Analysis of the Ordering Effects in Anthraquinone Thin Films
and Its Potential Application for Sodium Ion Batteries
The ordering effects in anthraquinone (AQ) stacking forced by thin-film application and its
influence on dimer solubility and current collector adhesion are investigated. The structural
characteristics of AQ and its chemical environment are found to have a substantial influence on
its electrochemical performance. Computational investigation for different charged states of AQ
on a carbon substrate obtained via basin hopping global minimization provides important insights
into the physicochemical thin-film properties. The results reveal the ideal stacking configurations
of the individual AQ-carrier systems and show ordering effects in a periodic supercell environment.
The latter reveals the transition from intermolecular hydrogen bonding toward the formation of
salt bridges between the reduced AQ units and a stabilizing effect upon the dimerlike rearrangement,
while the strong surface–molecular interactions in the thin-film geometries are found to be crucial
for the formed dimers to remain electronically active. Both characteristics, the improved current
collector adhesion and the stabilization due to dimerization, are mutual benefits of thin-film electrodes
over powder-based systems. This hypothesis has been further investigated for its potential application
in sodium ion batteries. Our results show that AQ thin-film electrodes exhibit significantly better
specific capacities (233 vs 87 mAh g–1 in the first cycle), Coulombic efficiencies, and long-term
cycling performance (80 vs 4 mAh g–1 after 100 cycles) over the AQ powder electrodes.
By augmenting the experimental findings via computational investigations, we are able to suggest design
strategies that may foster the performance of industrially desirable powder-based electrode materials.
J. Phys. Chem. C 125, 3745 (2021)
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