甘肅天水產(chǎn)花椒果實(shí)資源化學(xué)研究
發(fā)布時(shí)間：2018-08-29 09:34
【摘要】：蕓香科花椒屬植物花椒Zanthoxylum bungeanum Maxim.為藥食兩用植物,其干燥成熟果皮入藥稱花椒(Zanthoxyli Pericarpium),具有溫中止痛、殺蟲(chóng)止癢的功效,為中醫(yī)臨床常用溫里藥味,常用于脘腹冷痛、蟲(chóng)積腹痛、嘔吐泄瀉、蛔蟲(chóng)病等癥的治療;亦可外用治療濕疹瘙癢�；ń贩N子入藥稱椒目(Zanthoxyli Semen),具有滲水利濕、祛痰平喘之功,臨床主要用于水腫脹滿、哮喘等癥的治療。我國(guó)花椒資源豐富,產(chǎn)量巨大�，F(xiàn)代研究顯示,花椒果實(shí)中含有多種類型的資源性化學(xué)成分,在醫(yī)藥、食品、保健品和化妝品等多個(gè)領(lǐng)域應(yīng)用廣泛。在對(duì)相關(guān)文獻(xiàn)進(jìn)行整理分析,系統(tǒng)綜述我國(guó)花椒屬藥用植物資源研究現(xiàn)狀的基礎(chǔ)上,本研究選擇甘肅天水地區(qū)產(chǎn)花椒成熟果實(shí)為研究對(duì)象,基于中藥資源化學(xué)的研究思路與方法,立足于資源多途徑、多層次利用原則,以花椒資源的綜合利用和產(chǎn)業(yè)化發(fā)展為目的,對(duì)花椒果實(shí)開(kāi)展了資源性化學(xué)成分分析與評(píng)價(jià),并就其潛在資源價(jià)值與產(chǎn)品開(kāi)發(fā)作了初步探索,以期為花椒果實(shí)資源的綜合利用與產(chǎn)業(yè)化開(kāi)發(fā)提供科學(xué)依據(jù),也為提升花椒資源的利用效率和效益提供支撐。1.花椒果實(shí)資源性化學(xué)成分分析與評(píng)價(jià)為明確花椒果實(shí)中資源性物質(zhì)的組成及分布特征,充分釋放花椒果實(shí)資源價(jià)值,本研究分別采用氣相色譜-質(zhì)譜聯(lián)用法(GC-MS)、高效液相色譜法(HPLC-PAD/ELSD)、超高效液相色譜-質(zhì)譜聯(lián)用法(UPLC-TQ/MS)等技術(shù)手段,對(duì)花椒成熟果實(shí)的果皮、種子及種子油中所含的揮發(fā)油類、酚酸類、黃酮類等與藥用功效相關(guān)的資源性活性物質(zhì),以及脂肪酸類、糖類、蛋白質(zhì)及氨基酸類、核苷及堿基類等與營(yíng)養(yǎng)保健相關(guān)的資源性物質(zhì)進(jìn)行了系統(tǒng)分析與評(píng)價(jià)。(1)揮發(fā)油類資源性化學(xué)成分分析結(jié)果顯示,花椒果皮、種子中存在多種不同類型的揮發(fā)性成分,其中萜類及其含氧衍生物為揮發(fā)油中的主要組分,乙酸芳樟酯在花椒果實(shí)各部位揮發(fā)油所占比例相對(duì)較高。比較所檢測(cè)花椒果實(shí)不同部位,發(fā)現(xiàn)果皮中的揮發(fā)油類成分較種子組成相對(duì)更為豐富,主要成分的含量也相對(duì)較高。(2)黃酮類和酚酸類資源性化學(xué)成分分析結(jié)果表明,花椒果實(shí)中的黃酮類和酚酸類資源性化學(xué)成分主要分布于果皮部位,其主要組成成分綠原酸、槲皮素-3-O-蕓香糖苷、金絲桃苷、槲皮素-3-O-葡萄糖苷和槲皮苷的含量分別為2.15、1.99、3.94、1.69、2.04 mg/g;而花椒種子和花椒種子油中未檢測(cè)到上述酚酸類和黃酮類資源性化學(xué)成分。(3)脂肪酸類資源性化學(xué)成分研究顯示,花椒果皮和種子中的脂肪酸總量分別為108.42mg/g、331.63mg/g;由花椒種子壓榨制備的種子油中脂肪酸總量可達(dá)966.04mg/g,單不飽和及多不飽和脂肪酸總量約占其總量的78.95%,其中尤以油酸、亞油酸和亞麻酸含量相對(duì)較高,其質(zhì)量分?jǐn)?shù)分別達(dá)293.35mg/g、246.56mg/g、184.41mg/g。(4)糖類資源性化學(xué)成分分析結(jié)果顯示,花椒果皮與種子中可溶性多糖總含量分別為96.33mg/g、19.18mg/g;單糖/寡糖總含量分別為9.71mg/g和3.78mg/g�？梢�(jiàn),花椒果實(shí)中的糖類組分主要分布于果皮,而中性多糖為花椒果實(shí)主要多糖類型。(5)核苷及堿基類資源性化學(xué)成分分析結(jié)果顯示,花椒果皮與種子中的核苷及堿基類化學(xué)成分在組成與含量上均存在差異,花椒果皮與種子中核苷及堿基類成分的總含量分別為2.14mg/g、3.94mg/g,果皮與種子中均以尿苷含量最高分別為0.47mg/g、1.22mg/g,腺苷、肌苷和胸腺嘧啶在花椒果皮和種子中所占比例也相對(duì)較高。(6)總蛋白及氨基酸類資源性化學(xué)成分分析結(jié)果顯示,花椒果皮中總蛋白的含量(92.32mg/g)遠(yuǎn)高于種子(10.97mg/g);果皮中水解氨基酸總量約為52.90mg/g,其中以脯氨酸的含量為最高(9.95mg/g);種子中水解氨基酸總量約為4.66mg/g,以谷氨酸所占比例為最高(1.03mg/g)�；ń饭麑�(shí)中游離氨基酸測(cè)定結(jié)果表明,其在花椒果皮中的總量約為11.02mg/g,在花椒種子中含量相對(duì)較低,僅為0.57mg/g,且果皮和種子中游離氨基酸均為精氨酸和脯氨酸含量相對(duì)較高。2.花椒果實(shí)資源化利用研究(1)采用卵清白蛋白復(fù)合寒冷與過(guò)勞刺激致寒飲蘊(yùn)肺哮喘大鼠模型,對(duì)花椒種子水提物及種子油的效應(yīng)特征進(jìn)行評(píng)價(jià)研究,結(jié)果顯示,花椒種子水提物與種子油對(duì)模型大鼠血液炎性細(xì)胞、炎癥因子、肺組織病理學(xué)損傷均有一定程度的干預(yù)作用,各劑量花椒種子水提物給藥組及種子油給藥組哮喘大鼠均有趨于正�；内厔�(shì),表明花椒種子具有一定的防治哮喘作用。(2)基于代謝組學(xué)技術(shù)對(duì)花椒種子干預(yù)寒飲蘊(yùn)肺哮喘大鼠的作用機(jī)制研究發(fā)現(xiàn),模型組大鼠與正常組大鼠比較,在其血清和尿液中共鑒定28個(gè)潛在生物標(biāo)志物。