Environmental conditions drive self-organization of reaction pathways in a prebiotic reaction network

被引:48
作者
Robinson, William E. [1 ]
Daines, Elena [1 ]
van Duppen, Peer [1 ]
de Jong, Thijs [1 ]
Huck, Wilhelm T. S. [1 ]
机构
[1] Radboud Univ Nijmegen, Inst Mol & Mat, Nijmegen, Netherlands
关键词
CATALYZED FORMALDEHYDE CONDENSATION; FORMOSE REACTION; GLYCERALDEHYDE; KINETICS; GAS; MONOSACCHARIDES; GLYCOLALDEHYDE; IDENTIFICATION; AUTOCATALYSIS; ISOMERIZATION;
D O I
10.1038/s41557-022-00956-7
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The evolution of life from the prebiotic environment required a gradual process of chemical evolution towards greater molecular complexity. Elaborate prebiotically relevant synthetic routes to the building blocks of life have been established. However, it is still unclear how functional chemical systems evolved with direction using only the interaction between inherent molecular chemical reactivity and the abiotic environment. Here we demonstrate how complex systems of chemical reactions exhibit well-defined self-organization in response to varying environmental conditions. This self-organization allows the compositional complexity of the reaction products to be controlled as a function of factors such as feedstock and catalyst availability. We observe how Breslow's cycle contributes to the reaction composition by feeding C-2 building blocks into the network, alongside reaction pathways dominated by formaldehyde-driven chain growth. The emergence of organized systems of chemical reactions in response to changes in the environment offers a potential mechanism for a chemical evolution process that bridges the gap between prebiotic chemical building blocks and the origin of life.
引用
收藏
页码:623 / +
页数:19
相关论文
共 59 条
[1]  
Andersen J. L., 2013, J SYS CHEM, V4, P4, DOI [DOI 10.1186/1759-2208-4-4, 10.1186/1759-2208-4-4]
[2]  
Andersen JL, 2018, MATCH-COMMUN MATH CO, V80, P661
[3]   Discovery and Enumeration of Organic-Chemical and Biomimetic Reaction Cycles within the Network of Chemistry [J].
Bajczyk, Michal D. ;
Dittwald, Piotr ;
Wolos, Agnieszka ;
Szymkuc, Sara ;
Grzybowski, Bartosz A. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2018, 57 (09) :2367-2371
[4]   Ethoximation-silylation approach for mono- and disaccharide analysis and characterization of their identification parameters by GC/MS [J].
Becker, M. ;
Liebner, F. ;
Rosenau, T. ;
Potthast, A. .
TALANTA, 2013, 115 :642-651
[5]   Evaluation of different derivatisation approaches for gas chromatographic-mass spectrometric analysis of carbohydrates in complex matrices of biological and synthetic origin [J].
Becker, M. ;
Zweckmair, T. ;
Forneck, A. ;
Rosenau, T. ;
Potthast, A. ;
Liebner, F. .
JOURNAL OF CHROMATOGRAPHY A, 2013, 1281 :115-126
[6]   Unified prebiotically plausible synthesis of pyrimidine and purine RNA ribonucleotides [J].
Becker, Sidney ;
Feldmann, Jonas ;
Wiedemann, Stefan ;
Okamura, Hidenori ;
Schneider, Christina ;
Iwan, Katharina ;
Crisp, Antony ;
Rossa, Martin ;
Amatov, Tynchtyk ;
Carell, Thomas .
SCIENCE, 2019, 366 (6461) :76-+
[7]   THE KINETICS OF HEXOSE FORMATION FROM TRIOSES IN ALKALINE SOLUTION [J].
BERL, WG ;
FEAZEL, CE .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (05) :2054-2057
[8]  
BRESLOW R, 1959, TETRAHEDRON LETT, P22
[9]   Taming the Combinatorial Explosion of the Formose Reaction via Recursion within Mineral Environments [J].
Colon-Santos, Stephanie ;
Cooper, Geoffrey J. T. ;
Cronin, Leroy .
CHEMSYSTEMSCHEM, 2019, 1 (03)
[10]   Catalytic condensation of glycolaldehyde and glyceraldehyde with formaldehyde in neutral and weakly alkaline aqueous media: Kinetics and mechanism [J].
Delidovich, I. V. ;
Simonov, A. N. ;
Pestunova, O. P. ;
Parmon, V. N. .
KINETICS AND CATALYSIS, 2009, 50 (02) :297-303