Keller M, Blöchl E, Wächtershäuser G, Stetter K O
Nature. 1994 Apr 28;368(6474):836-8. doi: 10.1038/368836a0.
Amide bonds are of central importance for biochemistry; in the guise of peptide bonds, they form the backbone of proteins. The formation of amide bonds without the assistance of enzymes poses a major challenge for theories of the origin of life. Enzyme-free formation of amide bonds between amino acids has been demonstrated in the presence of condensing agents such as cyanamide. Here we report the formation of amide bonds in aqueous solution in the absence of any condensing agent. We find that the formation of pyrite (FeS2) from FeS and H2S can provide the driving force for reductive acetylation of amino acids with mercaptoacetic acid (HSCH2COOH). The redox energy of pyrite formation permits the activation of the carboxylic acid group, which is converted to a species that reacts readily with amines. This process provides support for the chemo-autotrophic theory for the origin of life, in which pyrite formation supplies the energy source for the first autocatalytic reproduction cycle.
酰胺键对生物化学至关重要;以肽键的形式,它们构成了蛋白质的骨架。在没有酶辅助的情况下形成酰胺键对生命起源理论构成了重大挑战。在诸如氰胺等缩合剂存在的情况下,已证明氨基酸之间可无酶形成酰胺键。在此我们报告在不存在任何缩合剂的水溶液中形成酰胺键的情况。我们发现由FeS和H₂S形成黄铁矿(FeS₂)可为氨基酸与巯基乙酸(HSCH₂COOH)的还原乙酰化提供驱动力。黄铁矿形成的氧化还原能量允许羧酸基团活化,该基团转化为一种易于与胺反应的物质。这一过程为生命起源的化学自养理论提供了支持,在该理论中黄铁矿的形成提供了第一个自催化复制循环的能量来源。