TY  - JOUR
A1  - Ruth, John C.
A1  - Schwarz, Fabian M.
A1  - Müller, Volker
A1  - Spormann, Alfred M.
T1  - Enzymatic hydrogen electrosynthesis at enhanced current density using a redox polymer
T2  - Catalysts
N2  - High-temperature tolerant enzymes offer multiple advantages over enzymes from mesophilic organisms for the industrial production of sustainable chemicals due to high specific activities and stabilities towards fluctuations in pH, heat, and organic solvents. The production of molecular hydrogen (H2) is of particular interest because of the multiple uses of hydrogen in energy and chemicals applications, and the ability of hydrogenase enzymes to reduce protons to H2 at a cathode. We examined the activity of Hydrogen-Dependent CO2 Reductase (HDCR) from the thermophilic bacterium Thermoanaerobacter kivui when immobilized in a redox polymer, cobaltocene-functionalized polyallylamine (Cc-PAA), on a cathode for enzyme-mediated H2 formation from electricity. The presence of Cc-PAA increased reductive current density 340-fold when used on an electrode with HDCR at 40 °C, reaching unprecedented current densities of up to 3 mA·cm−2 with minimal overpotential and high faradaic efficiency. In contrast to other hydrogenases, T. kivui HDCR showed substantial reversibility of CO-dependent inactivation, revealing an opportunity for usage in gas mixtures containing CO, such as syngas. This study highlights the important potential of combining redox polymers with novel enzymes from thermophiles for enhanced electrosynthesis.
KW  - hydrogen-dependent CO2 reductase
KW  - redox polymer
KW  - cobaltocene
KW  - enzymatic electrosynthesis
KW  - hydrogen evolution
KW  - carbon monoxide
Y1  - 2021
UR  - http://publikationen.ub.uni-frankfurt.de/frontdoor/index/index/docId/69251
UR  - https://nbn-resolving.org/urn:nbn:de:hebis:30:3-692512
SN  - 2073-4344
VL  - 11
IS  - 10, art. 1197
SP  - 1
EP  - 10
PB  - MDPI
CY  - Basel
ER  -