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ACS Appl Mater Interfaces. 2020 Jan 8;12(1):250-259. doi: 10.1021/acsami.9b17777. Epub 2019 Dec 30.

Immobilized Enzymes on Graphene as Nanobiocatalyst.

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Linz Institute for Organic Solar Cells (LIOS), Institute of Physical Chemistry , Johannes Kepler University Linz , Altenberger Straße 69 , Linz , 4040 , Austria.
Regional Centre for Advanced Technologies and Materials, Department of Physical Chemistry Faculty of Science , Palacký University Olomouc , Listopadu 1192/12 , Olomouc , 771 46 , Czech Republic.


Using enzymes as bioelectrocatalysts is an important step toward the next level of biotechnology for energy production. In such biocatalysts, a sacrificial cofactor as an electron and proton source is needed. This is a great obstacle for upscaling, due to cofactor instability and product separation issues, which increase the costs. Here, we report a cofactor-free electroreduction of CO2 to a high energy density chemical (methanol) catalyzed by enzyme-graphene hybrids. The biocatalyst consists of dehydrogenases covalently bound on a well-defined carboxyl graphene derivative, serving the role of a conductive nanoplatform. This nanobiocatalyst achieves reduction of CO2 to methanol at high current densities, which remain unchanged for at least 20 h of operation, without production of other soluble byproducts. It is thus shown that critical improvements on the stability and rate of methanol production at a high Faradaic efficiency of 12% are possible, due to the effective electrochemical process from the electrode to the enzymes via the graphene platform.


bioelectrocatalysis; carbon dioxide reduction; enzyme catalysis; enzyme immobilization; graphene; methanol

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