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Transfer of caesium and potassium from Japanese apricot ( Prunus mume Sieb.et Zucc. ) to Japanese apricot liqueur ( Ume liqueur)

2016; Wiley; Volume: 122; Issue: 3 Linguagem: Catalão

10.1002/jib.346

2050-0416

Masaki Okuda, Takeshi Akao, Masanori Sumihiro, Megumi Mizuno, Nami Goto‐Yamamoto,

Cassava research and cyanide

Journal of the Institute of BrewingVolume 122, Issue 3 p. 473-479 Research articleFree Access Transfer of caesium and potassium from Japanese apricot (Prunus mume Sieb.et Zucc.) to Japanese apricot liqueur (Ume liqueur) Masaki Okuda, Corresponding Author Masaki Okuda National Research Institute of Brewing, Higashihiroshima, JapanCorrespondence to: Masaki Okuda, National Research Institute of Brewing, 3-7-1 Kagamiyama, Higashihiroshima 739-0046, Japan. E-mail: [email protected]Search for more papers by this authorTakeshi Akao, Takeshi Akao National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorMasanori Sumihiro, Masanori Sumihiro National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorMegumi Mizuno, Megumi Mizuno National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorNami Goto-Yamamoto, Nami Goto-Yamamoto National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this author Masaki Okuda, Corresponding Author Masaki Okuda National Research Institute of Brewing, Higashihiroshima, JapanCorrespondence to: Masaki Okuda, National Research Institute of Brewing, 3-7-1 Kagamiyama, Higashihiroshima 739-0046, Japan. E-mail: [email protected]Search for more papers by this authorTakeshi Akao, Takeshi Akao National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorMasanori Sumihiro, Masanori Sumihiro National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorMegumi Mizuno, Megumi Mizuno National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this authorNami Goto-Yamamoto, Nami Goto-Yamamoto National Research Institute of Brewing, Higashihiroshima, JapanSearch for more papers by this author First published: 25 July 2016 https://doi.org/10.1002/jib.346Citations: 3AboutSectionsPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Abstract The potential contamination with radionuclides released by the Fukushima Daiichi Nuclear Power Plant Accident following the great east Japan earthquake and tsunami in March 2011 of agricultural products and processed foods derived from them is a matter of on-going concern. The stable 133Cs is a useful indicator for predicting the behaviour of radioactive Cs, and potassium (K) is a congener of Cs. In this study, the distribution of 133Cs and K in Ume fruit, and the transfer of 133Cs and K from Ume fruit to Ume liqueur, were investigated. The concentrations of 133Cs and K in Ume fruit were highest in the skin, followed by the kernel or flesh, and then the pit. About 80% of 133Cs and K in all Ume fruits was distributed in the flesh. The transfer ratios of 133Cs and K from Ume fruit to Ume liqueur were similar among all cultivars after 3 months, and they were similar to those of organic acids. The food retention factor (Fr = weight of 133Cs in Ume liqueur/weight of 133Cs in Ume fruit) was ca. 0.8, and the processing factor (Pf = concentration of 133Cs in Ume liqueur/concentration of 133Cs in Ume fruit) was 0.2–0.3. From the present study, the radioactivity of Ume liqueur would be below the legal limit if made using Ume fruits within the legal limit, thereby confirming the safety of Ume liqueur. Copyright © 2016 The Institute of Brewing & Distilling Introduction The accident at the Fukushima Daiichi Nuclear Power Plant following the Great East Japan earthquake and tsunami in March 2011 led to a large release of radionuclides. Since then, the radionuclide contamination of food has been of great concern. Among the radionuclides released by this accident, radiocaesium (Cs) is the most important in terms of assessing