4 resultados para C21

em Chinese Academy of Sciences Institutional Repositories Grid Portal


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  本实验对三种萝藦科植物通光散(Marsdenia tenacissima)、黑水藤(Biondia insignis Tsiang)和徐长卿(Cynanchum Paniculatum)中的C21甾体化合物进行了研究。从通光散藤茎乙酸乙酯提取物的水解产物中,分离得到两类八个C21甾类甙元。经光谱鉴定,它们的结构分别为11α-O-(2-甲基)-丁酰基-12β-O-顺芷酰通光藤甙元乙(1),11α-O-乙酰基-12β-O-乙酰基通光藤甙元乙(2),11α-O-(2-甲基)-丁酰基-12β-O-乙酰基通光藤甙元乙(3), 11α-O-苯甲酰基-12β-O-乙酰基通光藤甙元乙(4), 11α-O-顺芷酰基-12β-O-乙酰基通光藤甙元乙(5)11α-O-顺芷酰基-12β-O-顺芷酰基通光藤甙元乙(6),12β-O-乙酰基通光藤甙元甲(7)和12β-O-顺芷酰基通光藤甙元甲(8)。其中,化合物2和8为新化合物。从黑水藤乙醇提取物的水解产物中,分离得到了两个C21甾体化合物。经1D、2D NMR技术鉴定,分别为(3β,14β,15β,17β)-3, 14-二羟基-15,16-裂-孕甾-5-烯-15-醛-16-半缩醛-20-酮(1)和白前甙元C(2)。其中1为15,16-裂环的新骨架类型的C21甾体化合物,命名为黑水藤甙元甲。从采购于昆明、浙江、湖南三地药材市场的徐长卿的根及根茎中,分离得到了18个化合物(其中昆明徐长卿6个,浙江徐长卿9个,湖南徐长卿3个)。经光谱数据分析,这些化合物被鉴定为:cynapanoside-C (1), cynapanoside-A (2), 白前甙元B 3-O-β-D-磁嘛吡喃糖甙(3),白前甙元C 3-O-β-D-葡萄吡喃糖基-(1 → 4)-α-L-2-脱氧洋地黄吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-夹竹吡喃糖甙(4),白前甙元C3-O-β-D-葡萄吡喃糖基-(1 → 4)-α-D-夹竹桃吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-夹竹桃吡喃糖甙(5),白前甙元C 3-O-β-D-葡萄吡喃糖基-(1 → 4)-β-D-葡萄吡喃糖基-(1 → 4)-α-D-夹竹桃吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-夹竹桃吡喃糖甙(6),cynatratoside-B (7),cynatratoside-C (8);glaucoside A(9),新白薇甙元B 3-O-β-L-磁嘛吡喃糖基-(1 → 4)-β-D-洋黄吡喃糖基-(1 → 4)-β-D-夹竹桃吡喃糖甙(10),白前甙元 A 3-O-α-L-磁嘛吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(11),白前甙元 B 3-O-α-L-磁糖基吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(12),白前甙元D 3-O-α-L-磁嘛吡喃糖基(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(13),白前甙元 C 3-O-β-D-葡萄吡喃糖基-(1 → 4)-β-D-葡萄吡喃糖基-(1 → 4)-α-L-2-脱氧洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖基-(1 → 4)-β-D-夹竹桃吡喃糖甙(14),白前甙元 C 3-O-β-D-葡萄吡喃糖基-(1 → 4)-β-D-葡萄吡喃糖基-(1 → 4)-α-L-磁嘛吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-夹竹桃吡喃糖甙(15),白前甙元 B 3-O-α-D-夹竹桃吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(16),白前甙元 D 3-O-α-D-夹竹桃吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(17),白前甙元月B 3-O-α-L-磁嘛吡喃糖基-(1 → 4)-β-D-洋地黄吡喃糖基-(1 → 4)-β-D-磁嘛吡喃糖甙(18)。其中,化合物3-6,10-18为新化合物,10的甙元为一个新甙元,命名为新白薇甙无B。

