A1 Vertaisarvioitu alkuperäisartikkeli tieteellisessä lehdessä
NADH-Free Electroenzymatic Reduction of CO2 by Conductive Hydrogel-Conjugated Formate Dehydrogenase
Tekijät: Kuk SK, Gopinath K, Singh RK, Kim TD, Lee Y, Choi WS, Lee JK, Park CB
Kustantaja: AMER CHEMICAL SOC
Julkaisuvuosi: 2019
Journal: ACS Catalysis
Tietokannassa oleva lehden nimi: ACS CATALYSIS
Lehden akronyymi: ACS CATAL
Vuosikerta: 9
Numero: 6
Aloitussivu: 5584
Lopetussivu: 5589
Sivujen määrä: 11
ISSN: 2155-5435
DOI: https://doi.org/10.1021/acscatal.9b00127
Tiivistelmä
The electrocatalytic reduction of CO2 under low overpotential and mild conditions using redox enzyme is a propitious route for carbon capture and conversion. Here, we report bioelectrocatalytic CO2 conversion to formate by conjugating a strongly CO2-reductive, W-containing formate dehydrogenase from Clostridium ljungdahlii (ClFDH) to conductive polyaniline (PANi) hydrogel. The ClFDH in the hybrid electrode successfully gained electrons directly from PANi and exhibited high capability for electroenzymatic conversion of CO2 to formate at low overpotential without NADH. We describe a potential electron-transfer pathway in the PANi-ClFDH bioelectrode on the basis of multiple spectroscopic analyses and a QM/MM-based computational study. The 3D-nanostructured PANi hydrogel facilitated rapid electron injection to the active site of ClFDH. In the absence of NADH, the PANi-CIFDH electrode showed stable CO2-to-formate transformation at an overpotential as low as 40 mV, with 1.42 mu mol h(-1) cm(-2) conversion rate, 92.7% faradaic efficiency, and 976 h(-1) turnover frequency.
The electrocatalytic reduction of CO2 under low overpotential and mild conditions using redox enzyme is a propitious route for carbon capture and conversion. Here, we report bioelectrocatalytic CO2 conversion to formate by conjugating a strongly CO2-reductive, W-containing formate dehydrogenase from Clostridium ljungdahlii (ClFDH) to conductive polyaniline (PANi) hydrogel. The ClFDH in the hybrid electrode successfully gained electrons directly from PANi and exhibited high capability for electroenzymatic conversion of CO2 to formate at low overpotential without NADH. We describe a potential electron-transfer pathway in the PANi-ClFDH bioelectrode on the basis of multiple spectroscopic analyses and a QM/MM-based computational study. The 3D-nanostructured PANi hydrogel facilitated rapid electron injection to the active site of ClFDH. In the absence of NADH, the PANi-CIFDH electrode showed stable CO2-to-formate transformation at an overpotential as low as 40 mV, with 1.42 mu mol h(-1) cm(-2) conversion rate, 92.7% faradaic efficiency, and 976 h(-1) turnover frequency.
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