4 years ago

High Performance Poly(viologen)–Graphene Nanocomposite Battery Materials with Puff Paste Architecture

High Performance Poly(viologen)–Graphene Nanocomposite Battery Materials with Puff Paste Architecture
Shamaila Sadaf, Arsalan Mado Mahmood, Lorenz Walder, Seyyed Mohsen Beladi-Mousavi
Four linear poly(viologens) (PV1, PV2: phenylic, PV3: benzylic, and PV4: aliphatic) in tight molecular contact with reduced graphene oxide (rGO), that is, PV@rGO, were prepared and used as anodic battery materials. These composites show exceptionally high, areal, volumetric, and current densities, for example, PV1@rGO composites (with 15 wt % rGO, corresponding to 137 mAh g–1) show 13.3 mAh cm–2 at 460 μm and 288 mAh cm–3 with 98% Coulombic efficiency at current densities up to 1000 A g–1, better than any reported organic materials. These remarkable performances are based on (i) molecular self-assembling of PVs on individual GO sheets yielding colloidal PV@GO and (ii) efficient GO/rGO transformation electrocatalyzed by PVs. Ion breathing during charging/discharging was studied by electrochemical quartz crystal microbalance and electrochemical atomic force microscopy revealing an absolute reversible and strongly anisotropic thickness oscillation of PV1@rGO at a right angle to the macroscopic current collector. It is proposed that such stress-free breathing is the key property for good cyclability of the battery material. The anisotropy is related to a puff paste architecture of rGO sheets parallel to the macroscopic current collector. A thin graphite sheet electrode with an areal capacity of 1.23 mAh cm–2 is stable over 200 bending cycles, making the material applicable for wearable electronics. The polymer acts as a lubricant between the rGO layers if shearing forces are active.

Publisher URL: http://dx.doi.org/10.1021/acsnano.7b02310

DOI: 10.1021/acsnano.7b02310

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