한빛사 논문
Su Keun Kuk,†,⊥ Krishnasamy Gopinath,§,⊥ Raushan K. Singh,§ Tae-Doo Kim,§ Youngjun Lee,§ Woo Seok Choi,† Jung-Kul Lee,*,§ and Chan Beum Park*,†
†Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, 335 Science Road, Daejeon 305-701, Republic of Korea §Department of Chemical Engineering, Konkuk University, 120 Neungdong-ro, Seoul 05029, Republic of Korea
*Corresponding Authors
Author Contributions
⊥S.K.K. and K.G. contributed equally to this work.
Abstract
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-ClFDH electrode showed stable CO2-to-formate transformation at an overpotential as low as 40 mV, with 1.42 μmol h–1 cm–2 conversion rate, 92.7% faradaic efficiency, and 976 h–1 turnover frequency.
KEYWORDS:CO2 reduction, NADH-free biocatalysis, formate dehydrogenase, electrocatalysis, bioelectrode
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