public radiation exposure because of its relatively long half-life (134Cs, 2 years; 137Cs, 30.2 years) and wide distribution in the environment. Cs is an alkali metal and a congener of potassium (K); thus, Cs is relatively similar to K in terms of physical and chemical properties 1. Although radioactive contaminants were low or were not detected in most agricultural food harvested in eastern Japan, a few food items had radioactive Cs levels in excess of 100 Bq/kg, which has been set as the legal limits for general food stuffs in Japan 2. The transfer of radionuclides during food production is typically assessed by two parameters: the food retention factor (Fr) and the processing factor (Pf) 3. The Fr is the fraction of radioactivity that is retained in the food after food production. The Pf is the ratio of the radionuclide activity concentration in the food product to that in the original raw material. Since the accident, many studies on the transfer of Cs from field to agricultural food and the behaviour of radioactive Cs during food processing have been reported 4-12. In regard to alcoholic beverages, studies on the behaviour of Cs in beer 13 and wine 14 production were reported before the accident; however, the behaviour of Cs in Japanese traditional alcoholic beverages has not been studied. In general, isotopes behave similarly in terms of their physical properties and chemical reactivity 3. Therefore, we have previously examined both the behaviour of radioactive Cs and that of stable 133Cs during sake and wine making 15-17. The behaviour of stable 133Cs was the same as that of radioactive Cs in the production of sake and wine, and the results showed that stable Cs is a useful indicator for predicting the behaviour of radioactive Cs, as the International Atomic Energy Agency reported 3. In the production of sake 15, 16, ~90% of the total mass of Cs was removed by the steps of milling, washing and steeping in water during sake brewing. For wine making, although the radioactivity of wine relative to grapes was not decreased as much as in sake, the radioactivity of wine did not exceed the legal limit when made using grapes within the legal limit, and the safety of wine was confirmed 17. These data have provided useful information for alcoholic drink makers and consumers. Ume fruit, the Japanese apricot (Prunus mume Sieb.et Zucc.), is mostly processed into Ume-boshi (pickled Ume) and Ume liqueur. Ume liqueur has traditionally been a popular Japanese beverage and is made by steeping Ume fruit and crystal sugar in neutral spirits 18. Ume liqueur is made both commercially and at home. In addition to the Ume liqueur that is drunk, the Ume fruit steeped during Ume liqueur making is also eaten. Ume liqueur has distinct flavour characteristics of sweetness from the sugar and sourness from organic acids. The organic acids are extracted from the Ume fruit to the Ume liqueur and the crystal sugar is dissolved in neutral spirits gradually during steeping. For Ume fruit harvested in the 2011 season, the radioactive Cs contamination seemed to be mainly due both to the direct deposition of Cs from the Fukushima fallout on the young fruit and translocation from the above-ground plant parts, which were affected by direct Cs deposition on the existing above-ground plant parts and this may have been absorbed by the tree 19. After the 2012 season, the radioactive Cs contamination seemed to be due to translocation from the above-ground part from absorption of the radioactive Cs that remained in the fruit trees 19. Accordingly, for Ume liqueur making, a survey of transfer of Cs from Ume fruit to Ume liqueur is needed. Sekizawa et al. reported the Fr and Pf of Cs for Ume liqueur at 3 months after steeping using Ume fruits contaminated with radioactive Cs 20. However, the distribution of Cs in Ume fruit is not known, although the Ume fruit steeped during