其中,血清中鑒定的潛在生物標(biāo)志物涉及的代謝通路中,亞油酸代謝、花生四烯酸代謝、乙醛酸和二羧酸代謝和甘油磷脂代謝通路影響值相對(duì)較高;大鼠尿液中所鑒定的潛在生物標(biāo)志物涉及的代謝通路中,谷氨酰胺與谷氨酸代謝,戊糖與葡萄糖醛酸生物轉(zhuǎn)化,丙氨酸、天門冬氨酸和谷氨酸代謝,煙酸鹽與煙酰胺代謝,鞘脂類代謝、精氨酸與脯氨酸代謝通路影響值相對(duì)較高。對(duì)花椒種子水提物和種子油藥物治療組大鼠的血清與尿液中的上述潛在標(biāo)志性代謝物分析發(fā)現(xiàn),試藥通過(guò)影響亞油酸代謝、甘油磷脂代謝、戊糖和葡萄糖醛酸酯生物轉(zhuǎn)化、煙酸鹽和煙酰胺代謝這幾條代謝途徑對(duì)哮喘進(jìn)行干預(yù)治療。(3)對(duì)花椒種子油、花椒果皮揮發(fā)油與酰胺部位體外抗氧化活性研究結(jié)果表明,酰胺部位對(duì)DPPH和ABTS表現(xiàn)出較強(qiáng)的清除能力,其IC50(半數(shù)抑制濃度值)分別為1.55mg/m L、0.23 mg/m L;揮發(fā)油對(duì)ABTS自由基的清除效果顯著,IC50值為1.07 mg/m L,揮發(fā)油和種子油對(duì)DPPH自由基的清除能力較酰胺部位弱,IC50值分別為19.36 mg/m L和16.38 mg/m L;花椒揮發(fā)油在FRAP試驗(yàn)中表現(xiàn)還原能力最強(qiáng),其次為酰胺部位,三組樣品的抗氧化水平在FeSO4線性范圍內(nèi)呈現(xiàn)出一定的量效相關(guān)性。
[Abstract]:Zanthoxylum bungeanum Maxim, a Rutaceae Zanthoxylum plant, is an edible and medicinal plant. Its dried and ripe peel is called Zanthoxyli Pericarpium. It has the effect of stopping pain and killing itching. It is commonly used in traditional Chinese medicine clinic. It is used in the treatment of cold abdominal pain, epigastric pain, vomiting and diarrhea, ascariasis, etc. Zanthoxyli Semen is used to treat eczema and itching. Zanthoxyli Semen has the functions of water permeation, dampness elimination, expectoration and relieving asthma. It is mainly used in the treatment of edema, asthma and other symptoms. China is rich in Zanthoxyli resources and has a huge production. Modern research shows that Zanthoxyli Semen contains a variety of resource chemical components in the fruit, in medicine, food, health care. It is widely used in many fields, such as cosmetics and so on. On the basis of sorting out and analyzing the related literature and systematically reviewing the research status of Zanthoxylum medicinal plant resources in China, the ripe fruit of Zanthoxylum bungeanum in Tianshui area of Gansu province was selected as the research object. Based on the research ideas and methods of Chinese medicine resources chemistry, the resources of Zanthoxylum bungeanum bungeanum bungean Based on the principle of hierarchical utilization, the chemical composition of Zanthoxylum bungeanum was analyzed and evaluated for the purpose of comprehensive utilization and industrialization development of Zanthoxylum bungeanum resources, and the potential resource value and product development were preliminarily explored in order to provide scientific basis for the comprehensive utilization and industrialization development of Zanthoxylum bungeanum resources as well as to raise the capital of Zanthoxylum bungeanum. The analysis and evaluation of the chemical constituents of Zanthoxylum bungeanum fruits were carried out to clarify the composition and distribution characteristics of the resource substances in Zanthoxylum bungeanum fruits and fully release the resource value of Zanthoxylum bungeanum fruits. Phase chromatography-mass spectrometry (UPLC-TQ/MS) and other technical means, pepper mature fruit peel, seeds and seed oil contained in the volatile oils, phenolic acids, flavonoids and other medicinal efficacy-related resource active substances, as well as fatty acids, carbohydrates, proteins and amino acids, nucleosides and alkaloids related to nutrition and health resources The results showed that there were many different types of volatile components in the peel and seeds of Zanthoxylum bungeanum. Terpenoids and their oxygen-containing derivatives were the main components of volatile oils. Linalyl acetate accounted for a relatively high proportion of volatile oils in Zanthoxylum bungeanum fruit. Comparing the different parts of Zanthoxylum bungeanum fruits, it was found that the volatile oils in the peel were more abundant than those in the seed, and the contents of the main components were also relatively high. (2) The analysis of flavonoids and phenolic acids showed that the flavonoids and phenolic acids in Zanthoxylum bungeanum fruits were mainly distributed in the peel. The contents of chlorogenic acid, quercetin-3-O-rutin, hyperoside, quercetin-3-O-glucoside and quercetin were 2.15, 1.99, 3.94, 1.69, 2.04 mg/g, respectively, while the phenolic acids and flavonoids were not detected in Zanthoxylum bungeanum seeds and Zanthoxylum bungeanum seed oils. (3) The study of fatty acid resource chemical constituents was obvious. The results showed that the total fatty acids in peel and seed of Zanthoxylum bungeanum were 108.42 mg/g and 331.63 mg/g, respectively; the total fatty acids in seed oil prepared by pressing Zanthoxylum bungeanum bungeanum seeds were 966.04 mg/g, and the total monounsaturated and polyunsaturated fatty acids accounted for 78.95% of the total fatty acids, especially oleic acid, linoleic acid and linolenic acid, with relatively high contents and their mass fractions respectively. The total contents of soluble polysaccharides in peel and seed of Zanthoxylum bungeanum were 96.33 mg / g and 19.18 mg / g respectively, and the total contents of monosaccharide / oligosaccharides were 9.71 mg / g and 3.78 mg / g respectively. (5) Nucleosides and alkaloids in the peel and seed of Zanthoxylum bungeanum were different in composition and content. The total contents of nucleosides and alkaloids in the peel and seed of Zanthoxylum bungeanum were 2.14mg/g and 3.94mg/g, respectively. Uridine was found in the peel and seed of Zanthoxylum bungeanum bungeanum. The contents of adenosine, inosine and thymidine in peel and seed of Zanthoxylum bungeanum were 0.47 mg/g, 1.22 mg/g, respectively. (6) The analysis of total protein and amino acid resources showed that the total protein content in peel of Zanthoxylum bungeanum (92.32 mg/g) was much higher than that in seed (10.97 mg/g), and the total