Degradation of Multi-Components Polycyclic Aromatic Hydrocarbons in Oyster by Photodynamic Technology
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摘要: 目的：寻求一种高效、经济、安全可靠的新型食品中有机污染物降解方法。方法：通过比较三种光敏剂（姜黄素、核黄素、金丝桃素）对牡蛎肉外观品质的影响以及光动力对水溶液中多环芳烃的降解效果，对其进行工艺优化，在最优条件下探究光动力对牡蛎中多环芳烃的降解作用。结果：当光敏剂浓度为10 µmol/L时，富集量高达89.68%~92.22%，且牡蛎肉为正常的奶白色，并未发生变化。而当浓度为20 µmol/L时，富集量仅为71.90%~78.62%，牡蛎肉颜色发生肉眼可见的由白色到黄色的变化。与核黄素和金丝桃素相比，姜黄素介导的光动力降解效果最佳，光照15 min时降解率高达91.08%。因此，确定的最佳条件为：光敏剂为姜黄素，浓度10 µmol/L，光照时间15 min。在最优条件下，相比于空白对照组，光动力对牡蛎中多环芳烃的降解率达到21.92%~88.46%。结论：光动力方法可有效降解牡蛎中的多环芳烃，该技术对于水产品中残留多环芳烃的降解是一种可行的方法，应用前景广阔。Abstract: Objective: Finding an efficient, economic, safe and reliable method for degradation of organic pollutants in food. Methods: By comparing the effects of three photosensitizers (curcumin, riboflavin and hypericin) on the appearance quality of oyster meat and the degradation effect of photodynamic technology (PDT) on polycyclic aromatic hydrocarbons (PAHs) in aqueous solution, the process conditions were optimized, and the degradation effect of photodynamic on PAHs in oysters was explored under the optimal conditions. Results: When the concentration of photosensitizer was 10 μmol/L, the accumulation was up to 89.68%~92.22%, and the color of oyster meat was normal milky white without any change. However, when the concentration was 20 µmol/L, the accumulation was only 71.90%~78.62%, and the color of oyster meat changed significantly from white to yellow. Compared with riboflavin and hypericin, the degradation effect of curcumin-mediated photodynamic on PAHs was the best, and the degradation rate was up to 91.08% under 15 min illumination. Therefore, the optimal conditions were determined as follows: The photosensitizer was curcumin, the concentration was 10 µmol/L, and the illumination time was 15 min. Compared with the blank control group, the degradation rate of PAHs in oysters in the PDT group reached 21.92%~88.46% under the optimal conditions. Conclusion: PDT could effectively degrade polycyclic aromatic hydrocarbons (PAHs) in oysters. This technology would be a feasible method for the degradation of residual PAHs in aquatic products and would have a broad application prospect.
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Key words:
- oyster /
- polycyclic aromatic hydrocarbons /
- photodynamic technique /
- curcumin /
- degradation
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图 2 核黄素富集前后水体及牡蛎肉颜色变化
Figure 2. Color changes of water and oyster meat before and after bio-accumulation of riboflavin
图 3 金丝桃素富集前后水体及牡蛎肉颜色变化
