Published online by Cambridge University Press: 01 June 2020
Realization of the full potential of 2D nanosheet materials in energy storage and conversion devices requires heterogeneously structured electrodes having good electrical conductivity and large mean free paths for ion diffusion. Electrospinning of anisotropic objects usually obscures this anisotropy because of a large amount of carrier polymer typically required to form fibers. We demonstrate electrospinning of graphene with nearly quantitative retention of flake anisotropy to provide low to moderate density coatings of randomly oriented flakes having very large inter-flake mean free paths for ionic diffusion. Polyvinyl alcohol (PVA) is used as a carrier polymer and yields graphene anisotropy retention over an instability domain wherein electrospinning transitions to electrospraying. Graphene is deposited in polymer-encapsulated films at weight concentrations up to 50%, almost an order of magnitude higher than previously reported. Electrode applications will require at least partial replacement of PVA by electrically conducting polymers, and such polyelectrolytes should also suppress this electrospraying instability. We believe that large-scale electrospinning of graphene nanosheets will accelerate development of 2D materials in the fields of energy storage and conversion, catalysis, and tissue engineering.