Current approaches for the scalable production of holey graphene require graphene oxide (GO) or reduced graphene oxide (rGO) as starting materials. The molecular basis fundamentally determines that the holey graphene materials thus generated still contain a large number of defects on their basal planes, which not only complicate fundamental studies but also influence certain practical applications due to greatly decreased conductivity and chemical stability. This work reports a novel scalable approach exploiting dry microwave heating of slightly oxidized graphite intercalation compounds in air. The unique heating mechanism enables fabrication of holey graphene nanoplatelets with their basal planes nearly intact. Interestingly, it also begets holes with edges that are rich in zigzag geometry. The near-pristine nature of their basal planes and the zigzag edges were clearly observed <i>via</i> atomic resolution TEM and further supported by the studies of localized π-edge states associated with zigzag geometry <i>via</i> electron paramagnetic resonance (EPR) measurements. The holey graphene nanoplatelets were explored as metal free catalysts for hydrogen atom transfer reactions. High catalytic activity and desired selectivity were demonstrated. In addition, they provide excellent chemical stability for recyclability, which was not achievable by previously described holey graphene derivatives with basal plane defects. For the first time, the chemical catalytic activity of localized π-edge states was experimentally demonstrated unambiguously due to the absence of other defects in basal planes of these unique holey graphene nanoplatelets.

Microwave-enabled scalable fabrication of holey graphene nanoplatelets and their catalysis in reductive hydrogen atom transfer reactions

256th National Meeting (2018)

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