Taming the Combinatorial Explosion of the Formose Reaction via Recursion within Mineral Environments
Taming the Combinatorial Explosion of the Formose Reaction via Recursion within Mineral Environments
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DOI：
10.1002/syst.201900014
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发表时间：
2019-09-01
期刊：
影响因子：
--
通讯作者：
Cronin, Leroy
中科院分区：
文献类型：
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作者：
Colon-Santos, Stephanie;Cooper, Geoffrey J. T.;Cronin, Leroy
简单前体的一锅反应，如在甲醛反应或甲酰胺缩合中发现的那些，不断导致组合爆炸，其中存在能够发挥作用的简单构件，但浓度不足以自组织，适应，从而产生复杂性。我们着手探索递归对这种复杂的混合物的影响，通过“播种”的产品混合物到一个新的版本的反应，包括不同的矿物环境，在一些反应周期。通过对混合物的非靶向UPLC-HRMS分析，我们发现检测到的产物总数随着循环次数的增加而减少，这是递归增强的矿物环境选择性的结果，从而限制了组合爆炸。这一发现表明，矿物表面与简单反应的关系如何导致RNA、核糖和尿嘧啶中发现的一些构建模块的出现，而这些构建模块的出现条件比最初认为的要简单得多。
One-pot reactions of simple precursors, such as those found in the formose reaction or formamide condensation, continuously lead to combinatorial explosions in which simple building blocks capable of function exist, but are in insufficient concentration to self-organize, adapt, and thus generate complexity. We set out to explore the effect of recursion on such complex mixtures by `seeding' the product mixture into a fresh version of the reaction, with the inclusion of different mineral environments, over a number of reaction cycles. Through untargeted UPLC-HRMS analysis of the mixtures we found that the overall number of products detected reduces as the number of cycles increases, as a result of recursively enhanced mineral environment selectivity, thus limiting the combinatorial explosion. This discovery demonstrates how the involvement of mineral surfaces with simple reactions could lead to the emergence of some building blocks found in RNA, ribose and uracil, under much simpler conditions that originally thought.