Study on Processe of Aristolochia Contorta Bge. Based on Characteristic Spectrum Combined with Effective Toxicity Value and Appearance Characters
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摘要:
目的 基于特征图谱结合效毒值与外观性状的测定，研究蜜马兜铃炮制过程中毒性成分的变化规律。 方法 采用高效液相建立17批蜜马兜铃特征图谱, 对炮制蜜用量、稀释倍数、润制时间、炒制时间进行考察; 在炮制过程中隔点取样, 测定色度值及特征图谱, 进行外观性状与内在效毒值的综合评价。 结果 蜜马兜铃特征图谱标定了10个共有峰, 指认6个特征峰, 其中峰2为木兰花碱、峰5为7-羟基马兜铃酸A、峰6为马兜铃酸D、峰8为马兜铃酸B、峰9为马兜铃内酰胺Ⅰ、峰10为马兜铃酸Ⅰ。前处理考察确定蜜用量为每100 kg待炮炙品用炼蜜25 kg, 炼蜜加入3倍沸水稀释, 润制时间为60 min。炒制过程显示, 蜜马兜铃毒性成分的峰面积随着炮制时间的延长呈现明显的下降趋势, 木兰花碱与5个毒性成分的效毒值也逐渐增大。结合外观性状与内在效毒值进行综合评价, 炮制19~27 min的样品排名前5, 炮制时间确定为23~27 min。 结论 马兜铃经炮制后, 毒性成分的相对含量降低, 效毒值增加, 毒性减弱。效毒值结合外观性状的质量评价方法, 可为毒性中药饮片的炮制提供参考。 Abstract:OBJECTIVE Based on the characteristic spectrum combined with the determination of effective Toxiciy appearance character, to study the changes of toxic components in the processing of Aristolochia contorta Bge. METHODS The characteristic chromatogram of 17 batches of Aristolochia contorta Bge. was established by HPLC, and the parameters of honey, dilution times, humid time and frying time were investigated. Samples were taken at intervals in the process, the chromaticity value and characteristic map were measured, and the comprehensive evaluation of appearance characters and intrinsic toxicity values was carried out. RESULTS 10 common peaks were calibrated and 6 characteristic peaks were identified in the characteristic spectrum of Aristolochia contorta Bge., among which peak 2 was magnoflorine, peak 5 was 7-hydroxy aristolochic acid A, peak 6 was aristolochic acid D, peak 8 was aristolochic acid B, peak 9 was aristolochic acidⅠ, and peak 10 was aristolochic acidⅠ. According to the pre-treatment investigation, the dosage of honey was 25 kg of refined honey per 100 kg of products to be roasted, the honey was diluted by 3 times amount of water, and the humid time was 60 min. The processing process showed that the peak area of the toxic components of Aristolochia contorta Bge. decreased obviously with the processing time, and the toxic value of magnoflorine and five toxic components gradually increased. According to the comprehensive evaluation of appearance traits and intrinsic toxicity value, the samples processed for 19-27 min ranked in the top five, processing time was determined to be 23-27 min. CONCLUSION After Aristolochia contorta Bge. is processed, the relative contents of toxic components decreases, while the toxic value increases. The quality evaluation method of effective toxicity value combined with appearance characteristics can provide reference for the processing of toxic Chinese herbal pieces -
图 1 蜜马兜铃多批次炮制品特征图谱叠加图
注: 2.木兰花碱; 5.7-羟基马兜铃酸A; 6.马兜铃酸D(S); 8.马兜铃酸B; 9.马兜铃内酰胺Ⅰ; 10.马兜铃酸Ⅰ
Figure 1. The overlayed characteristic spectrum of multi batch of processe of Aristolochia Contorta Bge.
图 2 蜜马兜铃饮片对照特征图谱与特征峰指认
注: A.蜜马兜铃饮片对照特征图谱; B.混合对照品特征图谱；2.木兰花碱; 5.7-羟基马兜铃酸A; 6.马兜铃酸D(S); 8.马兜铃酸B; 9.马兜铃内酰胺Ⅰ; 10.马兜铃酸Ⅰ
Figure 2. Comparative characteristic spectrum and identification of characteristic peaks of Aristolochia Contorta Bge.
