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Impact of Carbon Nanotube Surface Chemistry on Hydrogen Oxidation by Membrane‐Bound Oxygen‐Tolerant Hydrogenases
Author(s) -
Monsalve Karen,
Mazurenko Ievgen,
GutierrezSanchez Cristina,
Ilbert Marianne,
Infossi Pascale,
Frielingsdorf Stefan,
GiudiciOrticoni Marie Thérèse,
Lenz Oliver,
Lojou Elisabeth
Publication year - 2016
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.201600460
Subject(s) - hydrogenase , chemistry , carbon fibers , carbon nanotube , chemical engineering , hydrogen , platinum , oxygen , aquifex aeolicus , catalysis , nanotechnology , materials science , organic chemistry , biochemistry , escherichia coli , composite number , engineering , composite material , gene
Oxygen‐tolerant [NiFe] hydrogenases are attractive biocatalysts for utilization in H 2 /O 2 fuel cells, which thereby reduces the amount of platinum‐based catalysts. The O 2 ‐tolerant membrane‐bound hydrogenases isolated from Ralstonia eutropha and Aquifex aeolicus were previously studied at planar electrodes. The design of a powerful enzymatic fuel cell, however, requires a considerable increase in enzyme loading. Herein, we immobilized the two hydrogenases on carbon nanotubes, and we demonstrated that the enzyme binding and electron‐transfer properties on the 3D networks relied on the same surface chemistry as that of the planar electrodes. We evaluated how the intrinsic properties of each hydrogenase, that is, temperature and O 2 tolerance, were affected by immobilization on different electrode surfaces. The role of the detergent used for protein purification was especially emphasized. We also demonstrated that O 2 reduction products affected more seriously the enzyme activity than molecular O 2 . If immobilized on pyrene‐modified carbon nanotubes, both enzymes were used for the first time in a mild‐temperature, membraneless H 2 /O 2 enzymatic fuel cell, fed with O 2 ‐rich gas mixture, opening new avenues toward the development of alternative energy supplies.