Taming the Combinatorial Explosion of the Formose Reaction via Recursion within Mineral Environments

Colón‐Santos, Stephanie; Cooper, Geoffrey J. T.; Cronin, Leroy

doi:10.1002/syst.201900014

Cited by 25 publications

(15 citation statements)

References 25 publications

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“…Abiotic samples were produced in a controlled synthesis without enzymes or other biological influence (besides the chemists that prepared them) and included dipeptides, and Miller–Urey spark discharge mixtures. We also investigated the incredibly messy sugar-based ‘formose’ reaction mixtures with and without mineral salts added 32 . Inorganic samples included extracts from terrestrial mineral sources such as quartz, limestone, sandstone, and granite.…”

Section: Resultsmentioning

confidence: 99%

Identifying molecules as biosignatures with assembly theory and mass spectrometry

et al. 2021

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The search for alien life is hard because we do not know what signatures are unique to life. We show why complex molecules found in high abundance are universal biosignatures and demonstrate the first intrinsic experimentally tractable measure of molecular complexity, called the molecular assembly index (MA). To do this we calculate the complexity of several million molecules and validate that their complexity can be experimentally determined by mass spectrometry. This approach allows us to identify molecular biosignatures from a set of diverse samples from around the world, outer space, and the laboratory, demonstrating it is possible to build a life detection experiment based on MA that could be deployed to extraterrestrial locations, and used as a complexity scale to quantify constraints needed to direct prebiotically plausible processes in the laboratory. Such an approach is vital for finding life elsewhere in the universe or creating de-novo life in the lab.

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Section: Resultsmentioning

confidence: 99%

Identifying molecules as biosignatures with assembly theory and mass spectrometry

et al. 2021

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“…Complex chemical mixtures with thousands, or tens of thousands, of different product species are often seen as an analytical problem, and the conventional approach of analyzing every single product species is not feasible. This is why researchers have attempted to develop a more system-level approach to detect changes and trends in spectra instead of attempting to identify isolated species 3 , 20 , 21 . The Mass Index is not able to capture the complexity of the data of a cycle completely, but rather simplifies the system.…”

Section: Resultsmentioning

confidence: 99%

“…The Mass Index is not able to capture the complexity of the data of a cycle completely, but rather simplifies the system. Previous recursive chemistry experiments already raised the problem of addressing every single feature of an experiment, but as the number of experimental cycles increases, the need to effective heuristics and metrics becomes even more significant 3 , 20 , 21 . The Mass Index value is a simple metric for each cycle, enabling a fast, algorithmically driven comparison and the adjustment of the experiment in real time based on these data.…”

Section: Resultsmentioning

confidence: 99%

A robotic prebiotic chemist probes long term reactions of complexifying mixtures

et al. 2021

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To experimentally test hypotheses about the emergence of living systems from abiotic chemistry, researchers need to be able to run intelligent, automated, and long-term experiments to explore chemical space. Here we report a robotic prebiotic chemist equipped with an automatic sensor system designed for long-term chemical experiments exploring unconstrained multicomponent reactions, which can run autonomously over long periods. The system collects mass spectrometry data from over 10 experiments, with 60 to 150 algorithmically controlled cycles per experiment, running continuously for over 4 weeks. We show that the robot can discover the production of high complexity molecules from simple precursors, as well as deal with the vast amount of data produced by a recursive and unconstrained experiment. This approach represents what we believe to be a necessary step towards the design of new types of Origin of Life experiments that allow testable hypotheses for the emergence of life from prebiotic chemistry.

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“…Classically, prebiotic chemists have focused on sugar syntheses involving the formose reaction (the polymerization of formaldehyde) − (Scheme a) or the Kiliani–Fischer-type homologation of hydrogen cyanide with cyanohydrin intermediates (Scheme b) . However, nature uses no such chemistry and leaves no trace that it ever did.…”

Section: Carbohydrate Metabolismmentioning

confidence: 99%

Nonenzymatic Metabolic Reactions and Life’s Origins

2020

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Prebiotic chemistry aims to explain how the biochemistry of life as we know it came to be. Most efforts in this area have focused on provisioning compounds of importance to life by multi-step synthetic routes that do not resemble biochemistry. However, gaining insight into why core metabolism uses the molecules, reactions, pathways, and overall organization that it does requires us to consider molecules not only as synthetic end goals. Equally important are the dynamic processes that build them up and break them down. This perspective has led many researchers to the hypothesis that the first stage of the origin of life began with the onset of a primitive non-enzymatic version of metabolism, initially catalyzed by naturally occurring minerals and metal ions. This view of life's origins has come to be known as "metabolism first". Continuity with modern metabolism would require a primitive version of metabolism to build and break down ketoacids, sugars, amino acids, and ribonucleotides in much the same way as the pathways that do it today. This review discusses metabolic pathways of relevance to the origin of life in a manner accessible to chemists, and summarizes experiments suggesting several pathways might have their roots in prebiotic chemistry. Finally, key remaining milestones for the protometabolic hypothesis are highlighted.

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Taming the Combinatorial Explosion of the Formose Reaction via Recursion within Mineral Environments

Cited by 25 publications

References 25 publications

Identifying molecules as biosignatures with assembly theory and mass spectrometry

Identifying molecules as biosignatures with assembly theory and mass spectrometry

A robotic prebiotic chemist probes long term reactions of complexifying mixtures

Nonenzymatic Metabolic Reactions and Life’s Origins

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