Bioelectrochemistry at the Graphene Edge

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The edge of graphene has long attracted special attention due to its distinct physical and chemical properties in contrast to the graphitic basal plane. Electrochemistry at an isolated graphene edge (GrEdge) electrode has been systematically studied recently. We have shown that we can achieve high mass transport rates for electroactive species at the one-dimensional edge, which has enabled the observation of fast electron transfer kinetics at the GrEdge, free of diffusion limitations. Moreover, the possibility to modify the edge selectively, using nanoparticles or organic moieties, opens avenues for engineering the GrEdge both for fundamental studies involving reaction mechanisms as well as for applications in sensing and electrocatalysis. The GrEdge can be used as a one-dimensional mesoscopic probe to access immobilized entities and investigate electron transfer at the nanoscale. In this project, we take the next step in this direction and propose to wire enzymes specifically to the graphene edge and thereby probe the fundamental aspects of electron transfer with the immobilized proteins. In addition to evaluating different methodologies for selective attachment of the proteins to the edge, we will use operando spectroscopic methods, which we have developed recently, to obtain mechanistic details about the bioelectrochemistry of enzymes attached to the carbon edge. The results expected from this project will have strong implications for enzymatic biosensing and for bioelectrocatalysis at nanoscale electrodes.