Figure 3. Color Changes of water and oyster meat before and after bio-accumulation of hypericin
图 4 光动力对水溶液中多环芳烃的降解效果
Figure 4. Degradation effect of photodynamic technology on PAHs in aqueous solution
注：A.水溶液中多环芳烃的降解效果；B.水溶液中多环芳烃的降解率；每个时间点各组之间进行比较，标有不同字母表示组间差异显著（P<0.05），相同字母代表组间没有显著性差异（P>0.05）。
图 5 多环芳烃的气相色谱-质谱总离子流图
Figure 5. Gas chromatography-mass spectrogram of PAHs
注：A.PAHs标准溶液的气相色谱-质谱图；B.空白对照组PAHs的气相色谱-质谱图；C.光动力组PAHs的气相色谱-质谱图；1.萘；2.苊烯；3.苊；4.芴；5.菲；6.蒽；7.荧蒽；8.芘；9.苯并[a]蒽；10. 䓛 ；11.苯并[b]荧蒽；12.苯并[k]荧蒽；13.苯并[a]芘；14.茚并[1,2, 3-c,d]芘；15.二苯并[a, h]蒽；16.苯并[g,h,i]苝。
图 6 光动力对牡蛎中多环芳烃的降解效果
Figure 6. Degradation effect of photodynamic technology on PAHs in oysters
注：与空白对照组相比，**表示P<0.01，***表示P<0.001。
表 1 牡蛎中富集姜黄素的量
Table 1. Quantity of curcumin bio-accumulate by oysters
姜黄素浓度
（µmol/L）富集前水体
的吸光值富集前水体中
姜黄素质量（mg）富集后海水
的吸光值富集后水体中
姜黄素质量（mg）姜黄素
富集量（%）牡蛎中姜黄素
添加量（mg/g）5 0.0394±0.0025 10.05±0.60 0.0004±0.0002 0.85±0.04 98.98±0.07 0.092±0.06 10 0.0702±0.0008 17.33±0.20 0.0056±0.0006 2.09±0.15 91.96±0.89 0.152±0.02 20 0.1474±0.0040 35.57±0.94 0.0315±0.0006 8.19±0.15 78.62±0.01 0.274±0.09 注：数据以平均值±标准差的形式表示，每个样品进行三次平行实验。表2~表4同。 
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表 2 牡蛎中富集核黄素的量
Table 2. Quantity of riboflavin bio-accumulate by oysters
核黄素浓度
（µmol/L）富集前水体
的吸光值富集前水体中
核黄素质量（mg）富集后海水
的吸光值富集后水体中
核黄素质量（mg）核黄素
富集量（%）牡蛎中核黄素
添加量（mg/g）5 0.0109±0.0010 9.79±0.67 0.0002±0.0002 1.79±1.55 98.15±0.17 0.080±0.07 10 0.0245±0.0012 18.93±0.78 0.0019±0.0006 3.45±0.39 92.22±0.38 0.155±0.08 20 0.0508±0.0006 36.27±0.40 0.0139±0.0004 11.60±0.28 72.62±0.33 0.247±0.04
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表 3 牡蛎中富集金丝桃素的量
Table 3. Quantity of hypericin bio-accumulate by oysters
金丝桃素浓度
（µmol/L）富集前水体
的吸光值富集前水体中金丝桃
素质量（mg）富集后海水
的吸光值富集后水体中金丝桃
素质量（mg）金丝桃素
富集量（%）牡蛎中金丝桃素
添加量（mg/g）5 0.0056±0.0003 12.95±0.50 0.0005±0.0003 4.37±0.44 91.06±0.48 0.086±0.05 10 0.0107±0.0004 21.47±0.59 0.0011±0.0004 5.44±0.68 89.68±0.34 0.160±0.06 20 0.0253±0.0004 46.02±0.59 0.0071±0.0004 15.41±0.59 71.90±0.39 0.306±0.06
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表 4 光动力对牡蛎中多环芳烃的降解率
Table 4. Degradation rate of PAHs in oyster by photodynamic technology
序号 PAHs 出峰时间（min） 降解率（%） 1 萘 4.494 75.09±0.34 2 苊烯 5.859 58.02±0.12 3 苊 6.010 88.46±0.67 4 芴 6.441 47.58±1.49 5 菲 7.261 31.82±0.12 6 蒽 7.301 36.73±0.95 7 荧蒽 8.290 24.89±1.25 8 芘 8.505 21.92±1.28 9 苯并[a]蒽 9.883 25.49±0.63 10 䓛 9.949 25.00±0.97 11 苯并[b]荧蒽 − − 12 苯并[k]荧蒽 − − 13 苯并[a]芘 − − 14 茚并[1,2,3-c,d]芘 − − 15 二苯并[a,h]蒽 − − 16 苯并[g,h,i]苝 − −
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