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29 November 2017

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ATP Synthesis and Biosensing Coupled to the Electroenzymatic Activity of a Hydrogenase on an Electrode/Biomimetic Membrane Interface †

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1
Instituto de Catálisis y Petroleoquímica, CSIC, Marie Curie 2, 28049 Madrid, Spain
2
Universidad Complutense de Madrid, Avda. Complutense, 28040 Madrid, Spain
3
Instituto de Tecnologia Quimica e Biologica, Universidade Nova de Lisboa Apartado 127, 2781-901 Oeiras, Portugal
*
Author to whom correspondence should be addressed.
Cells generate energy by coupling a proton gradient across a phospholipid bilayer membrane with the activity of a cross-membrane ATP synthase enzyme. In an effort to mimic this process in an artificial environment, we show that ATP can be efficiently produced starting from molecular hydrogen as a fuel. The proton concentration in an electrode/phospholipid bilayer interface can be controlled and monitorised electrochemically by immobilizing the membrane-bound [NiFeSe]-hydrogenase from Desulfovibrio vulgaris Hildenborough [1]. The electro-enzymatic oxidation of H2 generated a proton gradient across the supported biomimetic membrane that can be coupled to the in vitro synthesis of ATP by reconstituting ATP-synthase from E. coli on the biomimetic system [2]. Such a system is also suitable for developing an electrochemical biosensor of ATP.

Acknowledgement

This research was funded by the Spanish MINECO (Project CTQ2012-32448 and CTQ2015-71290-R) and by the Fundacao para a Ciencia e a Tecnologia (project PTDC/BBB- EP/0934/2012 and UID/Multi/04551/2013). I.L.-M acknowledges the European Research Council (ERC), grant no. ERC-StG-2013-338133 titled “MITOCHON” and RyC-2013-12609 from the Spanish MINECO.

References

  1. Gutiérrez-Sanz, O.; Tapia, C.; Marques, M.C.; Zacarias, S.; Velez, M.; Pereira, I.A.C.; de Lacey, A.L. Induction of a Proton Gradient across a Gold-Supported Biomimetic Membrane by Electroenzymatic H2 Oxidation. Angew. Chem. Int. Ed. 2015, 54, 2684–2687. [Google Scholar] [CrossRef] [Scilit]
  2. Gutiérrez-Sanz, O.; Natale, P.; Marquez, I.; Marques, M.C.; Zacarias, S.; Pita, M.; Pereira, I.A.C.; Lopez-Montero, I.; de Lacey, A.L. H2-Fueled ATP Synthesis on an Electrode: Mimicking Cellular Respiration. Angew. Chem. Int. Ed. 2016, 55, 6216–6220. [Google Scholar] [CrossRef] [Scilit]

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