Bioelectrocatalytic formate oxidation and carbon dioxide reduction at high current density and low overpotential with tungsten-containing formate dehydrogenase and mediators |
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| Institution: | 1. VTT Technical Research Centre of Finland Ltd, Espoo 02150, Finland;2. Department of Civil and Environmental Engineering, Stanford University, Stanford, CA 94305, USA;3. Tri-Institutional Training Program in Computational Biology and Medicine, Memorial Sloan Kettering Cancer Center, New York, NY 10065, USA;4. Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA;1. Department of Chemistry, Faculty of Science, National University of Singapore, Singapore 117543, Singapore;2. NUS Environmental Research Institute, National University of Singapore, Singapore 117411, Singapore;1. Clean Energy Research Center, Korea Institute of Science and Technology, Hwarangno 14-gil 5, Seongbuk-gu, Seoul 136-791, Republic of Korea;2. Department of Chemical Engineering, Hongik University, 72-1 Sangsu-dong, Mapo-gu, Seoul 121-791, Republic of Korea;3. Department of Bio & Nano Chemistry, College of Natural Sciences, Kookmin University, 861-1, jeongneung-dong, Sungbuk-gu, Seoul 137-702, Republic of Korea;3. From the Departments of Chemical and Environmental Engineering,;5. Biochemistry, and;4. Bioengineering Engineering and;6. Materials Science and Engineering Program, University of California, Riverside, California 92521;1. Clean Energy Research Centre, Korea Institute of Science and Technology, P.O. Box 131, Cheongryyang, Seoul 136 791, Republic of Korea;2. Department of Microbial Engineering, Konkuk University, 120 Neungdong-ro, Gwangjin-gu, Seoul 143-701, Republic of Korea;3. Department of Bio & Nano Chemistry, College of Natural Science, Kookmin University, 861-1, Jeongneung-dong, Sungbuk-gu, Seoul 137-702, Republic of Korea |
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| Abstract: | We show a great possibility of mediated enzymatic bioelectrocatalysis in the formate oxidation and the carbon dioxide (CO2) reduction at high current densities and low overpotentials. Tungsten-containing formate dehydrogenase (FoDH1) from Methylobacterium extorquens AM1 was used as a catalyst and immobilized on a Ketjen Black-modified electrode. For the formate oxidation, a high limiting current density (jlim) of ca. 24 mA cm− 2 was realized with a half wave potential (E1/2) of only 0.12 V more positive than the formal potential of the formate/CO2 couple (E°′CO2) at 30 °C in the presence of methyl viologen (MV2 +) as a mediator, and jlim reached ca. 145 mA cm− 2 at 60 °C. Even when a viologen-functionalized polymer was co-immobilized with FoDH1 on the porous electrode, jlim of ca. 30 mA cm− 2 was attained at 60 °C with E1/2 = E°′CO2 + 0.13 V. On the other hand, the CO2 reduction was also realized with jlim ≈ 15 mA cm− 2 and E1/2 = E°′CO2 − 0.04 V at pH 6.6 and 60 °C in the presence of MV2 +. |
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