期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 33, 页码 11253-11256出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201902287
关键词
artificial life; chemical recursion; depsipeptides; evolution; polymers
资金
- EPSRC [EP/P00153X/1, EP/J015156/1, EP/K021966/1, EP/K038885/1, EP/L015668/1, EP/L023652/1]
- BBSRC [BB/M011267/1]
- ERC [670467 SMART-POM]
- EU H2020 MADONNA [766975]
- John Templeton Foundation [60625, 61184]
- BBSRC [BB/M011267/1] Funding Source: UKRI
- EPSRC [EP/P00153X/1, EP/J015156/1, EP/L023652/1, EP/S019472/1, EP/L015668/1, EP/K038885/1, EP/K021966/1] Funding Source: UKRI
Living systems are characterised by an ability to sustain chemical reaction networks far-from-equilibrium. It is likely that life first arose through a process of continual disruption of equilibrium states in recursive reaction networks, driven by periodic environmental changes. Herein, we report the emergence of proto-enzymatic function from recursive polymerisation reactions using amino acids and glycolic acid. Reactions were kept out of equilibrium by diluting products 9:1 in fresh starting solution at the end of each recursive cycle, and the development of complex high molecular weight species is explored using a new metric, the Mass Index, which allows the complexity of the system to be explored as a function of cycle. This process was carried out on a range of different mineral environments. We explored the hypothesis that disrupting equilibrium via recursive cycling imposes a selection pressure and subsequent boundary conditions on products. After just four reaction cycles, product mixtures from recursive reactions exhibit greater catalytic activity and truncation of product space towards higher-molecular-weight species compared to non-recursive controls.
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