hydrolyzed amino acid content in peel was about 52.90 M. The content of proline was the highest (9.95 mg/g), the total amount of hydrolyzed amino acids in seeds was about 4.66 mg/g, and the proportion of glutamic acid was the highest (1.03 mg/g). The total content of free amino acids in Pepper pericarp was about 11.02 mg/g, and the content of free amino acids in pepper seed was relatively low (0.57 mg/g). The content of free amino acids in seeds was relatively high. 2. Utilization of Zanthoxylum bungeanum L. fruits was studied. (1) The effects of water extract and seed oil from Zanthoxylum bungeanum L. seeds on asthmatic rats induced by cold and overwork combined with ovalbumin were evaluated. Seed oil could interfere with inflammatory cells, inflammatory factors and lung histopathological injury in model rats to a certain extent, and the asthmatic rats tended to normalize in the water extract treatment group and the seed oil treatment group of Zanthoxylum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bun The mechanism of Zanthoxylum bungeanum seed intervention on asthmatic rats with cold-retention lung syndrome was studied. 28 potential biomarkers were identified in serum and urine of model rats compared with normal rats. Among them, linoleic acid metabolism, arachidonic acid metabolism, glyoxylic acid and dicarboxylic acid metabolism were involved in the potential biomarkers identified in serum. Among the metabolic pathways identified in rat urine, glutamine and glutamate metabolism, pentose and glucuronic acid biotransformation, alanine, aspartate and glutamate metabolism, nicotinate and nicotinamide metabolism, sphingolipid metabolism, arginine and glutamate metabolism were involved. Proline metabolic pathways were relatively high. The analysis of the above potential markers in serum and urine of rats treated with water extract and seed oil from Zanthoxylum bungeanum seeds showed that the tested drugs affected linoleic acid metabolism, glycerol phospholipid metabolism, pentose and glucuronide ester biotransformation, nicotinate and nicotinamide metabolism. (3) In vitro antioxidant activity of Zanthoxylum bungeanum seed oil, Zanthoxylum bungeanum peel volatile oil and amide fraction showed strong scavenging ability to DPPH and ABTS, and their IC50 (half inhibitory concentration) were 1.55 mg/ml, 0.23 mg/ml, respectively. The IC50 value was 1.07 mg/ml, the scavenging ability of volatile oil and seed oil to DPPH free radical was weaker than that of amide part, IC50 value was 19.36 mg/ml and 16.38 mg/ml, respectively; the volatile oil of Zanthoxylum bungeanum showed the strongest reducing ability in FRAP test, followed by amide part, and the antioxidant level of the three groups of samples showed a certain dose-effect phase in the linear range of FeSO4. Customs.
