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中文题名:

 四种香薷属植物防治嗜卷书虱活性物质研究    

姓名:

 张嘉玮    

保密级别:

 公开    

论文语种:

 chi    

学科代码:

 0705Z1    

学科专业:

 自然资源    

学生类型:

 硕士    

学位:

 理学硕士    

学位类型:

 学术学位    

学位年度:

 2024    

校区:

 北京校区培养    

学院:

 地理科学学部    

研究方向:

 中药资源    

第一导师姓名:

 杜树山    

第一导师单位:

 地理科学学部    

提交日期:

 2023-12-08    

答辩日期:

 2023-12-07    

外文题名:

 Secondary metabolites of four Elsholtzia spp. against Liposcelis bostrychophila    

中文关键词:

 香薷属 ; 嗜卷书虱 ; 次生代谢物质 ; 化学多样性    

外文关键词:

 Elsholtzia ; Liposcelis bostrychophila ; secondary metabolites ; chemical diversity    

中文摘要:

在我国的发展战略中,中医药正在逐年扩大影响力。中药材及饮片储备在其中具有举足轻重的地位。然而从中药材采收到制成饮片的全过程都需要进行储藏和运输,在此过程中中药材极易受到外界环境的影响,而发生霉变、虫蛀、受潮,不仅会降低其经济价值,影响药效,更可能产生有毒有害物质。嗜卷书虱(啮虫目:虱啮科)是一种危害严重的仓储害虫,生殖繁衍能力强,食源复杂,对仓储中药材和饮片极易产生严重威胁。然而,传统的化学合成杀虫剂虽然价格低、效果好、见效快、使用方便,但也会对仓储物及环境造成污染,甚至导致害虫产生抗药性。在我国传统中药材及饮片的保藏中使用的对抗同贮法是应用中药材中挥发性物质的相互影响来防止害虫滋生的方法,但是并不是所有中药材及饮片都可以找到有效同贮药材,该法也难以在大宗单一药材储藏时应用。因此通过拓展对抗同贮的思路,使用植物挥发性提取物进行中药材仓储害虫防治可以进一步发展对抗同贮的概念,应用现代技术生产植物源杀虫剂,从而在保护中药材质量的同时避免化学合成农药对中药材及饮片的损害。

唇形科香薷属植物资源分布广泛,且富含挥发性成分,具有开发为植物源杀虫剂的潜力。本研究通过控制采集时间和地点,收集四种香薷属植物(四方蒿、水香薷、野拔子、白香薷)的样品并提取挥发油,利用气相色谱-质谱联用技术(GC-MS)测定挥发油的化学组成。以嗜卷书虱为靶标昆虫,测定四种香薷属植物挥发油对其的触杀和熏蒸活性。从数据库中收集采样地和采集时间的环境因子,通过相关系数分析阐释环境因子-挥发油化学成分-抗虫活性之间的关系。选择富含去氢香薷酮和香薷酮的野拔子和白香薷挥发油,采用硅胶柱层析法对其进行分离,并应用核磁共振法对得到的化合物进行鉴定,测试其抗虫活性。本研究得到的主要结果与结论如下:

1、对四种香薷属植物各选取12个地点于2021年7至9月采集样品,提取其挥发油,测定其成分并针对嗜卷书虱进行抗虫活性测试。结果显示四方蒿挥发油的化学成分多样性最高,可分为五种化学型;水香薷主要成分为去氢香薷酮和香芹酮,可分为四种化学型;野拔子挥发油中去氢香薷酮均大于90%;而白香薷挥发油中香薷酮均大于90%。抗虫活性中,触杀活性的顺序为野拔子>水香薷>白香薷>四方蒿,且嗜卷书虱对野拔子挥发油浓度变化的响应更为敏感而对四方蒿挥发油较不敏感。熏蒸活性中,四种香薷属植物的LC50之间差异不显著。在环境因子-化学成分-抗虫活性间的相关性分析中,多种环境因子与四种香薷属植物挥发油成分间相关性显著;挥发油中的多种成分与抗虫活性间也存在显著相关性;抗虫活性与环境因子间也存在显著相关系数,降水量与水香薷、野拔子和白香薷的触杀活性呈正相关关系,但是其中存在的内在关联仍需进一步研究。