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本学位论文共有5章。第一章报道白芍的化学成分及芍药苷的微生物转化研究成果;第二章报道天山雪莲的化学成分研究;第三章报道两面针的化学成分研究;第四章报道通关藤的化学成分研究成果;第五章概述了花椒属植物中最近十年报道的新化合物及药理研究情况。 在第1章的第一部分报道了白芍(Paeonia lactiflora Pall.)的化学成分。我们采用正、反相硅胶柱层析等各种分离方法,从白芍的干燥根中共分离出14个化合物,其中1个为新化合物,其结构通过波谱分析证实为没食子酰白芍苷,另外还有2个为首次从该植物中分离得到。第二部分报道了芍药苷的微生物转化生产芍药苷代谢素-I的研究,从15株厌氧菌中筛选出10株有转化活性的菌株,其中短乳杆菌Lactobacillus brevis AS1.12的转化活性最好,对其转化条件进行了初步的筛选,确定了相对合理的转化工艺。 在第2章报道了天山雪莲(Saussurea involucrate Kar.et Kir.)全草乙醇提取物化学成分的分离纯化和结构鉴定。通过正、反相硅胶柱层析等分离纯化和MS、NMR等波谱解析,共分离鉴定了28个化合物,结构类型分属于黄酮、倍半萜和木脂素等,其中2个新倍半萜化合物的结构分别表征为6α-羟基云木香酸6-β-D-吡喃葡萄糖苷和11βH-11,13-二氢去氢云木香内酯8α-O-(6′-乙酰)-β-D-吡喃葡萄糖苷。 第3章报道了两面针(Zanthoxylum nitidum (Roxb.)DC.)干燥根的乙醇提取物化学成分的分离纯化和结构鉴定。通过正、反相硅胶柱层析等分离纯化和MS、NMR等波谱解析以及X-射线单晶衍射,共分离鉴定了16个生物碱,结构类型分属于苯并啡啶类、喹啉类和阿朴啡类等,其中2个新苯并啡啶类生物碱的结构分别表征为二聚双氢两面针碱和丙酮基双氢崖定椒碱。 第4章报道了通关藤(Marsdenia tenacissima (Roxb.) Wight et Arn.)水提取物化学成分的分离纯化和结构鉴定。通过正、反相硅胶柱层析等分离纯化和MS、NMR等波谱解析以及X-射线单晶衍射,共分离鉴定了14个化合物,结构类型均属于C21多羟基甾醇,其中4个新化合物tenacigenoside A, tenacigenoside B, tenacigenoside C和tenacigenoside D的结构分别表征为3-O-6-deoxy-3-O-methyl-β-D-allopyranosyl-(1→4)-β-D-oleandropyranosyl-17β-tenacigenin B (62), 3-O-2,6- dideoxy-4-O-methyl-D-lyxo-hexopyranosly-11α-O- methylbutyryl-12β-O-acetyl-tenacigenin B (63), 3-O-6-deoxy-3-O-methyl-β-D- allopyranosyl-(1→4)-β-D-oleandropyranosyl-11α-O-tigloyl-tenacigenin C (64)和3-O-6-deoxy-3-O-methyl-β-D-allopyranosyl-(1→4)-β-D-oleandropyranosyl-11α-O-2- methylbutyryl-tenacigenin C (65)。 第5章概述了花椒属植物的化学成分及药理活性研究进展。 This dissertation consists of 5 chapters. The first chapter elaborate the phytochemical investigation of Paeonia lactiflora Pall., and microbial transformation of paeoniforin. The second, third and four chapters elaborate the phytochemical investigation of Saussurea involucrate Kar.et Kir., Zanthoxylum nitidum (Roxb.) DC. and Marsdenia tenacissima (Roxb.) Wight et Arn., respectively. Chapter 5 is a review on chemical constituents and bioactivities of Zanthoxylum species. The part one of chapter 1 focus on the isolation and identification of chemical constituents from P. lactiflora. Fourteen compounds were isolated from the roots of P. lactiflora by repeat column chromatography over normal and reversed phase silica gel. Among them, one is a new compound and the structure was suggested as galloyl-albiflorin by spectral evidence. In addition, two compounds were firstly reported in this plant. The part 2 is about microbial transformation of paeoniforin. Chapters 2, 3 and 4 were isolations and identifications of chemical constituents from S. involucrate, Z. nitidum and M. tenacissima, respectively. From the aerial parts of S. involucrate, 28 compounds including 7 flavonoids and 13 sesquiterpenoids were isolated and identified. Among them, 2 new compounds were characterized as 6α-hydroxycostic acid 6-β-D-glucoside and 11βH-11,13-dihydrodehydro- costuslactone 8α-O-(6'-acetyl)-β-D-glucoside, respectively, by means of spectroscopic analysis. Otherwise, 11 ones were firstly reported from this plant. The third chapter is about the phytochemical investigation of Z. nitidum. Sixteen compounds were isolated and identified. Among them, 2 new benzophenanthridine alkaloids were characterized as 8-acetonyldihydrofagaridine and 1,3-bis(8-dihydronitidinyl)-acetone by spectroscopic analysis. The fourth chapter is about the phytochemical investigation of M. tenacissima. Fourteen compounds were isolated and identified. Among them, 4 new compounds, tenacigenosides A~D, were characterized as 3-O-6-deoxy-3-O-methyl-β-D-allopyranosyl-(1→4)-β-D-oleandropyranosyl-17β- tenacigenin B, 3-O-2,6-dideoxy-4-O-methyl-D-lyxo-hexopyranosly-11α-O-methyl butyryl-12β-O-acetyl-tenacigenin B, 3-O-6-deoxy-3-O-methyl-β-D-allopyranosyl- (1→4)-β-D-oleandropyranosyl-11α-O-tigloyl-tenacigenin C, and 3-O-6-deoxy-3-O- methyl-β-D-allopyranosyl-(1→4)-β-D-oleandropyranosyl-11α-O-2-methylbutyryl- tenacigenin C. Chapter 5 is a review on recent progress in bioactive constituents from plants of Zanthoxylum species.