【學(xué)位授予單位】：江蘇大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：R284.1
本文編號(hào)：2210805
[Abstract]:Zanthoxylum bungeanum Maxim, a Rutaceae Zanthoxylum plant, is an edible and medicinal plant. Its dried and ripe peel is called Zanthoxyli Pericarpium. It has the effect of stopping pain and killing itching. It is commonly used in traditional Chinese medicine clinic. It is used in the treatment of cold abdominal pain, epigastric pain, vomiting and diarrhea, ascariasis, etc. Zanthoxyli Semen is used to treat eczema and itching. Zanthoxyli Semen has the functions of water permeation, dampness elimination, expectoration and relieving asthma. It is mainly used in the treatment of edema, asthma and other symptoms. China is rich in Zanthoxyli resources and has a huge production. Modern research shows that Zanthoxyli Semen contains a variety of resource chemical components in the fruit, in medicine, food, health care. It is widely used in many fields, such as cosmetics and so on. On the basis of sorting out and analyzing the related literature and systematically reviewing the research status of Zanthoxylum medicinal plant resources in China, the ripe fruit of Zanthoxylum bungeanum in Tianshui area of Gansu province was selected as the research object. Based on the research ideas and methods of Chinese medicine resources chemistry, the resources of Zanthoxylum bungeanum bungeanum bungean Based on the principle of hierarchical utilization, the chemical composition of Zanthoxylum bungeanum was analyzed and evaluated for the purpose of comprehensive utilization and industrialization development of Zanthoxylum bungeanum resources, and the potential resource value and product development were preliminarily explored in order to provide scientific basis for the comprehensive utilization and industrialization development of Zanthoxylum bungeanum resources as well as to raise the capital of Zanthoxylum bungeanum. The analysis and evaluation of the chemical constituents of Zanthoxylum bungeanum fruits were carried out to clarify the composition and distribution characteristics of the resource substances in Zanthoxylum bungeanum fruits and fully release the resource value of Zanthoxylum bungeanum fruits. Phase chromatography-mass spectrometry (UPLC-TQ/MS) and other technical means, pepper mature fruit peel, seeds and seed oil contained in the volatile oils, phenolic acids, flavonoids and other medicinal efficacy-related resource active substances, as well as fatty acids, carbohydrates, proteins and amino acids, nucleosides and alkaloids related to nutrition and health resources The results showed that there were many different types of volatile components in the peel and seeds of Zanthoxylum bungeanum. Terpenoids and their oxygen-containing derivatives were the main components of volatile oils. Linalyl acetate accounted for a relatively high proportion of volatile oils in Zanthoxylum bungeanum fruit. Comparing the different parts of Zanthoxylum bungeanum fruits, it was found that the volatile oils in the peel were more abundant than those in the seed, and the contents of the main components were also relatively high. (2) The analysis of flavonoids and phenolic acids showed that the flavonoids and phenolic acids in Zanthoxylum bungeanum fruits were mainly distributed in the peel. The contents of chlorogenic acid, quercetin-3-O-rutin, hyperoside, quercetin-3-O-glucoside and quercetin were 2.15, 1.99, 3.94, 1.69, 2.04 mg/g, respectively, while the phenolic acids and flavonoids were not detected in Zanthoxylum bungeanum seeds and Zanthoxylum bungeanum seed oils. (3) The study of fatty acid resource chemical constituents was obvious. The results showed that the total fatty acids in peel and seed of Zanthoxylum bungeanum were 108.42 mg/g and 331.63 mg/g, respectively; the total fatty acids in seed oil prepared by pressing Zanthoxylum bungeanum bungeanum seeds were 966.04 mg/g, and the total monounsaturated and polyunsaturated fatty acids accounted for 78.95% of the