膜技术在杜仲有效成分分离纯化中的应用研究进展

doi:10.11949/0438-1157.20240319

摘要/Abstract

摘要：

杜仲是我国传统名贵药材，具有抗肿瘤、抗氧化、抗骨质疏松、消炎和调节血压等医疗保健作用，其中绿原酸、黄酮等小分子具有较高的药用价值。然而传统中药存在成分复杂，生产工艺落后的问题。膜分离技术具有分离效率高、能耗低、操作简单、无二次污染等特点，在中药的分离纯化中展现出良好的应用前景。由于杜仲是中国特有的药材，国际上对于膜分离杜仲有效成分研究较少，国内对其研究还处在起步阶段，希望综述杜仲有效成分的提取、检测、分离、纯化方法为杜仲有效成分的多极化利用提供理论支撑。分析了膜的分离机理，综述了膜在杜仲有效成分分离纯化中的应用进展，讨论了膜分离过程的影响因素最后，进一步指出膜技术用于中药有效成分分离纯化时在膜材料及膜污染等方面存在的问题，并对未来膜技术在低成本专用膜材料及系统开发和膜污染控制方面的研究进行了展望。

关键词: 绿原酸, 膜, 中药, 纯化, 分离, 杜仲

Abstract:

Eucommia ulmoides is a traditional and precious medicinal material in China, which has the functions of anti-tumor, anti-oxidation, anti-osteoporosis, anti-inflammatory and blood pressure regulation. Its active ingredients such as chlorogenic acid and flavonoids have high medicinal value. However, the traditional Chinese medicine has the problems of complex composition and backward production technology. Membrane separation technology has the characteristics of high separation efficiency, low energy consumption, simple operation and no secondary pollution, which shows a good application prospect in the separation and purification of traditional Chinese medicine. As Eucommia ulmoides is a unique medicinal material in China, there are few studies on membrane separation of Eucommia ulmoides active components in the world, and the domestic research on it is still in the initial stage. It is hoped that the extraction, detection, separation and purification methods of Eucommia ulmoides active components will be reviewed to provide theoretical support for the multipolar utilization of eucommia active components. The separation mechanism of membrane was analyzed, the application of membrane in the separation and purification of Eucommia ulmoides was reviewed, and the factors affecting the separation process were discussed. Finally, the problems of membrane materials and membrane pollution in the separation and purification of Eucommia ulmoides active components were further pointed out, and the future research of membrane technology in the development of low-cost special membrane materials and systems and membrane pollution control was prospected.

Key words: chlorogenic acid, membrane, traditional Chinese medicine, separation, purification, Eucommia ulmoides

中图分类号:

TQ 028.8

顾天宇, 陈献富, 王思琪, 徐鹏, 邱鸣慧, 范益群. 膜技术在杜仲有效成分分离纯化中的应用研究进展[J]. 化工学报, DOI: 10.11949/0438-1157.20240319.

Tianyu GU, Xianfu CHEN, Siqi WANG, Peng XU, Minghui QIU, Yiqun FAN. Application of membranes for separation and purification of Eucommia ulmoides active ingredients[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240319.

图/表 11

表1 杜仲有效成分功能性

Table 1 Functional of some active pharmaceutical ingredients in Eu

成分名称	代表物质	中国药典的要求	功能性
木脂素类	松脂醇二葡萄糖苷	含量不得低于0.10%	双向调节血压
苯丙素类	绿原酸	叶中含量不得低于0.080%	杀菌、消炎、抗衰老等
环烯醚萜类	桃叶珊瑚苷	-	镇痛、抗菌消炎和利尿等
黄酮类	芦丁	-	抗氧化、抗病毒、抗炎、抗菌、降血脂等

表2 杜仲提取液体系有效成分和杂质的相对分子质量

Table 2 Relative molecular masses of some active pharmaceutical ingredients and impurities in Eu extract

成分名称	分子量/Da	成分名称	分子量/Da
淀粉	50k-500k	绿原酸	354
树脂、果胶	15k-300k	黄酮类	300-600
蛋白质	5k-500k	车业草苷	414
多糖	5k-500k	松脂醇二葡萄糖苷	683
单糖、二糖	180-360	桃叶珊瑚苷	346
细菌	40k-200k	京尼平苷酸	374
鞣酸	500-3000	氨基酸	75-210

表3 杜仲有效成分不同提取方法的比较

Table 3 Comparison of different extraction methods for active ingredients of Eu

方法	优势	劣势	目标物	收率/含量
浸提	提取率高能耗低、成本低	提取周期长	绿原酸杜仲胶绿原酸	4.36 mg/g ^[28] 4.42% ^[29] 1.06% ^[30]
超声	提取时间短、效率高、温度低	受频率影响、处理量小	总黄酮杜仲多糖	1.45% ^[31] 4.02%±0.03% ^[32]
微波	加热均匀、效率高、环保	适用于热稳定性的物质	绿原酸杜仲多糖	3.59% ^[33] 12.31% ^[34]
超临界萃取	效率高而且能耗较少	萃取物中有夹带剂残留	杜仲翅果油杜仲籽油	14.73% ^[35] 28.75g/100g ^[36]

图1 水提醇沉工艺改进前后流程图

Fig.1 Flow chart of Chinese medicine production process before and after improvement

图2 杜仲提取液陶瓷膜分离过程示意图

Fig.2 Schematic diagram of ceramic membrane separation process for Eu extract

图3 不同孔径陶瓷膜的渗透性能和分离性能[66]

Fig.3 Permeance and separation performances of ceramic membranes with different pore sizes [66]

图4 进料浓度对PEI膜性能的影响[74]

Fig.4 Effect of feed concentration on the PEI membrane performance [74]

表4 干燥固体的成分分析［79］

Table 4 Chemical compositions of dried solids ［79］

样品	质量分数/(mg·g^-1)
样品	蛋白质	绿原酸
G1	8.84	7.31
G2	5.17	7.99
G3	4.95	5.84
G4	0.85	8.88

图5 膜分离过程的操作方式注:(a) 死端过滤 (b) 错流过滤

Fig.5 Operating modes of membrane separation process

图6 不同孔径的PAA改性膜的表征及膜过滤BSA溶液和纯水洗涤过程中的归一化通量[93]

Fig.6 Characterization of PAA-modified membrane with pore size & normalized flux of original and PAA-modified membranes in BSA solution filtration and pure water washing process [93]

图7 通过原膜、污染膜和清洁膜相对通量差异评估的化学清洗效率[95]

Fig.7 The efficiency of chemical cleaning assessed by the relative similarity in flux values of pristine, fouled, and cleaned membranes [95]

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