Ume liqueur making is eaten. In addition, Ume liqueur is usually made with about 6 months of steeping 18, and there is a need to examine the change in Cs concentration in detail during steeping. Therefore, the distribution of Cs in the Ume fruit and the detailed behaviours of Cs and maturation indices during Ume liqueur production require further study. In the present study, the behaviours of stable 133Cs and K were investigated during the production of Ume liqueur using seven kinds of Ume fruit without contamination of radioactive Cs. First, the distribution of 133Cs and K in Ume fruit was examined. Next, the transfer of 133Cs and K from Ume fruit to Ume liqueur as well as organic acid concentration, specific gravity and colouration during steeping were examined. Finally, both the Fr and Pf of Cs were determined. Materials and methods Materials Seven kinds of Ume fruits were used (shown in Table 1). Neutral spirits (Alc.35%) were from a commercial source (Takara Holdings, Kyoto, Japan). Crystal sugar was from a commercial source (Nissin Sugar Manufacturing, Tokyo, Japan). Table 1. Ume fruit used for Ume liqueur making Cultivar Area Number of fruit used for Ume liquer Weight/Ume fruit Weight proportion in each tissue of Ume fruit (%) Citric acid Malic acid (g) skin flesh pit kernel (mg/g fresh weight) (mg/g fresh weight) Shirokaga Kansai 43 23.2 ± 2.6 9.8 79.7 8.1 2.4 27.1 ± 2.6 9.7 ± 0.4 Shirokaga Kanto 48 20.9 ± 2.0 7.8 81.1 9.0 2.1 23.3 ± 3.3 11.8 ± 0.7 Shirokaga Tohoku A 45 22.2 ± 2.1 12.0 77.6 7.9 2.5 25.0 ± 2.5 11.1 ± 0.4 Shirokaga Tohoku B 33 30.3 ± 2.8 8.2 83.8 6.1 1.9 35.2 ± 3.1 9.6 ± 0.5 Gojiro Kansai 39 25.7 ± 2.3 10.4 79.4 8.0 2.1 34.4 ± 1.8 10.4 ± 2.9 Bungo Tohoku 67 14.9 ± 1.9 12.3 65.4 17.8 4.5 13.3 ± 2.0 10.8 ± 0.6 Nanko Kansai 30 33.3 ± 2.9 6.8 83.0 8.3 1.9 41.9 ± 4.6 4.8 ± 0.8 Reagents Nitric acid (HNO3) (Kantokagaku, Tokyo, Japan) and hydrogen peroxide (H2O2; Kantokagaku, Tokyo, Japan) were ultra-pure analytical grade. The Cs, K and Yttrium standard solutions were purchased from Kantokagaku, Tokyo, Japan. Ultra-pure water (>18.1 MΩ), obtained via a MilliQ system (Millipore, USA), was used throughout the work. Ume liqueur production Individual Ume fruit was weighed, and Ume fruits with a weight range of 90% confidence were selected for making the Ume liqueur. The selected Ume fruits were washed with water and dried at 15 °C for 20 h by air-drying or by sun-drying for 3–5 h. The Ume fruit (1.0 kg) was held in a fruit net and crystal sugar (1.0 kg) and neutral spirits (1.8 L) were placed in a glass vessel, which was kept at 15 °C for steeping. The Ume liqueur mixture was stirred once a day for one month, and then once a week. The Ume fruits and liqueur were sampled as follows in order not to change the weight ratio of the Ume fruit to Ume liqueur. Before sampling, the Ume fruits and Ume liqueur were separated and weighed. Two fruits were sampled and weighed, the sampling weight of the Ume liqueur was calculated from the weight ratio of the Ume fruit and Ume liqueur before sampling, and then the calculated weight of liquid was sampled. The volume of the Ume liqueur after steeping for 6 months was calculated by adding on the amount removed by sampling. Analysis of 133Cs and K Each tissue of the Ume fruit was separated using a scalpel. The samples were prepared by wet-ashing using a microwave digestion system (MLS-1200MEGA, Milestone, Bergamo, Italy) according to a previous method 17. The concentration of 133Cs in the samples was determined using inductively coupled plasma–mass spectrometry(Agilent 7700x, Tokyo, Japan) according to a previous method 17. The concentration of potassium (K) in the samples was determined using inductively coupled plasma–emission spectrometry (Shimadzu ICPS-9000E, Kyoto, Japan) according to a previous method 16. The recovery of spiked Cs and K was checked for samples. The concentration of