A low-cost and high-loading viologen-based organic electrode for rechargeable lithium batteries

Organic active materials are regarded as a very promising choice for lithium batteries because of several outstanding advantages such as low-cost, flexible tunability and pollution-free sources. Viologen compounds are attractive two-electron storage materials with low redox potentials, which are mainly used as anolytes in redox flow batteries (RFBs) considering their high solubility in electrolytes. However, due to their relatively large molecular weight and low density, it is difficult to prepare high-loading and stable-cycling electrodes for lithium battery application. In this research, by adopting 4,4'-bipyridine as the raw material and combining salification with a high-energy ball milling method, a low-solubility and high-stability viologen carbon-coated composite, ethyl viologen dihexafluorophosphate-Ketjen black (EV-KB), is synthesized. Then, by optimizing the electrode preparation process, a high-loading viologen-based electrode is successfully prepared. Salification effectively reduces the solubility of viologen compounds in the electrolyte so that the EV-KB composite can be used in lithium batteries. At the same time, it is pointed out that current collectors and slurry solvents play an important role in achieving the high-loading electrode. By deliberately selecting carbon paper as the current collector and ethanol as the solvent, the EV-KB composite organic electrode with a loading up to 1.5-9 mg cm^-2 can achieve a specific capacity of 106-79 mA h g^-1 for 400 stable cycles with a coulombic efficiency of 96% as well as a good rate capability. The synthesis method and electrode preparation optimization process introduced in this paper provide a reference for other types of organic active materials to be used in high-loading lithium batteries.