A model system approach to understanding heteroatom-doped graphene electrocatalysts

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Research Question:Heteroatom-doped graphene are emerging as a new class of electrocatalysts which show great promise as earth-abundant replacements for the current state-of-the-art.The current bottleneck for development of these catalysts is a poor understanding of their structure, surface chemistry and catalytic mechanisms. Part of this is due to their structural complexity, the conventional doping process (adding in a precursor gas which contains the heteroatoms during growth of the graphene) results in randomly distributed heteroatoms which can sit in several inequivalent chemical environments. This disorder makes it very difficult to understand the relative activities of chemically different dopant atoms and the roles of dopant density and dopant-dopant interactions. Approach:In this project we will explore different methodologies to produce highly-ordered, high quality heteroatom-doped graphene and then characterise the resultant graphene on the atomic scale using a combination of Scanning Tunnelling Microscopy and X-Ray Photoelectron Spectroscopy (see references for a similar study on 2D oxide materials). This information will then be correlated to electrochemical testing to gain a new level of mechanistic understanding of these promising catalytic materials.Novelty:Model system approach: By producing a well-defined model system via CVD grown graphene we intend to be able to directly correlate electrochemical activity to specific surface species. This is a novel approach which could be broadly applicable to other electrocatalysts and energy materials.