spiked Cs was 1 μg/kg in the Ume flesh and Ume liqueur, and the recovery percentages were 92.3 and 102.3%, respectively. The concentration of spiked K was 1250 mg/kg in the Ume flesh and 1000 mg/kg in Ume liqueur, and the recovery percentages were 96.1 and 98.9%, respectively. Thus, it was confirmed that recovery of the spiked Cs and K was sufficient for a reliable analysis. The detection limits for 133Cs and K in the sample of the Ume fruit were ~0.02 μg/kg and ~0.9 mg/kg, respectively. Analysis of Ume fruit and liqueur The specific gravity of the Ume liqueur was measured by a density hydrometer (DA-300, Kyoto Electronics, Kyoto, Japan). Ethanol concentration was measured by gas chromatography, using a GC14A instrument (Shimadzu), according to a previous method 21. A 2 g aliquot of Ume flesh was mixed with 25 mL of 80% ethanol and shaken overnight, and the extract was used for measuring the concentration of organic acids. The concentrations of the organic acids in the Ume fruit and Ume liqueur were determined by high-performance liquid chromatography (HPLC) using a model LC-10ADVp (Shimadzu) equipped with a conductivity detector (model CDD-10 A; Shimadzu) and a Shim-pack SPR-H column (Shimadzu), according to a previous method 22. Results and discussion Distribution of 133Cs and K in Ume fruit Seven kinds of Ume fruit, uncontaminated with radioactive Cs, were used in this study (Table 1). The proportion of skin, flesh, pit and kernel by weight was 8.2–12.3, 65.4–83.0, 6.1–17.8 and 1.9–4.5%, respectively. The proportion of flesh to whole fruit was highest in the large Ume fruit. The distribution of 133Cs and K in the Ume fruit was examined (Fig. 1). The concentration of 133Cs and K of the Ume fruit was highest in the skin, followed by the kernel or flesh and then the pit in all samples, even though the exact concentrations differed among the samples. While the concentration of K in each tissue ranged from 700 to 6000 mg/kg fresh weight, that of 133Cs was very low in each tissue, ranging from 0.3 to 14.6 μg/kg fresh weight (Fig. 1A). The distribution of 133Cs and K in each tissue was calculated from the weight of each tissue. About 80% of 133Cs and K in all Ume fruits was distributed in the flesh, owing to the high weight ratio of the flesh to whole Ume fruit (Fig. 1B and C). The concentration of 133Cs did not show a high correlation with that of K among the fruit samples. Figure 1Open in figure viewerPowerPoint Concentration of 133Cs and K in Ume fruit parts and distributions. Shi (Ks), Shirokaga (Kansai); Shi (Kt), Shirokaga (Kanto); Shi (ToA), Shirokaga (Tohoku A); Shi (ToB), Shirokaga (Tohoku B); Goj (Ks), Gojiro (Kansai); Bu (To), Bungo (Tohoku); Na (Ks), Nanko (Kansai). Ume liqueur production Next, Ume liqueur making was conducted. Because the skins and flesh could not be separated sufficiently after steeping, the concentrations of 133Cs and K were measured in the flesh with skin, pit and kernel during Ume liqueur making. After steeping in neutral spirits, the kernel in the Ume fruits was soaked with Ume liqueur and the components of the kernel such as minerals appeared to have been extracted into the Ume liqueur. Bungo with the lowest weight ratio of flesh had the lowest volume of Ume liqueur, and Nanko with the highest weight ratio of flesh had the highest volume of Ume liqueur (Table 1). The volume of Ume liqueur appeared high, in line with the weight ratio of flesh in the fruit. As indices of maturation, the specific gravity, colouration (Abs. 420) and organic acid concentration of the Ume liqueur were measured during Ume liqueur making process using Nanko with large fruit (33.2 g/fruit), Shirokaga with standard size fruit (23.2 g/fruit) and Bungo with small fruit (14.9 g/fruit), as shown in Fig. 2. Although the crystal sugar was completely dissolved after one month of Ume liqueur making for all cultivars, the changes in specific