Shalayel Ibrahim, Coulibaly Seydou, Ly Kieu Dung, Milet Anne, Vallée Yannick
Univ. Grenoble Alpes, CNRS, Département de Chimie Moléculaire, Campus, F-38058 Grenoble, France.
Life (Basel). 2018 Oct 19;8(4):47. doi: 10.3390/life8040047.
The Strecker reaction of aldehydes with ammonia and hydrogen cyanide first leads to α-aminonitriles, which are then hydrolyzed to α-amino acids. However, before reacting with water, these aminonitriles can be trapped by aminothiols, such as cysteine or homocysteine, to give 5- or 6-membered ring heterocycles, which in turn are hydrolyzed to dipeptides. We propose that this two-step process enabled the formation of thiol-containing dipeptides in the primitive ocean. These small peptides are able to promote the formation of other peptide bonds and of heterocyclic molecules. Theoretical calculations support our experimental results. They predict that α-aminonitriles should be more reactive than other nitriles, and that imidazoles should be formed from transiently formed amidinonitriles. Overall, this set of reactions delineates a possible early stage of the development of organic chemistry, hence of life, on Earth dominated by nitriles and thiol-rich peptides (TRP).
醛与氨和氰化氢的斯特雷克反应首先生成α-氨基腈,然后α-氨基腈水解生成α-氨基酸。然而,在与水反应之前,这些氨基腈可以被氨基硫醇(如半胱氨酸或高半胱氨酸)捕获,生成5元或6元环杂环化合物,这些杂环化合物继而水解生成二肽。我们认为,这一两步过程能够在原始海洋中形成含硫醇的二肽。这些小肽能够促进其他肽键和杂环分子的形成。理论计算支持我们的实验结果。计算预测α-氨基腈应该比其他腈更具反应活性,并且咪唑应该由瞬时形成的脒基腈生成。总体而言,这一系列反应描绘了地球上海洋中以腈和富含硫醇的肽(TRP)为主导的有机化学乃至生命发展的一个可能的早期阶段。