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Self-assembling biomolecular catalysts for hydrogen production

Nature Chemistry volume 8, pages 179–185 (2016)Cite this article

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Abstract

The chemistry of highly evolved protein-based compartments has inspired the design of new catalytically active materials that self-assemble from biological components. A frontier of this biodesign is the potential to contribute new catalytic systems for the production of sustainable fuels, such as hydrogen. Here, we show the encapsulation and protection of an active hydrogen-producing and oxygen-tolerant [NiFe]-hydrogenase, sequestered within the capsid of the bacteriophage P22 through directed self-assembly. We co-opted Escherichia coli for biomolecular synthesis and assembly of this nanomaterial by expressing and maturing the EcHyd-1 hydrogenase prior to expression of the P22 coat protein, which subsequently self assembles. By probing the infrared spectroscopic signatures and catalytic activity of the engineered material, we demonstrate that the capsid provides stability and protection to the hydrogenase cargo. These results illustrate how combining biological function with directed supramolecular self-assembly can be used to create new materials for sustainable catalysis.

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Figure 1: Expression schematic showing a cartoon representation of EcHyd-1 with both subunits (hyaA and hyaB) fused to a scaffold protein encapsulated within the P22 capsid.
Figure 2: Expression and characterization of P22-Hydopt and P22-Hyd.
Figure 3: Expression and characterization of two other P22 hydrogenase constructs.
Figure 4: The P22 capsid provides protection from protease, thermal denaturation and air exposure with subsequent reactivation to its hydrogenase cargo.
Figure 5: FTIR spectra of P22-Hydopt and free, purified hydrogenase.

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Acknowledgements

This research was supported by a grant from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (DE-FG02-08ER46537). The authors acknowledge the gift of EcHyd-1 antibodies from F. Sargent (University of Dundee).

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Authors and Affiliations

  1. Department of Chemistry, Indiana University, Bloomington, 47407-7102, Indiana, USA

    Paul C. Jordan, Ethan J. Edwards, Megan C. Thielges & Trevor Douglas

  2. Department of Chemistry and Biochemistry, Montana State University, Bozeman, 59717, Montana, USA

    Paul C. Jordan, Kendall N. Saboda & Ethan J. Edwards

  3. Department of Chemistry & Biochemistry, University of Texas at Tyler, Tyler, 75799, Texas, USA

    Dustin P. Patterson

  4. Department of Microbiology & Immunology, Montana State University, Bozeman, 59717, Montana, USA

    Heini M. Miettinen

  5. Department of Biophysics, Bose Institute, Kolkata, 700054, India

    Gautam Basu

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Contributions

P.C.J., D.P.P. and T.D. conceived the concept. P.J. designed and carried out the experiments. K.N.S. assisted in characterization. E.J.E. assisted with TEM and ICP-MS. H.M.M. assisted in molecular biology. M.C.T. supervised the spectroscopy. P.J. and T.D. wrote the manuscript. T.D. directed the research. All authors discussed the results.

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Correspondence to Trevor Douglas.

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Jordan, P., Patterson, D., Saboda, K. et al. Self-assembling biomolecular catalysts for hydrogen production. Nature Chem 8, 179–185 (2016). https://doi.org/10.1038/nchem.2416

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