Journal
ADVANCED ENERGY MATERIALS
Volume 9, Issue 25, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201900029
Keywords
photobiocatalysis; photoelectrochemical cells; photovoltaics; solar CO2 reduction; titanium nitride
Categories
Funding
- National Research Foundation (NRF) via the Basic Science Research Program, Republic of Korea [NRF-2017R1A2B3011676]
- National Research Foundation (NRF) via Creative Materials Discovery Program, Republic of Korea [2017M3D1A1039558]
- National Research Foundation (NRF) via Creative Research Initiative Center, Republic of Korea [NRF-2015 R1A3A2066191]
- National Research Foundation of Korea [2017M3D1A1039558, 2017M3D1A1039556] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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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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