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题名: 雄黄酒中砷形态特征、生物有效性及其人体尿砷代谢产物研究
作者: 张英男
学位类别: 博士
答辩日期: 2010
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 朱永官
关键词: realgar wine, arsenic, speciation, bioaccessibility, simulated gastrointestinal system, urine ; 雄黄酒,砷,形态学,生物有效性,模拟胃肠道系统,尿
其他题名: Study on Speciation and Bio-accessibility of Arsenic in Realgar Wine and Its Urinary Metabolites
中文摘要:       雄黄为硫化物类矿物雄黄的矿石,又名黄金石、石黄等。其应用最早见于我国首部药学专著《神农本草经》。该书中记载:“黄金石,辛温,主寒热,鼠瘘,恶疮,疽痔,死肌,杀白虫毒。” 中国古代主要把雄黄用在房屋物品的驱虫防虫上。近代人们开始用雄黄做印泥、制蚊香、做烟火等。欧美国家把雄黄添加在油漆中粉刷海船,可以防止贝壳附着船身。而雄黄用于皮革行业,则能很好地给皮草除虫防蛀。每年的农历五月初五,是中国的传统节日端午节,在这天,人们除了包粽子、赛龙舟,另外一项主要的活动是喝雄黄酒、涂抹雄黄酒,其目的是为了辟邪、驱毒。 雄黄的主要化学成分是As4S4或As2S2,另外还含有少量三氧化二砷(As2O3)及五氧化二砷(As2O5)。近年来,雄黄在临床应用过程中出现的毒副作用已越来越受到广泛重视。雄黄单味药的毒性作用主要包括致突变作用、细胞毒性作用、肝肾毒性作用等。对于雄黄在体内发挥药效的作用物质基础,究竟是少量的可溶性砷,还是难溶性的硫化砷,还是进人体内后的代谢产物,目前尚不清楚。而且,可溶性砷有三价砷(AsIII)和五价砷(AsV)两种价态,具有显著不同的生物学效应。 本文主要以常见市场饮用酒及雄黄粉为原料,分析雄黄酒的砷含量及形态,并探讨雄黄酒经饮用、涂抹进入人体后的形态变化及代谢转归,就其对人体机能所造成的潜在影响作出评估。 1)从药店中购入雄黄粉,6种饮用酒分别为市场购得及家庭自酿,酒精度数自12%至60%不等。将雄黄粉(0.025、0.05、0.25、0.5、2.5 g)与饮用酒5ml混合得到不同浓度的雄黄酒(0.005、0.01、0.05、0.1、0.5 g ml-1)。其中可溶性砷含量随雄黄浓度增长亦呈明显线性增长,同时,对含量与时间的相关性分析显示,随放置时间的延长,可溶性砷含量也增加。雄黄酒中可溶性砷主要有三价砷和五价砷,未检出有机砷。砷含量与酒精浓度也显著相关,随酒精浓度的增加,砷含量明显降低,这种降低主要源于五价砷的溶出减少。此外,随雄黄浓度增加,砷浓度亦呈线性增加,未发现有饱和现象。 2)雄黄酒中砷的生物有效性分析。引入模拟胃肠道系统,将室温静置48h的不同浓度雄黄酒按比例假如胃相和肠相,结果显示砷含量在肠相中最高可达823.8 mg L-1(0.5 g ml-1,醇雕),与之相应,在胃相中的含量为644.4 mg L-1,而在未经过模拟胃的雄黄酒中,含量则只有247.6 mg L-1。提示胃肠道环境能够显著提高雄黄酒中砷的溶出度。成年人单次饮用100ml雄黄酒(0.5 g ml-1,醇雕),其砷的摄入量将达到49.4-74.1 mg,以成人平均体重70kg计,砷的摄入量数百倍超出世界卫生组织规定的每日最大摄入量(2 g kg-1)。 3)口服雄黄酒的尿砷形态变化。将雄黄粉与家酿米酒混合制成雄黄酒,由来自湖南永州某村的10名成年男性志愿者口服,分段收集尿样并进行尿砷形态分析。在喝下雄黄酒16小时后,尿液总砷含量可达555.6 g L-1,88小时候,依然可达109.9 g L-1,近3倍于对照值。在形态上,尿样背景对照中,总砷中的无机砷(AsIII+AsV)和有机砷(DMA+MMA)分别占2.3% 和 85.4%。饮酒16小时候,无机砷比例迅速增加到47.7%,而有机砷虽然含量也增加,但所占比例锐减至49.9%。随着时间延长,无机砷所占比例逐渐减小,而有机砷比例则持续增加,在40小时之后在尿样中比例达到86.8%,占据主导地位。另外在受试者尿样中有少量砷甜菜碱(AsB)检出,AsB的存在主要与鱼类饮食有关。 4)将雄黄粉与家酿米酒混合制成雄黄酒,由来自湖南永州某村的6名儿童涂抹于前额,分段收集尿样并进行尿砷形态分析。尿样对照中砷含量为19.6 g L-1,无机砷与有机砷比例分别为13.2%和82.1%。在涂抹雄黄酒40小时后,尿砷总量达到峰值(85.3 g L-1),其后缓慢下降,但直到88小时后,依然有68.2 g L-1,近3倍于背景对照。无机砷与AsB的含量无显著变化,而有机砷(DMA+MMA)含量则在40小时后达到峰值。皮肤对砷的吸收与其形态有重要关系,AsIII经皮吸收的速度要比AsV快29倍。进入体内后,大部分砷发生甲基化形成有机砷,随尿液排出。皮肤是砷发生毒性的一个重要器官,砷可以与巯基结合,从而造成砷在皮肤中的沉积与缓慢渗透。 总之,雄黄酒的消费,尤其是大量饮用及涂抹,可导致尿液中的砷含量剧增。这项中国传统节日中的传统活动对人体的健康具有显著的潜在威胁。
英文摘要:       Consumption of realgar wine is a traditional activity during the classic Chinese festival of Duanwu, colloquially known worldwide as Dragon Boat Festival. Made by blending alcohol and realgar, realgar wine is drunk in the morning of the fifth day of the fifth lunar calendar month to commemorate the death of Chu Yuan, a famed Chinese official who drowned himself in protest of a corrupt government, and to protect against ill fortune. Realgar, also named golden rock, was initially reffered in “The Shennong Herb-Root Classic”. It is an popular traditional Chinese medicine. People believe that drinking it and painting it on body can exorcise evil spirits and abolish