4.8 Article

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

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 296, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120349

Keywords

Tantalum nitride; Artificial photosynthesis; Graphitic carbon nitride; NADH regeneration; Formate dehydrogenase

Funding

  1. Research Council of Norway (RCN) project CO2BiOPEC [250261]
  2. Norwegian NMR
  3. Norwegian NMR Platform, NNP [226244/F50]
  4. European Research Council (ERC) under the European Union [856446]
  5. RCN project PH2ON [288320]
  6. European Research Council (ERC) [856446] Funding Source: European Research Council (ERC)

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This study achieved stable and efficient reduction of CO2 to formate in a bio-hybrid PEC cell using a novel cathode and efficient regeneration mechanism, approaching the efficiency of natural photosynthesis.
Mimicking natural photosynthesis by direct photoelectrochemical (PEC) reduction of CO2 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-C3N4 films. We demonstrate stable (20 h) aerobic PEC CO2-to-formate reduction at close to 100 % faradaic efficiency and unit selectivity in a bio-hybrid PEC cell of minimal engineering with optimized Ta3N5 nanotube photoanode powered by simulated sunlight with a solar to fuel efficiency of 0.063 %, approaching that of natural photosynthesis.

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