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In situ cofactor regeneration enables selective CO2 reduction in a stable and efficient enzymatic photoelectrochemical cell.

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Title: In situ cofactor regeneration enables selective CO2 reduction in a stable and efficient enzymatic photoelectrochemical cell.
Authors: Xu, Kaiqi1 (AUTHOR), Chatzitakis, Athanasios1 (AUTHOR) a.e.chatzitakis@smn.uio.no, Backe, Paul Hoff2,3 (AUTHOR), Ruan, Qiushi4 (AUTHOR), Tang, Junwang1,4 (AUTHOR) junwang.tang@ucl.ac.uk, Rise, Frode5 (AUTHOR), Bjørås, Magnar2,6 (AUTHOR), Norby, Truls1 (AUTHOR) truls.norby@kjemi.uio.no
Source: Applied Catalysis B: Environment & Energy. Nov2021, Vol. 296, pN.PAG-N.PAG. 1p.
Subjects: Photoelectrochemical cells, Cofactors (Biochemistry), Carbon dioxide, Energy consumption, Radiolabeling, Nicotinamide, Cathodes
Abstract: [Display omitted] • Co-modified Ta 3 N 5 nanotubes reach a photocurrent of 9.4 mA/cm2 at 1.23 V. • g-C 3 N 4 can selectively electro-regenerate NAD+ to 1,4-NADH. • An enzymatic photoelectrochemical cell with a Ta 3 N 5 anode and g-C 3 N 4 cathode is constructed. • A solar-to-formate efficiency of 0.064 % is achieved. • C-13 isotope labelling proves the direct utilisation of CO 2 in the enzymatic cathode. Mimicking natural photosynthesis by direct photoelectrochemical (PEC) reduction of CO 2 to chemicals and fuels requires complex cell assemblies with limitations in selectivity, efficiency, cost, and stability. Here, we present a breakthrough cathode utilizing an oxygen tolerant formate dehydrogenase enzyme derived from clostridium carboxidivorans and coupled to a novel and efficient in situ nicotinamide adenine dinucleotide (NAD+/NADH) regeneration mechanism through interfacial electrochemistry on g-C 3 N 4 films. We demonstrate stable (20 h) aerobic PEC CO 2 -to-formate reduction at close to 100 % faradaic efficiency and unit selectivity in a bio-hybrid PEC cell of minimal engineering with optimized Ta 3 N 5 nanotube photoanode powered by simulated sunlight with a solar to fuel efficiency of 0.063 %, approaching that of natural photosynthesis. [ABSTRACT FROM AUTHOR]
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Abstract:[Display omitted] • Co-modified Ta 3 N 5 nanotubes reach a photocurrent of 9.4 mA/cm2 at 1.23 V. • g-C 3 N 4 can selectively electro-regenerate NAD+ to 1,4-NADH. • An enzymatic photoelectrochemical cell with a Ta 3 N 5 anode and g-C 3 N 4 cathode is constructed. • A solar-to-formate efficiency of 0.064 % is achieved. • C-13 isotope labelling proves the direct utilisation of CO 2 in the enzymatic cathode. Mimicking natural photosynthesis by direct photoelectrochemical (PEC) reduction of CO 2 to chemicals and fuels requires complex cell assemblies with limitations in selectivity, efficiency, cost, and stability. Here, we present a breakthrough cathode utilizing an oxygen tolerant formate dehydrogenase enzyme derived from clostridium carboxidivorans and coupled to a novel and efficient in situ nicotinamide adenine dinucleotide (NAD+/NADH) regeneration mechanism through interfacial electrochemistry on g-C 3 N 4 films. We demonstrate stable (20 h) aerobic PEC CO 2 -to-formate reduction at close to 100 % faradaic efficiency and unit selectivity in a bio-hybrid PEC cell of minimal engineering with optimized Ta 3 N 5 nanotube photoanode powered by simulated sunlight with a solar to fuel efficiency of 0.063 %, approaching that of natural photosynthesis. [ABSTRACT FROM AUTHOR]
ISSN:09263373
DOI:10.1016/j.apcatb.2021.120349