poison. Although realgar minerals are characteristically composed of sparingly soluble tetra-arsenic tetra-sulfides (As4S4) purity does vary with up to 10% of the As being present as non-sulphur bound, more toxic species, such as arsenate (AsV) and arsenite (AsIII). Despite, the renewed interest of late regarding As speciation and the bioassessibility of the active As components in realgar based Chinese medicines, little is known about the safety surrounding the cultural practice of drinking As wine. In a series of experiments the speciation and solubility of As in a range of wines was investigated. Furthermore, a simulated gastrointestinal system was employed to predict the impact of digestive processes on As bioavailability. The predominant soluble As species found in all the wines were AsIII and AsV. No organic or thio- species were detected. Based on typical As wine recipes employing 0.1 g realgar ml-1 wine the concentration of dissolved As ranged from ca. 100-400 mg L-1 depending on the ethanol content of the preparation: with the As solubility found to be higher in wines with a lower proportion of ethanol. Based on a common 100 ml measure of wine with a concentration of 400 mg As L-1, the amount of soluble As would equate to around half of the acute minimal lethal dose for adults. Although this is likely an underestimate of the bioassessible concentration, based upon the findings from the stimulated gastrointestinal system, which showed a ca. 3-fold increase in bioacessibility in the intestinal phase. Highly toxic arsenic in realgar wine can cause potential health risk to consumers by ingestion or percutaneous absorption. Urine samples of volunteers for drinking or painting were collected and As species were analysed. The total As reached the maximum of 220.2 g L-1 after 16 h of ingestion and 85.3 g L-1 after 40 h of painting. For drinking realgar wine, inorganic As was enhanced at 16 h, up to 47.7% of total urinary As. The inorganic level decreased sharply and DMA+MMA was the main As species, up to 74.2 and 86.8% at 28 and 40 h respectively. For painting of realgar wine on the forehead, the maximum As level (85.3g L-1) appeared after 40 h of painting, and DMA+MMA was always the major As species in urine during the 88-h monitoring period. Drinking or painting realgar wine increased urinary As dramatically and caused potential health risk to consumers, especially to children. This information on arsenic exposure of realgar wine is essential in a reliable assessment of the health risks to the public with the consumption of realgar wine by drinking or painting on the forehead, and perhaps also useful for sources of arsenic exposures.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35057
Appears in Collections:中澳联合土壤环境研究室_学位论文

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Recommended Citation:
张英男. 雄黄酒中砷形态特征、生物有效性及其人体尿砷代谢产物研究[D]. 北京. 中国科学院研究生院. 2010.
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