图 3 蜜马兜铃不同蜜用量各特征峰面积柱形图
Figure 3. Column chart of characteristic peak area about honey dosage of the processing of Aristolochia Contorta Bge.
图 4 蜜马兜铃不同蜜稀释倍数各特征峰面积柱形图
Figure 4. Column chart of characteristic peak area about honey diluted of the processing of Aristolochia Contorta Bge.
图 5 蜜马兜铃不同润制时间各特征峰面积柱形图
Figure 5. Column chart of characteristic peak area about humid time of the processing of Aristolochia Contorta Bge.
图 6 蜜马兜铃不同炒制功率和时间各特征峰面积柱形图
Figure 6. Column Chart of characteristic peak area about different processing power and time of Aristolochia Contorta Bge.
图 7 蜜马兜铃炮制过程样品特征图谱叠加图
注: 2.木兰花碱; 5.7-羟基马兜铃酸A; 6.马兜铃酸D; 8.马兜铃酸B; 9.马兜铃内酰胺Ⅰ; 10.马兜铃酸Ⅰ
Figure 7. The overlayed characteristic spectrum of multi batch of the processing of Aristolochia Contorta Bge.
图 8 蜜马兜铃炮制过程样品粉末图
Figure 8. Sample powder chart of the processing of Aristolochia Contorta Bge.
图 9 蜜马兜铃炮制过程样品PCA得分图
Figure 9. PCA score chart of the processing of Aristolochia Contorta Bge.
图 10 蜜马兜铃炮制过程样品聚类谱系图
Figure 10. Cluster pedigree chart of the processing of Aristolochia Contorta Bge.
表 1 马兜铃与蜜马兜铃来源信息表
Table 1. Source information of Aristolochia contorta Bge. and processing of Aristolochia contorta Bge.
序号 马兜铃药材批号 对应蜜马兜铃批号 药材来源 1 MDL01 MMDL01 广东省广州市清平中药材市场 2 MDL02 MMDL02 河北省安国市中药材市场 3 MDL03 MMDL03 河北省安国市中药材市场 4 MDL04 MMDL04 安徽省毫州市谯城区康美中药城 5 MDL05 MMDL05 安徽省毫州市谯城区康美中药城 6 MDL06 MMDL06 安徽省毫州市谯城区康美中药城 7 MDL07 MMDL07 广西省玉林市中药港 8 MDL08 MMDL08 广西省玉林市中药港 9 MDL09 MMDL09 黑龙江省哈尔滨市 10 MDL10 MMDL10 黑龙江省哈尔滨市 11 MDL11 MMDL11 黑龙江省哈尔滨市 12 MDL12 MMDL12 黑龙江省哈尔滨市 13 MDL13 MMDL13 黑龙江省哈尔滨市 14 MDL14 MMDL14 黑龙江省哈尔滨市 15 MDL15 MMDL15 黑龙江省尚志市 16 MDL16 MMDL16 黑龙江省尚志市 17 MDL17 MMDL17 黑龙江省尚志市 
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表 2 蜜马兜铃饮片炮制过程取样信息表
Table 2. Sample information table of the processing of Aristolochia Contorta Bge.
取样点 炮制批号 炒制时间/min 出锅药温/℃ 1 MZ01 - - 2 MZ02 9 62~65 3 MZ03 13 86~90 4 MZ04 15 100~110 5 MZ05 17 113~115 6 MZ06 19 115~120 7 MZ07 21 120~125 8 MZ08 23 125~130 9 MZ09 25 131~133 10 MZ10 27 134~140 11 MZ11 29 138~145 12 MZ12 31 142~148 13 MZ13 33 143~150 14 MZ14 35 138~143 15 MZ15 37 135~139
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表 3 蜜马兜铃炮制过程样品特征峰峰面积相对生品比值结果
Table 3. Results of ratio of characteristic peak area of the processing of Aristolochia Contorta Bge.
