School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, Shandong 264209, China.
State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.
J Phys Chem Lett. 2022 Jan 20;13(2):567-573. doi: 10.1021/acs.jpclett.1c03486. Epub 2022 Jan 11.
Phosphorylation for ribonucleotide formation is a critical step in the origin of life but has had limited success due to the thermodynamic and kinetic constraints in aqueous media. Here, we report that the production of ribonucleotides from ribonucleosides in the presence of monopotassium phosphate (KHPO) spontaneously proceeded in aqueous microdroplets under ambient conditions and without using a catalyst. A full set of ribonucleotides including adenosine monophosphate (AMP), guanosine monophosphate (GMP), uridine monophosphate (UMP), and cytidine monophosphate (CMP) were generated on the scale of a few milliseconds. The aqueous microdroplets could transfer the ribonucleotides to oligoribonucleotides and showed mutual compatibility for individual phosphorylation. Conditions established the dependence of the conversion ratio on the droplet size and suggested that the condensation reactions occurred at or near the microdroplets' surface. This aqueous microdroplet approach also provides a route for elucidating phosphorylation chemistry in the prebiotic era.
核苷酸的形成中的磷酸化是生命起源的关键步骤，但由于水相介质中的热力学和动力学限制，其一直没有取得太大的成功。在这里，我们报告了在单磷酸钾（KHPO）的存在下，核糖核苷在水微滴中，在环境条件下且无需使用催化剂的情况下，自发地进行，从而产生了核糖核苷酸。一整套的核糖核苷酸包括腺嘌呤单核苷酸（AMP）、鸟嘌呤单核苷酸（GMP）、尿嘧啶单核苷酸（UMP）和胞嘧啶单核苷酸（CMP）在几毫秒的时间内生成。水微滴可以将核糖核苷酸转移到寡核糖核苷酸上，并表现出对单个磷酸化的相互兼容性。所建立的条件表明，转化率取决于液滴的大小，并暗示缩合反应发生在微滴表面或附近。这种水微滴方法还为阐明前生物时代的磷酸化化学提供了一条途径。