2、对四种香薷属植物各选取一固定采样地,于2021年9月至2022年8月采集样品,提取其挥发油,测定其成分并进行针对嗜卷书虱的抗虫活性测试。结果显示四方蒿挥发油的主要成分随时间变化很大,且无一定规律性。水香薷挥发油中香芹酮和去氢香薷酮的比例存在季节性变化。野拔子挥发油中去氢香薷酮的含量在夏季最高。白香薷中香薷酮的含量全年均大于90%。触杀活性中,野拔子的活性略强于水香薷,但差异不显著,而四方蒿和白香薷的活性整体弱于野拔子和水香薷。从熏蒸活性来看,野拔子、水香薷和白香薷的活性总体差异不大,四方蒿的活性最弱。在环境因子-化学成分-抗虫活性间的相关性分析中,温度、总降水量、预测反照率、向下的表面热辐射以及土壤温度和土壤含水层体积与水香薷、野拔子和白香薷的抗虫活性均有显著正相关关系;而表面压力与四种香薷属植物的抗虫活性均存在负相关关系。

3、分离并鉴定四种香薷属植物中野拔子和白香薷挥发油中主要的成分并进行针对嗜卷书虱的抗虫活性测试。分离出的两个化合物经鉴定为去氢香薷酮和香薷酮;抗虫活性结果显示去氢香薷酮的触杀和熏蒸活性都显著强于香薷酮,且触杀活性显著强于阳性对照药除虫菊酯。

本研究探索了四种香薷属植物挥发油成分与采集地点和时间的关系,并测定其对嗜卷书虱的抗虫活性。通过多种分析方法揭示了四种香薷属植物挥发油成分间的关系;并应用相关系数分析对环境因子-化学成分-抗虫活性间的关系进行了初探,确定了四种香薷属植物挥发油中抗虫次生代谢物质的累积规律及影响因素;此外测定了挥发油中重要成分去氢香薷酮和香薷酮的抗虫活性,为拓展传统中药思维理论,进一步发掘该四种香薷属植物的应用潜力提供了思路和数据。

外文摘要:

Traditional Chinese Medicine (TCM) is expanding increasingly its influence in the strategy of the health development. The stock of Chinese herbal medicines’ raw materials and the pieces used in clinical practices plays a pivotal role in the development of TCM. However, the whole process, from the harvesting to the making of pieces of Chinese herbal medicines, needs to be stored and transported, through which Chinese herbal medicines are susceptible to the influence of the external environment, causing moulds, insect damage and dampness, which reduces their economic value and medicinal efficacy, and consequently generates toxic and hazardous substances. Liposcelis bostrychophila (Psocoptera: Liposcelididae) is a severe storage pest with strong reproductive ability and a complex food source, which can easily threaten the storage of Chinese herbal medicines. However, although the traditional chemical synthetic insecticides are low-priced, effective, fast-acting and easy to use, they may also pollute the storage materials and the environment, even leading to drug resistance of the pests. In China, the method of ‘antagonistic storage’ is used in the storage of traditional Chinese herbal medicines using the counteracting of medicines’ volatile substances to prevent pest breeding, but not all Chinese herbal medicines can find an effective co-storage medicinal material; moreover, the antagonistic storage method is difficult to be applied in the bulk of a single medicinal materials storage. Therefore, by expanding the idea of the antagonistic storage method, the use of plant volatile extracts for the pest control in herbal medicine storage can further develop the concept of antagonistic storage and invent plant-derived insecticides through modern technology to reach the goal of ensuring the quality of herbal medicines and avoiding the damage caused by chemically synthesised pesticides on the herbs at the same time.

Plants in genus Elsholtzia of the family Lamiaceae are widely distributed and rich in volatile components, and have the potential in plant-derived insecticide development. In this study, we collected samples of four Elsholtzia spp. (E. blanda, E. kachinensis, E. rugulosa and E. winitiana) by controlling the time and place of collection and extracted their essential oils (EOs). The chemical constitutions of the EOs were determined by using gas chromatography-mass spectrometry (GC-MS). Then the EOs were used to test the contact and fumigant activities against the target insect, L. bostrychophila. The environmental factors at the collecting location and time were obtained from databases, and the correlation coefficients were calculated to explain the relationship between the environmental factors, the chemical compositions of the EOs, and the insecticidal activities. The EOs of E. rugulosa and E. winitiana, whose major component were dehydroelsholtzia ketone and elsholtzia ketone, was selected to separate by silica gel column chromatography, and the compounds obtained were identified by nuclear magnetic resonance (NMR) and tested for their insecticidal activity. The main results and conclusions obtained in this study are as follows:

