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Design of multi-phase dynamic chemical networks

Nature Chemistry volume 9, pages 799–804 (2017)Cite this article

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Abstract

Template-directed polymerization reactions enable the accurate storage and processing of nature's biopolymer information. This mutualistic relationship of nucleic acids and proteins, a network known as life's central dogma, is now marvellously complex, and the progressive steps necessary for creating the initial sequence and chain-length-specific polymer templates are lost to time. Here we design and construct dynamic polymerization networks that exploit metastable prion cross-β phases. Mixed-phase environments have been used for constructing synthetic polymers, but these dynamic phases emerge naturally from the growing peptide oligomers and create environments suitable both to nucleate assembly and select for ordered templates. The resulting templates direct the amplification of a phase containing only chain-length-specific peptide-like oligomers. Such multi-phase biopolymer dynamics reveal pathways for the emergence, self-selection and amplification of chain-length- and possibly sequence-specific biopolymers.

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Figure 1: Dynamic peptide network analyses.
Figure 2: NF-CHO dynamic peptide network.
Figure 3: NFF-CHO dynamic peptide network.
Figure 4: Cross-seeding the NFF-CHO network.

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Acknowledgements

We are grateful to H. Yi and J. Taylor in the Emory Robert P. Apkarian Microscopy Core for TEM, the Emory Microscopy Core for fluorescence imaging, J. Bacsa in the Emory X-ray Crystallography Center for X-ray diffraction, F. Strobel in the Emory Mass Spectrometry Center for LC-MS, M. Zhou and F. Fernandez in the School of Chemistry and Biochemistry, Georgia Institute of Technology for IMS-MS, the NASA Astrobiology Program, under the NSF CCI, CHE-1004570 (CC, PT, MCH), the James S. McDonnell Foundation (J.T., M.C.H.), Emory University for supplies and personnel support, the US Department of Energy, Office of Science, Office of Basic Energy Sciences DE-FG02-02ER15377 for personnel support (C.C.) and equipment, and NSF CHE-1507932 for supplies, equipment, and structural characterization support.

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Authors and Affiliations

  1. Departments of Chemistry and Biology, Emory University, Atlanta, Georgia 30322, USA

    Chenrui Chen, Junjun Tan, Ting Pan, Jay T. Goodwin, Anil K. Mehta & David G. Lynn

  2. School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, USA

    Ming-Chien Hsieh & Martha A. Grover

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  1. Chenrui Chen
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C.C., J.T., M.C.H, T.P, A.K.M., J.T.G, M.A.G and D.G.L. designed experiments, analysed data and wrote the paper.

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Correspondence to David G. Lynn.

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Chen, C., Tan, J., Hsieh, MC. et al. Design of multi-phase dynamic chemical networks. Nature Chem 9, 799–804 (2017). https://doi.org/10.1038/nchem.2737

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