A1 Vertaisarvioitu alkuperäisartikkeli tieteellisessä lehdessä
Continuous 3D Titanium Nitride Nanoshell Structure for Solar-Driven Unbiased Biocatalytic CO2 Reduction
Tekijät: Kuk SK, Ham Y, Gopinath K, Boonmongkolras P, Lee Y, Lee YW, Kondaveeti S, Ahn CG, Shin B, Lee JK, Jeon S, Park CB
Kustantaja: WILEY-V C H VERLAG GMBH
Julkaisuvuosi: 2019
Lehti: Advanced Energy Materials
Tietokannassa oleva lehden nimi: ADVANCED ENERGY MATERIALS
Lehden akronyymi: ADV ENERGY MATER
Artikkelin numero: ARTN 1900029
Vuosikerta: 9
Numero: 25
Sivujen määrä: 10
ISSN: 1614-6832
DOI: https://doi.org/10.1002/aenm.201900029
Tiivistelmä
Z-scheme-inspired tandem photoelectrochemical (PEC) cells have received attention as a sustainable platform for solar-driven CO2 reduction. Here, continuously 3D-structured, electrically conductive titanium nitride nanoshells (3D TiN) for biocatalytic CO2-to-formate conversion in a bias-free tandem PEC system are reported. The 3D TiN exhibits a periodically porous network with high porosity (92.1%) and conductivity (6.72 x 10(4) S m(-1)), which allows for high enzyme loading and direct electron transfer (DET) to the immobilized enzyme. It is found that the W-containing formate dehydrogenase from Clostridium ljungdahlii (ClFDH) on the 3D TiN nanoshell is electrically activated through DET for CO2 reduction. At a low overpotential of 40 mV, the 3D TiN-ClFDH stably converts CO2 to formate at a rate of 0.34 mu mol h(-1) cm(-2) and a faradaic efficiency (FE) of 93.5%. Compared to a flat TiN-ClFDH, the 3D TiN-ClFDH shows a 58 times higher formate production rate (1.74 mu mol h(-1) cm(-2)) at 240 mV of overpotential. Lastly, a bias-free biocatalytic tandem PEC cell that converted CO2 to formate at an average rate of 0.78 mu mol h(-1) and an FE of 77.3% only using solar energy and water is successfully assembled.
Z-scheme-inspired tandem photoelectrochemical (PEC) cells have received attention as a sustainable platform for solar-driven CO2 reduction. Here, continuously 3D-structured, electrically conductive titanium nitride nanoshells (3D TiN) for biocatalytic CO2-to-formate conversion in a bias-free tandem PEC system are reported. The 3D TiN exhibits a periodically porous network with high porosity (92.1%) and conductivity (6.72 x 10(4) S m(-1)), which allows for high enzyme loading and direct electron transfer (DET) to the immobilized enzyme. It is found that the W-containing formate dehydrogenase from Clostridium ljungdahlii (ClFDH) on the 3D TiN nanoshell is electrically activated through DET for CO2 reduction. At a low overpotential of 40 mV, the 3D TiN-ClFDH stably converts CO2 to formate at a rate of 0.34 mu mol h(-1) cm(-2) and a faradaic efficiency (FE) of 93.5%. Compared to a flat TiN-ClFDH, the 3D TiN-ClFDH shows a 58 times higher formate production rate (1.74 mu mol h(-1) cm(-2)) at 240 mV of overpotential. Lastly, a bias-free biocatalytic tandem PEC cell that converted CO2 to formate at an average rate of 0.78 mu mol h(-1) and an FE of 77.3% only using solar energy and water is successfully assembled.
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