1. Samples of each of the four Elsholtzia spp. were collected from 12 locations from July to September 2021, and their EOs were extracted, determined, and tested for insecticidal activities against L. bostrychophila. The results showed that the EO of E. blanda had the highest chemical diversity and could be classified into five chemotypes; E. kachinensis was mainly composed of dehydroelsholtzia ketone and carvone and could be classified into four chemotypes; the dehydroelsholtzia ketone in the EOs of E. rugulosa was greater than 90%; and the elsholtzia ketone in the EOs of E. winitiana was greater than 90%. In insecticidal activity tests, the order of contact activities was E. rugulosa > E. kachinensis > E. winitiana > E. blanda, and the response of L. bostrychophila to the change of the concentration of the EOs of E. rugulosa was more sensitive to that of E. blanda. In fumigant activity tests, the differences in LC50 among the four Elsholtzia spp. were insignificant. The correlation coefficients between environmental factors, chemical compositions and insecticidal activity were analysed. Many correlation coefficients between environmental factors and EOs of Elsholtzia spp. were significant; there was also a significant correlation between EOs and insecticidal activity. Moreover, some significant correlation coefficients existed between insecticidal activity and environmental factors. Total precipitation was positively correlated to the insecticidal activities of EOs of E. kachinensis, E. rugulosa and E. winitiana. However, the intrinsic correlation between these two variables needs to be further researched.

2. Samples of each of the four Elsholtzia spp. were collected from September 2021 to August 2022, and their EOs were extracted, determined, and tested for insecticidal activities against L. bostrychophila. The results showed that the main components of the EO of E. blanda varied greatly over time without a certain regularity. The proportion of carvone and dehydroelsholtzia ketone in the EOs of E. kachinensis varied seasonally. The content of dehydroelsholtzia ketone in the EO of E. rugulosa was highest in summer. The contents of elsholtzia ketone in E. winitiana were greater than 90% throughout the year. In terms of contact activity, the activity of E. rugulosa was slightly better than that of E. kachinensis, but the difference was not significant, while the activity of E. blanda and E. winitiana was weaker than that of E. rugulosa and E. kachinensis as a whole. Regarding fumigant activity, there was little difference between the activities of E. rugulosa, E. kachinensis and E. winitiana, with E. blanda being the least active. In the correlation analysis between environmental factors, the chemical compositions of the EOs, and the insecticidal activities, temperature, total precipitation, forecast albedo, surface thermal radiation downwards, soil temperature and volume of soil water layers had a positive correlation to the insecticidal activities of EOs of E. kachinensis, E. rugulosa and E. winitiana; surface pressure was negatively correlated to the insecticidal activities of four Elsholtzia spp.

3. The main components of the EOs of E. rugulosa and E. winitiana were isolated and identified, and tested for their insecticidal activity against the L. bostrychophila. The two isolated compounds were identified as dehydroelsholtzia ketone and elsholtzia ketone. The results of insecticidal tests showed that dehydroelsholtzia ketone was significantly stronger than elsholtzia ketone in contact and fumigant activities, even the contact activity of which was significantly stronger than that of the positive control pyrethrin.

This study explored the relationship between the EO composition of four Elsholtzia spp. and the location and time of collection, and determined their insecticidal activity against L. bostrychophila. Various analytical methods revealed the relationships among the components of the EOs of the four Elsholtzia spp. The relationships among environmental factors – chemical components – insecticidal activities were initially explored by correlation coefficient analysis, which determined the accumulation pattern of the insecticidal secondary metabolites in the EOs of the four Elsholtzia spp. and their influencing factors. In addition, the insecticidal activities of dehydroelsholtzia ketone and elsholtzia ketone, which were important components of the EOs against L. bostrychophila, were determined. The results provide ideas and data for expanding the theory of TCM thinking and further exploring the application potential of these four Elsholtzia spp.

参考文献总数:

 173    

馆藏号:

 硕0705Z1/24054    

开放日期:

 2024-12-10    

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