 0.41 10.25 70.16 14.37 70.63n 14.14 70.26n 16.62 70.51nn 10.06 7 0.23 12.57 7 0.45 12.94 7 0.40 13.94 7 0.57n 10.44 7 0.22 11.38 7 0.38 10.16 7 0.27 11.53 7 0.43 Values expressed as mean 7 S.E.M. and units are in seconds (n¼ 10). n po 0.01 compared to vehicle-treated group. p o 0.001 compared to vehicle-treated group. nn Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] 7 Table 4 Effect of MPP on nociceptive response in the formalin test. Treatment Vehicle Tramadol Naloxoneþ Tramadol Indomethacin Naloxoneþ Indomethacin MPP MPP Naloxoneþ MPP Dose (mg/kg) – 15 5 þ15 10 5 þ10 250 500 5 þ500 Early phase (0–5 min) Late phase (25–40 min) Licking time (s) Inhibition (%) Licking time (s) Inhibition (%) 124.80 7 6.90 56.34 7 7.88 102.32 7 7.02 117.957 6.79 112.60 7 7.49 84.407 7.04 76.88 7 6.43 91.097 4.60 – 54.85nn 18.01## 5.48 9.77 32.37n 38.40nn 27.01n 140.26 7 8.81 52.35 7 7.30 124.367 6.15 63.23 7 13.49 69.24 7 5.06 97.37 7 10.80 60.827 7.90 93.57 7 4.40 – 62.68nn 11.34## 54.92nn 50.64nn 30.58n 56.64nn 33.29n,# Values expressed as mean 7 S.E.M. (n¼ 12). Naloxone (5 mg/kg) was pre-treated 15 min prior to the drug administration. p o0.01 compared to vehicle-treated group. po 0.001 compared to vehicle-treated group. p o 0.01 compared to naloxone-untreated group. ## p o0.001 compared to naloxone-untreated group. n nn # another key enzyme in inflammation. MPP pre-treatment in combination with IFN-g and LPS stimulation led to a reduction in COX-2 expression. Thus, it seems quite plausible that MPP may inhibit COX-2-mediated PGE2 production. However, further studies are required to determine whether MPP is a selective inhibitor of COX-2. The induction of pro-inflammatory mediators is largely regulated by transcriptional factors such as NF-kB which is essential for the transcription of pro-inflammatory molecules (Muller et al., 1993). Therefore, we examined whether MPP altered the translocation of NF-kB into the nucleus in activated macrophages. Here we demonstrate that MPP decreased the NF-kB level in the nucleus and increased in the cytosol, indicating MPP suppressed iNOS and COX-2 expression by inhibiting the NF-kB dependent signaling pathway and the subsequent production of proinflammatory mediators. Then, we further tested MPP’s anti-inflammatory effects using trypsin-induced paw edema model in mice. Since injection of trypsin, a proteinase-activated receptor2 (PAR2) agonist, into the paw of animal induces features of inflammatory reactions including infiltration of granulocyte and increase in vascular permeability (Kawabata et al., 1998; Vergnolle et al., 1999), this model is a suitable method for evaluating the anti-inflammatory agents. Consistent with in vitro studies, MPP reduced the trypsin-induced change of paw volume in a dose dependent manner. It has been reported that PAR2 is activated through proteolytic unmasking of the N-terminal tethered ligand by trypsin results in enhanced COX-2 dependent PGE2 production (Kawao et al., 2005; Nagataki et al., 2008). Therefore, MPP’s anti-edematogenic effects might be connected with attenuation of COX-2 expression, at least in part. Previous phytochemical investigations on P. padus revealed that it has anthocyanins and flavonoids such as isorhamnetin, astragalin, and quercetin (ISI database, 2003; Olszewska and Kwapisz, 2011). Interestingly, all of them have been known to possess inhibitory effects on the pro-inflammatory mediators like iNOS and COX-2 (Hamalainen et al., 2011; Hwang et al., 2011; Kim and Kim, 2011; Zhang et al., 2011). Moreover, previous study suggests that chlorogenic acid also reduces inflammatory edema (Chagas-Paula et al., 2011). Therefore, we speculate that these compounds might play an important role in the anti-inflammatory activity of MPP. Next, we decided to analyze anti-nociceptive activities of MPP using various experimental pain models in mice. To determine central anti-nociceptive activity of MPP, we used thermal nociception models such