批号 峰1 峰2 峰3 峰4 峰5 峰6 峰7 峰8 峰9 峰10 5个毒性成分变化率/% 其余5个成分变化率/% MZ01 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 0 0 MZ02 0.892 0.921 0.910 0.824 0.903 0.928 1.117 1.007 1.138 1.027 0.97 -4.90 MZ03 0.899 0.825 0.821 0.883 0.845 0.915 0.948 0.925 0.971 0.895 -8.65 -12.43 MZ04 0.825 0.789 0.536 0.824 0.757 0.837 1.030 0.893 0.716 0.862 -19.57 -21.06 MZ05 0.819 0.783 0.531 0.817 0.751 0.831 1.022 0.886 0.710 0.855 -20.21 -21.68 MZ06 0.740 0.768 0.213 0.801 0.651 0.794 1.343 0.815 0.499 0.804 -29.77 -24.26 MZ07 0.736 0.723 0.126 0.725 0.569 0.705 1.751 0.691 0.438 0.787 -35.89 -17.98 MZ08 0.753 0.824 0.104 0.782 0.493 0.629 1.839 0.575 0.419 0.658 -43.76 -13.72 MZ09 0.747 0.740 0.072 0.748 0.452 0.570 1.840 0.569 0.396 0.635 -47.17 -16.47 MZ10 0.736 0.793 0.058 0.683 0.425 0.513 1.770 0.512 0.378 0.583 -51.33 -18.87 MZ11 0.717 0.865 0.053 0.733 0.430 0.521 1.824 0.565 0.388 0.606 -49.89 -16.17 MZ12 0.731 0.828 0.056 0.695 0.421 0.495 1.770 0.480 0.373 0.573 -52.43 -18.32 MZ13 0.766 0.812 0.046 0.695 0.408 0.493 1.827 0.473 0.404 0.588 -51.44 -16.79 MZ14 0.731 0.756 0.037 0.690 0.376 0.468 1.752 0.434 0.377 0.550 -54.53 -20.51 MZ15 0.722 0.719 0.041 0.612 0.372 0.428 1.769 0.428 0.380 0.544 -55.82 -21.71
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表 4 蜜马兜铃炮制过程样品色度值与水分值
Table 4. Chromatic value and moisture value of the processing of Aristolochia Contorta Bge.
批号 炮制时间/min L* a* b* ΔL* Δa* Δb* ΔE* 水分/% MZ01 0 53 7 32 - - - - 11.19 MZ02 9 49 7 30 -4 0 -2 4.47 12.86 MZ03 13 50 8 30 -3 1 -2 3.74 7.37 MZ04 15 52 8 30 -1 1 -2 2.45 5.30 MZ05 17 52 7 31 -1 0 -1 1.41 4.66 MZ06 19 53 6 30 0 -1 -2 2.24 3.97 MZ07 21 48 8 29 -5 1 -3 5.92 4.18 MZ08 23 47 7 28 -6 0 -4 7.21 3.51 MZ09 25 45 8 30 -8 1 -2 8.31 2.90 MZ10 27 43 8 30 -10 1 -2 10.25 2.90 MZ11 29 42 10 29 -11 3 -3 11.79 2.76 MZ12 31 41 9 25 -12 2 -7 14.04 2.60 MZ13 33 40 10 23 -13 3 -9 16.09 2.40 MZ14 35 39 10 22 -14 3 -10 17.46 2.28 平均值 45.5 8.3 27.7 -7.5 1.3 -4.3 9.0 4.3 最小值 36.0 6.0 21.0 -17.0 -1.0 -11.0 1.4 2.1 最大值 53.0 10.0 31.0 0.0 3.0 -1.0 20.5 12.9
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表 5 蜜马兜铃炮制过程样品饮片评分表
Table 5. The sample score of the processing of Aristolochia Contorta Bge.
