美国科学家的一项最新研究,解开了新鲜泥土的清香气味形成之谜。他们发现,微生物体内一种具有两种不同功能的蛋白酶在土味素(geosmin)的合成过程中起着关键的作用。该研究成果将对水净化产生重要影响,相关论文9月16日在线发表于《自然—化学生物学》上。
早在100多年前,科学家就发现了决定泥土气味的土味素。土壤中的土味素主要由细菌制造,除了能散发出令人愉悦的香味,土味素还会使水中产生刺激性的泥苦味。不过,到目前为止,科学家对土味素的生物合成机制知之甚少。
领导最新研究的是美国布朗大学的化学教授David Cane。几年前,他发现了天蓝链霉菌(Streptomyces coelicolor)与制造土味素有关的基因。去年,他的研究小组又发现了一种名为germacradienol/geosmin合成酶蛋白能将法尼基焦磷酸(farnesyl diphosphate)转化为土味素。
在最新的研究中,Cane小组发现,该蛋白会折叠成两个不同但相连的部分(类似于哑铃),其中一部分负责土味素合成反应的前半部分,产生的化学物质会传送到该蛋白的另一部分,从而合成出土味素。Cane表示,“土味素是由具有两种不同功能的酶制造出来的,该过程的两个步骤之间在代谢上是相关的。同时,这种酶也是与制造土味素等萜类物质相关、且具有双重功能的第一种酶。”
论文第一作者、布朗大学化学系的Jiaoyang Jiang表示,新的发现将帮助微生物学家找到新的途径,以避免水中产生不好的气味。“土味素在玻璃杯中并不好闻,”她说。(科学网 任霄鹏/编译)
原始出处:
Nature Chemical Biology
Published online: 16 September 2007 | doi:10.1038/nchembio.2007.29
Biosynthesis of the earthy odorant geosmin by a bifunctional Streptomyces coelicolor enzyme
Jiaoyang Jiang1, Xiaofei He1 & David E Cane1
Geosmin (1) is responsible for the characteristic odor of moist soil, as well as off-flavors in drinking water and foodstuffs1, 2. Geosmin is generated from farnesyl diphosphate (FPP, 2) by an enzyme that is encoded by the SCO6073 gene in the soil organism Streptomyces coelicolor A3(2) (ref. 3). We have now shown that the recombinant N-terminal half of this protein catalyzes the Mg2+-dependent cyclization of FPP to germacradienol (3) and germacrene D (4), while the highly homologous C-terminal domain, previously thought to be catalytically silent, catalyzes the Mg2+-dependent conversion of germacradienol to geosmin. Site-directed mutagenesis confirmed that the N- and C-terminal domains each harbor a distinct, independently functioning active site. A mutation in the N-terminal domain of germacradienol-geosmin synthase of a catalytically essential serine to alanine results in the conversion of FPP to a mixture of sesquiterpenes that includes an aberrant product identified as isolepidozene (6), which was previously suggested to be an enzyme-bound intermediate in the cyclization of FPP to germacradienol.
Department of Chemistry, Box H, Brown University, Providence, Rhode Island 02912-9108, USA.
Correspondence to: David E Cane1 Email: david_cane@brown.edu