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A large number of mantle-derived fluid activities occurred in the Dongying Sag. On the basis of the studies on the geochemical characteristics of these fluids in this sag, the spatial distribution of biomarkers in petroleum and their relationships with the parameters of mantle-derived fluids were studied, to reveal the influence of mantle-derived fluids on the biomarkers and to evaluate the reliability of these biomarkers when applied to oil-source correlation and maturity analysis. Most biomarkers used in oil correlation kept the characteristics of their sources during burial thermal evolution. Even some of them were not influenced by mantle derived fluids, such as the relative content of C27-C29 steroid(ααα20R)and C21/C23 tricyclic terpane. However, Pr/Ph and C35/C34 hopanes were sensitive to both heat energy and materiel input by the mantle-derived fluids. γ-waxnae/C30hopanes and C24 tetracyclic terpanes /C26 tricyclic terpanes responded only to thermal influence by mantle-derived fluids. They did not chemically reacted with the mantle-derived fluids. Fluorene series compounds reacted with hydrogen and / or carbon dioxide from the mantle. Mantle-derived fluids affected most maturity index. The huge thermal energy with mantle-devied fluids weakened the relationship between the maturity parameters and depth. Among them, pregnane/C27-29 steroid and Ts/(Ts+Tm) were more sensitive to the heat of the fluids. ααα20S/(20S+20R) took the second place. αββ/(ααα+αββ) and 22S/(22S+22R) were not thermally influenced by the mantle-derived fluid. Besides, the substance of mantle-derived fluids reacted with fragrants, hopanes or moretanoids and thus altered the values of MPI1, MPI2, MPR, C30 hopanes/(C30 hopanes + moretanoids) and alkyl-diben zothiophene/diben zothiophene. The thermal alernation of phenanthrene series and their spatial distribution show that the heat energy carried by mantle-derived fluids was not fierce but spread widely in Dongying Sag, which is favorable to hydrocarbon generation with little destroy. In sum, mantle-derived fluids affected biomarkers through thermal energy and chemical reactions and changed the values of oil-source correlation and maturity parameters in the deep-seated fault belts. Therefore, in the deep-seated fault belts, oil-source correlation should be restudied and the new parameters need to be explored.

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本文通过对墨西哥湾Bush Hill 的5个冷泉碳酸盐岩样品和Alaminos Canyon 的1个冷泉碳酸盐岩样品的总有机质含量、可溶有机质含量、饱和烃、芳烃、脂肪酸、δ13C组成分布特征和部分地球化学参数的研究,探讨了冷泉碳酸盐岩中有机质来源、成熟度和沉积环境。 Bush Hill的冷泉碳酸盐岩样品的总有机碳为0.78-9.02%,可溶有机质含量5.77-65.06mg/g。总有机碳达9.02%的GC-B样品高碳数正构烷烃奇偶优势明显,存在荧蒽、芘和苝系列化合物,表明该样品有陆源物质的输入,并明显受深部渗漏原油的影响,其中烷烃的δ13C为-27.64~-32.36‰,正构脂肪酸δ13C为-26.52~-39.99‰,与现代菌藻类及下伏油气藏的δ13C值(-27~-31‰)相似,表明样品中的有机质主体可能来源于深部油气藏。其余4个Bush Hill冷泉碳酸盐岩样品和1个Alaminos Canyon冷泉碳酸盐岩样品正构烷烃的低碳优势明显,而奇偶优势不明显,低碳数分布的环己烷和长链烷基苯,以及三芳甾烷和甲基三芳甾烷的存在,推断这些样品的母质以菌藻类来源为主。 所有分析样品的甾烷成熟度参数C29ββ/(ββ+αα)为0.28-0.40,C2920S/(20S + 20R)为0.42-0.61、及C20-C21三芳孕甾烷TA(Ⅰ)/C26-C28三芳甾烷TA(Ⅱ)为0.49都说明样品的有机质成熟度较低,。 AC深水区AC-E样品UCM隆起不明显,Bush Hill浅水区样品(GC-B、GC-D、GC-F、GC-G,GC-H)UCM隆起均十分明显,这种隆起的形成是因为正烷烃、甚至五环三萜烷遭受生物降解。被微生物降解的正构烷烃与未被降解的环烷烃和支链烷烃等形成不能被溶解的复杂混合物(UCM)。因此,UCM隆起通常被认为是有机质遭受生物降解最直接的证据。深水区AC-E和Bush Hill浅水区GC-F样品中芴、氧芴和硫芴之间的丰度关系为硫芴﹥芴﹥氧芴,表明其为弱氧化-弱还原的沉积环境。具有较负碳同位素组成(-63.95‰ ~ -50.48‰)的异构/反异构脂肪酸是硫酸盐还原细菌的典型生物标志化合物,进一步证实冷泉碳酸盐岩的形成与甲烷缺氧氧化作用有关。 关键词:墨西哥湾 冷泉碳酸盐岩 有机质组成分布 单体烃碳同位素 沉积环境