gravity and organic acid concentration of the Ume liqueur differed among the cultivars. The specific gravity of the Ume liqueur of Nanko was higher than that of Shirokaga and Bungo at 1 month after steeping. In addition, the specific gravity of the Ume liqueur of Nanko had decreased at 2 months, but that of Shirokaga and Bungo did not change significantly. At 3 months, this index was almost the same for all cultivars. The reason for the decrease in specific gravity over 3 months for Nanko was that the moisture in the Ume fruit was extracted to Ume liqueur and the concentration of sugars decreased. The difference in the change in specific gravity between Nanko and the other two cultivars suggests that the extraction rate depended on fruit size. From 3 to 6 months, the specific gravity increased slightly for all cultivars. The inversion of sucrose to fructose and glucose occurs during Ume liqueur making 18. The hydrolysis reaction of this inversion appeared to decrease moisture in the Ume liqueur and caused the increase in specific gravity. Figure 2Open in figure viewerPowerPoint Changes in specific gravity, colouration and organic acid concentration during Ume liqueur production. The concentration of citric acid was higher than that of malic acid. The concentrations of citric acid and malic acid in Nanko and Shirokaga had increased at 1–2 months after steeping, whereas that in Bungo did not change significantly. The extent of the increase in citric acid was higher for Nanko than for Shirokaga at 2 months after steeping. These results suggest that the difference in the decrease in specific gravity and the increase in citric acid at 2 months after Ume liqueur making was dependent on the differences in extraction rates owing to the differences in fruit size. The components of Nanko with large fruit were extracted to Ume liqueur more slowly as compared with other cultivars. The transfer ratios of organic acids from the Ume fruit to Ume liqueur were 84.4–102.3% in citric acid and 83.3–90.4% in malic acid at 6 months after Ume liqueur making. In contrast, colouration (Abs.420) in all cultivars increased gradually during Ume liqueur making. The change in colouration was due to an amino-carbonyl reaction between sugars and amino compounds extracted from fruit 18. Transfer of 133Cs and K during Ume liqueur making The transfer of 133Cs and K in Ume liqueur during three kinds of Ume liqueur making is shown in Fig. 3. The concentrations of 133Cs and K in Ume fruit after steeping were lower than those before steeping. The transfer ratio of 133Cs from Ume fruit to Ume liqueur was almost the same as that of K. Regarding the cultivars, Shirokaga with standard size fruit and Bungo with small fruit showed a transfer ratio of 70–80% to Ume liqueur at 1 month with no further change thereafter. On the other hand, Nanko with large fruit showed a transfer ratio of 60% after 1 month, and a transfer ratio of 70–80% at 2 months. This difference in 133Cs and K transfer ratio between Nanko and the other cultivars at 1 month was similar to that in the changes in organic acids and specific gravity (Fig. 2). Therefore, the reason for the slower transfer of 133Cs and K of Nanko appears to be due to the slow extraction caused by the large fruit size. The transfer ratios of 133Cs and K were similar among all cultivars after 3 months, and they were also similar to those of organic acids. Figure 3Open in figure viewerPowerPoint Transfer of 133Cs and K during Ume liqueur production. Figure 4 shows the correlation between the 133Cs and K concentrations of the Ume fruits and those of Ume liqueur at 6 months. The 133Cs and K concentration in the raw material of Ume fruits showed a high correlation with those in Ume liqueur. Table 2 shows the Fr and Pf values during Ume liqueur making. The Pf value for Ume liqueur to Ume fruit before steeping was sufficiently low (0.2–0.3). The