total fatty acids, especially oleic acid, linoleic acid and linolenic acid, with relatively high contents and their mass fractions respectively. The total contents of soluble polysaccharides in peel and seed of Zanthoxylum bungeanum were 96.33 mg / g and 19.18 mg / g respectively, and the total contents of monosaccharide / oligosaccharides were 9.71 mg / g and 3.78 mg / g respectively. (5) Nucleosides and alkaloids in the peel and seed of Zanthoxylum bungeanum were different in composition and content. The total contents of nucleosides and alkaloids in the peel and seed of Zanthoxylum bungeanum were 2.14mg/g and 3.94mg/g, respectively. Uridine was found in the peel and seed of Zanthoxylum bungeanum bungeanum. The contents of adenosine, inosine and thymidine in peel and seed of Zanthoxylum bungeanum were 0.47 mg/g, 1.22 mg/g, respectively. (6) The analysis of total protein and amino acid resources showed that the total protein content in peel of Zanthoxylum bungeanum (92.32 mg/g) was much higher than that in seed (10.97 mg/g), and the total hydrolyzed amino acid content in peel was about 52.90 M. The content of proline was the highest (9.95 mg/g), the total amount of hydrolyzed amino acids in seeds was about 4.66 mg/g, and the proportion of glutamic acid was the highest (1.03 mg/g). The total content of free amino acids in Pepper pericarp was about 11.02 mg/g, and the content of free amino acids in pepper seed was relatively low (0.57 mg/g). The content of free amino acids in seeds was relatively high. 2. Utilization of Zanthoxylum bungeanum L. fruits was studied. (1) The effects of water extract and seed oil from Zanthoxylum bungeanum L. seeds on asthmatic rats induced by cold and overwork combined with ovalbumin were evaluated. Seed oil could interfere with inflammatory cells, inflammatory factors and lung histopathological injury in model rats to a certain extent, and the asthmatic rats tended to normalize in the water extract treatment group and the seed oil treatment group of Zanthoxylum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bungeanum bun The mechanism of Zanthoxylum bungeanum seed intervention on asthmatic rats with cold-retention lung syndrome was studied. 28 potential biomarkers were identified in serum and urine of model rats compared with normal rats. Among them, linoleic acid metabolism, arachidonic acid metabolism, glyoxylic acid and dicarboxylic acid metabolism were involved in the potential biomarkers identified in serum. Among the metabolic pathways identified in rat urine, glutamine and glutamate metabolism, pentose and glucuronic acid biotransformation, alanine, aspartate and glutamate metabolism, nicotinate and nicotinamide metabolism, sphingolipid metabolism, arginine and glutamate metabolism were involved. Proline metabolic pathways were relatively high. The analysis of the above potential markers in serum and urine of rats treated with water extract and seed oil from Zanthoxylum bungeanum seeds showed that the tested drugs affected linoleic acid metabolism, glycerol phospholipid metabolism, pentose and glucuronide ester biotransformation, nicotinate and nicotinamide metabolism. (3) In vitro antioxidant activity of Zanthoxylum bungeanum seed oil, Zanthoxylum bungeanum peel volatile oil and amide fraction showed strong scavenging ability to DPPH and ABTS, and their IC50 (half inhibitory concentration) were 1.55 mg/ml, 0.23 mg/ml, respectively. The IC50 value was 1.07 mg/ml, the scavenging ability of volatile oil and seed oil to DPPH free radical was weaker than that of amide part, IC50 value was 19.36 mg/ml and 16.38 mg/ml, respectively; the volatile oil of Zanthoxylum bungeanum showed the strongest reducing ability in FRAP test, followed by amide part, and the antioxidant level of the three groups of samples showed a certain dose-effect phase in the linear range of FeSO4. Customs.
【學(xué)位授予單位】：江蘇大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：R284.1
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