as tail immersion test and hot plate test. In both tests, MPP showed significant analgesic effects compared to tramadol, a reference drug, suggesting involvement of spinal and supraspinal analgesic pathways. In both tests, MPP reached the maximum analgesic level 60 min after administration, while tramadol exhibited a rapid effect with a maximum peak in a short amount of time, which is similar to the action of opioid agonists (e.g. morphine). This difference in the maximum analgesic point could be explained by the methods of drug administration (i.p or p.o.) or the metabolic rate of each drug. To investigate peripheral anti-nociceptive effect of MPP, we adopted the acetic acid-induced writhing model which is associated with increased levels of prostaglandins (PGs), particularly PGE2, in peritoneal fluids (Deraedt et al., 1980). Here in this study, MPP showed potent inhibition of acetic acid-induced abdominal constrictions. Since PGs induce inflammatory pain by activating and sensitizing the peripheral chemosensitive nociceptors (Dirig et al., 1998), one possible analgesic mechanism of MPP may be the inhibition of the COX-2 enzyme. Indeed, indomethacin, a nonsteroidal anti-inflammatory drug, produced a significant decrease in the writhing response through inhibition of PG synthesis, resulting in peripheral analgesic consequent. Last, we conducted formalin test to evaluate the analgesic mechanism of MPP. The present study has shown that tramadol blocks both the early and late phases of formalin-induced nociception, while indomethacin primarily suppressed the later phase. In keeping with these results, many reports suggest that drugs acting primarily on the central nervous system inhibit equally in both phases, while peripherally acting drugs, such as steroids and NSAIDs, cause slight inhibition in the early phase of the formalin test (Hunskaar et al., 1985; Trongsakul et al., 2003; Vongtau et al., 2004). In agreement with the results from above tests, MPP was effective in preventing both the first and second phases, suggesting suppressive properties on both neurogenic and inflammatory nociception. These data provide further confirmation for the central and peripheral anti-nociceptive activity of MPP. Indeed, previous studies on the several active compounds of P. padus such as anthocyanin, quercetin and chlorogenic acid demonstrated that they have analgesic effect on the inflammatory pain (Tall et al., 2004; dos Santos et al., 2006; Valerio et al., 2009). To check the possible connection between MPP’s antinociception and opioid receptor, we carried out combination test using naloxone, a non-selective opioid receptor antagonist. Interestingly, naloxone was able to antagonize the analgesic action of MPP partly, but not completely. These results indicate that MPP provide anti-nociception through not only acting as an opioid agonist, but other mechanisms including anti-inflammatory properties. Here in the current study, we demonstrated that MPP has significant inhibitory effects on pro-inflammatory mediators Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023 8 J.H. Choi et al. / Journal of Ethnopharmacology ] (]]]]) ]]]–]]] including NO, iNOS and COX-2 via the down regulation of NF-kB translocation to the nucleus. In addition, MPP also exhibited potent anti-nociceptive activities on both central and peripheral mechanism by acting as a partial opioid receptor agonist. Based on these properties, MPP may be useful in many diseases as an effective immunomodulatory and analgesic agent. Acknowledgments This work was supported by the research grant from Woosuk University. References Baek, W.K., Park, J.W., Lim, J.H., Suh, S.I., Suh, M.H., Gabrielson, E., Kwon, T.K., 2002. 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Please cite this article as: Choi, J.H., et al., Anti-inflammatory and anti-nociceptive properties of Prunus padus. Journal of Ethnopharmacology (2012), http://dx.doi.org/10.1016/j.jep.2012.09.023