Pf value for Ume flesh to raw material of Ume flesh (Pf = concentration of 133Cs and K in Ume flesh after steeping/concentration of 133Cs and K in raw material of Ume flesh) was ca. 0.4 for 133Cs and ca. 0.5 for K. The Pf value for Ume flesh to raw material of Ume fruit was ca. 0.3 for 133Cs and ca. 0.4 for K. The Fr of Ume liqueur was ca. 0.8. The Fr of Ume flesh was ca. 0.2. These data show a similar tendency to those in Sekizawa's report 20. Figure 4Open in figure viewerPowerPoint 133Cs and K concentration in Ume fruit and Ume liqueur after 6 months of steeping. Table 2. Processing factors (Pfa) and food retention factors (Frb) and during Ume liqueur making Shirokaga Shirokaga Shirokaga Shirokaga Gojiro Bungo Nanko Average Standard Kansai Kanto Tohoku A Tohoku B Kansai Tohoku Kansai Alcohol (%) 18.2 18.6 18.6 18.5 18.5 18.7 18.5 18.5 0.1 Extract (%) 33.0 33.0 33.6 33.5 33.5 33.4 33.3 33.3 0.2 Absorbance at 420 nm 0.110 0.116 0.087 0.088 0.110 0.210 0.084 0.115 0.044 Weight of Ume liqueur (g) 3248 3065 3236 3313 3159 2882 3349 3179 161 Weight of Ume fruit after 6 months of steeping (g) 477 661 490 413 570 844 377 548 162 Weight of flesh of Ume fruit after 6 months of steeping (g) 349 516 377 330 449 641 261 418 128 Cs Pf(Ume liqueur/Ume fruit) 0.25 0.26 0.25 0.22 0.27 0.23 0.28 0.25 0.02 Pf(Ume flesh/Ume flesh) 0.54 0.44 0.39 0.36 0.76 0.36 0.47 0.42 0.14 Pf(Ume flesh/Ume fruit) 0.43 0.35 0.32 0.29 0.44 0.26 0.38 0.34 0.07 Fr(Ume liqueur/Ume fruit) 0.81 0.80 0.80 0.74 0.84 0.65 0.95 0.78 0.09 Fr(Ume flesh/Ume flesh) 0.19 0.23 0.15 0.12 0.34 0.23 0.12 0.18 0.08 Fr(Ume flesh/Ume fruit) 0.15 0.18 0.12 0.10 0.20 0.17 0.10 0.14 0.04 K Pf(Ume liqueur/Ume fruit) 0.26 0.29 0.28 0.26 0.27 0.25 0.23 0.26 0.02 Pf(Ume flesh/Ume flesh) 0.55 0.57 0.53 0.69 0.60 0.35 0.44 0.52 0.11 Pf(Ume flesh/Ume fruit) 0.41 0.45 0.43 0.48 0.38 0.26 0.35 0.39 0.07 Fr(Ume liqueur/Ume fruit) 0.83 0.89 0.90 0.86 0.85 0.72 0.78 0.83 0.06 Fr(Ume flesh/Ume flesh) 0.19 0.29 0.20 0.23 0.27 0.22 0.11 0.22 0.06 Fr(Ume flesh/Ume fruit) 0.14 0.23 0.16 0.16 0.17 0.17 0.09 0.16 0.04 a : Pf, processing factor (Pf for a foodstuff is the ratio of the Cs or K concentration in the processed food to that in the original raw material). b : Fr, food processing retention factor (Fr is the ratio of Cs or K retained in the food after processing). The above results show that the transfer ratio of Cs and K in Ume liqueur making was almost the same, and that it was dependent on the size of Ume fruit in the early stage of steeping. Ultimately, about 80% of Cs and K in all Ume fruits were transferred from Ume fruit to Ume liqueur, and the Cs and K concentrations of Ume liqueur were ~20% that of Ume fruit before steeping. In addition, the Cs and K concentrations of Ume fruit after steeping were about 50% of that of Ume fruit before steeping. According to the survey results of radiocaesium in ca. 3000 samples of alcoholic beverages, including Ume liqueur produced in Japan in 2011 23, radioactive contaminants were not detected in any samples except for one. Even in the positive sample, the radioactivity was far lower (11 Bq/kg) than the legal limit (100 Bq/kg). 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(2011) Analyses of peptides in sake mash: Forming a profile of bitter-tasting peptides, J. Biosci. Bioeng. 112, 238– 246. 22Kitagaki, H., Katou, T., Isogai, A., Mikami, S., and Shimoi, H. (2008) Inhibition of mitochondrial fragmentation during sake brewing causes high malate production in sake yeast, J. Biosci. Bioeng. 105, 675– 678. 23Hashiguchi, T., Izu, H., and Matsumaru, K. (2013) Survey results of radiocesium in alcoholic beverages and brewing water, pp. 27–31, Report of the National Research Institute of Brewing, Available in Japanese from: http://www.nrib.go.jp/data/nrlpdf/185-03.pdf. Citing Literature Volume122, Issue32016Pages 473-479 FiguresReferencesRelatedInformation