Abstract
AbstractOne‐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.
Highlights
The mechanism which led to the first genetic-machine, an adaptive chemical system that uses a genetic code to organise metabolic function and propagate that code, is one of the most important outstanding questions in science.[1,2] Modern organisms are genetic machines that take part in open-ended information transfer using biopolymers such as RNA and DNA, which are ubiquitous to all known life forms
Two relevant examples are the preferential formation of ribose when borate minerals are added to the formose reaction,[21] a system known for the incredible complexity of its product distribution, and the clear selectivity towards the production of certain nucleobases when formamide condensation is carried out on different mineral surfaces.[22]
We carried out the formose reaction in formamide with different mineral environments, see Figure 1, to assess whether the selectivity imparted by the environment can be amplified through recursion, whilst truncating the combinatorial explosion by reducing the overall number of products
Summary
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 generate complexity. 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, 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.
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