Analysis of the Ordering Effects in Anthraquinone Thin Films and Its Potential Application for Sodium Ion Batteries

Abstract

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.

Anthraquinone and its derivatives as sustainable materials for electrochemical applications – a joint experimental and theoretical investigation of the redox potential in solution

“…24 Among the various types of organic materials, small molecular compounds are considered as highly promising candidates. In particular, quinone-based derivatives, such as anthraquinones (AQ), [25][26][27] are intensely studied for their potential application as a cathode material in metal-ion batteries. 28 This is inter alia a consequence of their capability to accommodate a two-electron reduction, resulting in a high energy storage capability in combination with fast charging/discharging rates.…”

Direct Electrochemical CO2 Capture Using Substituted Anthraquinones in Homogeneous Solutions: A Joint Experimental and Theoretical Study

“…As quinones in electrochemical applications are often limited due to reductive dissolution from the electrode surface, 44 metal-ion battery research is focused on the prevention of this dissolving process via polymerization or tuning of the substrate-quinone binding strength. 40 , 45 …”

“…Besides the use of quinones for electrochemical CO 2 capture, also numerous applications of quinones for metal-ion batteries − as well as redox-flow batteries − are reported. As quinones in electrochemical applications are often limited due to reductive dissolution from the electrode surface, metal-ion battery research is focused on the prevention of this dissolving process via polymerization or tuning of the substrate-quinone binding strength. , …”

Substrate Dependent Charge Transfer Kinetics at the Solid/Liquid Interface of Carbon‐Based Electrodes with Potential Application for Organic Na‐Ion Batteries

“…[27] Carbon materials derived from biomass are widely applied in bioelectrochemical systems, [28][29][30] biosensing applications, [31] and ITO electrode replacement. [32] Additionally, their high electrical conductivity and overall stability during cycling, makes carbon based materials suitable for rechargeable electrochemical power sources, such as batteries, including stationary and large-scale systems, [10,33,34] supercapacitors, [35,36] Na-ion batteries, [37][38][39] and Na-ion capacitors. [40] For all these applications, an efficient charge transfer at the materials interfaces (solid/solid or solid/liquid) is crucial and found to be ideal for applications in combination with organic semiconductors (OSCs).…”