批号 炮制时间/min 颜色 质地 气味 总评分 综合评分 果皮 种仁 果皮 种仁 果皮 种仁 果皮 种仁 MZ01 0 10 15 15 12 20 20 45 47 46 MZ02 9 20 15 15 12 20 20 55 47 51 MZ03 13 25 25 25 20 20 20 70 65 67 MZ04 15 30 25 25 25 20 20 75 70 72 MZ05 17 38 34 30 25 20 20 88 79 83 MZ06 19 40 37 30 29 30 30 100 96 98 MZ07 21 38 40 28 30 30 30 96 100 98 MZ08 23 36 35 28 28 25 25 89 88 88 MZ09 25 32 25 25 25 25 25 82 75 78 MZ10 27 25 25 25 25 25 25 75 75 75 MZ11 29 23 18 15 15 20 20 58 53 55 MZ12 31 18 18 15 15 20 20 53 53 53 MZ13 33 15 18 15 12 10 10 40 40 40 MZ14 35 10 12 10 12 10 10 30 34 32 MZ15 37 10 12 10 10 10 10 30 32 31
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表 6 蜜马兜铃炮制过程样品5个毒性成分的效毒值及评分
Table 6. Toxicity value and score of five toxic componentsof the processing of Aristolochia Contorta Bge.
批号 炮制时间/min 木兰花碱/7-羟基马兜铃酸A 木兰花碱/马兜铃酸D 木兰花碱/马兜铃酸B 木兰花碱/马兜铃内酰胺Ⅰ 木兰花碱/马兜铃内酰胺Ⅰ 效毒值 评分 效毒值 评分 效毒值 评分 效毒值 评分 效毒值 评分 MZ01 0 0.18 49.77 0.10 59.51 0.72 57.44 0.10 44.92 0.09 69.20 MZ02 9 0.18 50.77 0.10 59.12 0.66 52.57 0.08 36.38 0.08 62.06 MZ03 13 0.18 48.55 0.09 53.66 0.64 51.22 0.09 38.17 0.08 63.75 MZ04 15 0.19 51.87 0.09 56.09 0.63 50.74 0.11 49.52 0.08 63.35 MZ05 17 0.19 51.87 0.09 56.09 0.63 50.74 0.11 49.52 0.08 63.35 MZ06 19 0.21 58.73 0.09 57.55 0.68 54.14 0.16 69.20 0.09 66.08 MZ07 21 0.23 63.23 0.10 61.04 0.75 60.07 0.17 74.04 0.08 63.58 MZ08 23 0.30 83.23 0.13 78.00 1.03 82.24 0.20 88.26 0.11 86.71 MZ09 25 0.30 81.36 0.13 77.17 0.93 74.70 0.19 83.82 0.10 80.55 MZ10 27 0.34 92.81 0.15 92.04 1.11 88.98 0.22 94.32 0.12 94.14 MZ11 29 0.36 99.99 0.16 98.70 1.10 87.85 0.23 100.00 0.13 98.76 MZ12 31 0.36 97.83 0.16 99.57 1.24 99.00 0.23 99.66 0.13 100.00 MZ13 33 0.36 99.12 0.16 97.90 1.23 98.50 0.21 90.31 0.12 95.47 MZ14 35 0.36 100.00 0.16 96.22 1.25 100.00 0.21 90.11 0.12 95.08 MZ15 37 0.35 96.13 0.16 100.00 1.20 96.44 0.20 84.93 0.12 91.52
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表 7 蜜马兜铃炮制过程样品外观与内在质量综合得分与排序
Table 7. Comprehensive score and ranking of appearance and internal quality of the processing of Aristolochia Contorta Bge.
批号 炮制时间/min 综合得分 排名 MZ01 0 51.13 15 MZ02 9 51.41 14 MZ03 13 59.17 13 MZ04 15 63.29 11 MZ05 17 68.70 8 MZ06 19 79.48 4 MZ07 21 81.29 3 MZ08 23 86.07 1 MZ09 25 78.85 5 MZ10 27 83.73 2 MZ11 29 76.17 6 MZ12 31 76.11 7 MZ13 33 68.13 9 MZ14 35 64.23 10 MZ15 37 62.45 12
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