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

Autor(en): Beladi-Mousavi, Seyyed Mohsen
Sadaf, Shamaila
Mahmood, Arsalan Mado
Walder, Lorenz 
Stichwörter: ACTIVE MATERIALS; AQUEOUS-ELECTROLYTE; battery; Chemistry; Chemistry, Multidisciplinary; Chemistry, Physical; composites; electrochemical AFM; ENERGY-STORAGE; eQCM; graphene; graphene oxide; LITHIUM-ION BATTERIES; Materials Science; Materials Science, Multidisciplinary; Nanoscience & Nanotechnology; ORGANIC ELECTRODE; POLYIMIDE ANODE; QUARTZ-CRYSTAL MICROBALANCE; RADICAL POLYMER-CATHODE; RECHARGEABLE DEVICE; Science & Technology - Other Topics; STORAGE MATERIAL; viologen
Erscheinungsdatum: 2017
Journal: ACS NANO
Volumen: 11
Ausgabe: 9
Startseite: 8730
Seitenende: 8740
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 pm 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 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.
ISSN: 19360851
DOI: 10.1021/acsnano.7b02310

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