期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 1, 页码 250-259出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b17777
关键词
bioelectrocatalysis; carbon dioxide reduction; enzyme catalysis; graphene; enzyme immobilization; methanol
资金
- Austrian Climate and Energy Fund within the MELOS project [861392]
- Austrian Science Foundation (FWF) within the Wittgenstein Prize [Z222-N19]
- Operational Programme Research, Development and Education European Regional Development Fund of the Ministry of Education, Youth, and Sports of the Czech Republic [CZ.02.1.01/0.0/0.0/16_019/0000754]
- ERC Consolidator Grant (H2020) [683024]
- Czech Science Foundation (project GA CR-EXPRO) [19-27454X]
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.
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