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Generating system-level responses from a network of simple synthetic replicators

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Generating system-level responses from a network of simple synthetic replicators. / Sadownik, Jan W.; Kosikova, Tamara; Philp, Douglas.

In: Journal of the American Chemical Society, Vol. 139, No. 48, 06.12.2017, p. 17565-17573.

Research output: Contribution to journalArticlepeer-review

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Sadownik, JW, Kosikova, T & Philp, D 2017, 'Generating system-level responses from a network of simple synthetic replicators', Journal of the American Chemical Society, vol. 139, no. 48, pp. 17565-17573. https://doi.org/10.1021/jacs.7b09735

APA

Sadownik, J. W., Kosikova, T., & Philp, D. (2017). Generating system-level responses from a network of simple synthetic replicators. Journal of the American Chemical Society, 139(48), 17565-17573. https://doi.org/10.1021/jacs.7b09735

Vancouver

Sadownik JW, Kosikova T, Philp D. Generating system-level responses from a network of simple synthetic replicators. Journal of the American Chemical Society. 2017 Dec 6;139(48):17565-17573. https://doi.org/10.1021/jacs.7b09735

Author

Sadownik, Jan W. ; Kosikova, Tamara ; Philp, Douglas. / Generating system-level responses from a network of simple synthetic replicators. In: Journal of the American Chemical Society. 2017 ; Vol. 139, No. 48. pp. 17565-17573.

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@article{e0f34f1ba3f9459381cb0afa0af7c187,
title = "Generating system-level responses from a network of simple synthetic replicators",
abstract = "The creation of reaction networks capable of exhibiting responses that are properties of entire systems represents a significant challenge for the chemical sciences. The system- level behavior of a reaction network is linked intrinsically to its topology and the functional connections between its nodes. A simple network of chemical reactions constructed from four reagents, in which each reagent reacts with exactly two others, can exhibit up-regulation of two products even when only a single chemical reaction is addressed catalytically. We implement a system with this topology using two maleimides and two nitrones of different sizes—either short or long and each bearing complementary recognition sites—that react pairwise through 1,3-dipolar cycloaddition reactions to create a network of four length-segregated replicating templates. Comprehensive 1H NMR spectroscopy experiments unravel the network topology, confirming that, in isolation, three out of four templates self-replicate, with the shortest template exhibiting the highest efficiency. The strongest template effects within the network are the mutually cross-catalytic relationships between the two templates of intermediate size. The network topology is such that the addition of different preformed templates as instructions to a mixture of all starting materials elicits system-level behavior. Instruction with a single template up-regulates the formation of two templates in a predictable manner. These results demonstrate that the rules governing system-level behavior can be unraveled through the application of wholly synthetic networks with well-defined chemistries and interactions.",
author = "Sadownik, {Jan W.} and Tamara Kosikova and Douglas Philp",
note = "The financial support for this work was provided by EaStCHEM and the Engineering and Physical Sciences Research Council (Grant EP/K503162/1).",
year = "2017",
month = dec,
day = "6",
doi = "10.1021/jacs.7b09735",
language = "English",
volume = "139",
pages = "17565--17573",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "AMER CHEMICAL SOC",
number = "48",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Generating system-level responses from a network of simple synthetic replicators

AU - Sadownik, Jan W.

AU - Kosikova, Tamara

AU - Philp, Douglas

N1 - The financial support for this work was provided by EaStCHEM and the Engineering and Physical Sciences Research Council (Grant EP/K503162/1).

PY - 2017/12/6

Y1 - 2017/12/6

N2 - The creation of reaction networks capable of exhibiting responses that are properties of entire systems represents a significant challenge for the chemical sciences. The system- level behavior of a reaction network is linked intrinsically to its topology and the functional connections between its nodes. A simple network of chemical reactions constructed from four reagents, in which each reagent reacts with exactly two others, can exhibit up-regulation of two products even when only a single chemical reaction is addressed catalytically. We implement a system with this topology using two maleimides and two nitrones of different sizes—either short or long and each bearing complementary recognition sites—that react pairwise through 1,3-dipolar cycloaddition reactions to create a network of four length-segregated replicating templates. Comprehensive 1H NMR spectroscopy experiments unravel the network topology, confirming that, in isolation, three out of four templates self-replicate, with the shortest template exhibiting the highest efficiency. The strongest template effects within the network are the mutually cross-catalytic relationships between the two templates of intermediate size. The network topology is such that the addition of different preformed templates as instructions to a mixture of all starting materials elicits system-level behavior. Instruction with a single template up-regulates the formation of two templates in a predictable manner. These results demonstrate that the rules governing system-level behavior can be unraveled through the application of wholly synthetic networks with well-defined chemistries and interactions.

AB - The creation of reaction networks capable of exhibiting responses that are properties of entire systems represents a significant challenge for the chemical sciences. The system- level behavior of a reaction network is linked intrinsically to its topology and the functional connections between its nodes. A simple network of chemical reactions constructed from four reagents, in which each reagent reacts with exactly two others, can exhibit up-regulation of two products even when only a single chemical reaction is addressed catalytically. We implement a system with this topology using two maleimides and two nitrones of different sizes—either short or long and each bearing complementary recognition sites—that react pairwise through 1,3-dipolar cycloaddition reactions to create a network of four length-segregated replicating templates. Comprehensive 1H NMR spectroscopy experiments unravel the network topology, confirming that, in isolation, three out of four templates self-replicate, with the shortest template exhibiting the highest efficiency. The strongest template effects within the network are the mutually cross-catalytic relationships between the two templates of intermediate size. The network topology is such that the addition of different preformed templates as instructions to a mixture of all starting materials elicits system-level behavior. Instruction with a single template up-regulates the formation of two templates in a predictable manner. These results demonstrate that the rules governing system-level behavior can be unraveled through the application of wholly synthetic networks with well-defined chemistries and interactions.

U2 - 10.1021/jacs.7b09735

DO - 10.1021/jacs.7b09735

M3 - Article

VL - 139

SP - 17565

EP - 17573

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 48

ER -

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