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In the search for novel polymeric molecules that could be used as electroactive materials, seven novel polyenaminones were prepared in high yields by the transaminative polymerization of resorcinol-derived bis-enaminones with m- and p-phenylenediamine and with 2,5-diaminohydroquinone. The obtained polymers show very low solubility in organic solvents and absorb UV light and visible light at wavelengths below 500 nm. All the obtained polymeric products were tested for redox activity in a Li battery setup. The 2,5-diaminohydroquinone-derived compound showed the best redox activity, with a maximum capacity of 86 mAh/g and relatively good capacity retention, thus confirming the hydroquinone group as the primary redox-active group. Other potential redox-active groups, such as resorcinol and conjugated carbonyls, showed limited activity, while variations in the phenylene groups and the substitution of phenolic groups in the resorcinol residue did not impact the electrochemical activity of the polymers. Their electrochemical properties, together with their previously established chemical recyclability, make polyenaminones promising scaffolds for the development of materials for sustainable energy storage applications. [ABSTRACT FROM AUTHOR]

One of the possible solutions to circumvent the sluggish kinetics, low capacity, and poor integrity of inorganic cathodes commonly used in rechargeable aluminium batteries (RABs) is the use of redox-active polymers as cathodes. They are not only sustainable materials characterised by their structure tunability, but also exhibit a unique ion coordination redox mechanism that makes them versatile ion hosts suitable for voluminous aluminium cation complexes, as demonstrated by the poly(quinoyl) family. Recently, phenazine-based compounds have been found to have high capacity, reversibility and fast redox kinetics in aqueous electrolytes because of the presence of a C＝N double bond. Here, we present one of the first examples of a phenazine-based hybrid microporous polymer, referred to as IEP-27-SR, utilized as an organic cathode in an aluminium battery with an AlCl3/EMIMCl ionic liquid electrolyte. The preliminary redox and charge storage mechanism of IEP-27-SR was confirmed by ex situ ATR-IR and EDS analyses. The introduction of phenazine active units in a robust microporous framework resulted in a remarkable rate capability (specific capacity of 116 mA h g−1 at 0.5C with 77% capacity retention at 10C) and notable cycling stability, maintaining 75% of its initial capacity after 3440 charge–discharge cycles at 1C (127 days of continuous cycling). This superior performance compared to reported Al//n-type organic cathode RABs is attributed to the stable 3D porous microstructure and the presence of micro/mesoporosity in IEP-27-SR, which facilitates electrolyte permeability and improves kinetics. [ABSTRACT FROM AUTHOR]

Enhancing the performance of electrolytes stands as one of the key challenges for moving toward practical applications of Mg batteries. Within this work, we investigate different synthesis procedures for the state-of-the-art MgAlhfip electrolyte. The results show that the purity and electrochemical performance of MgAlhfip electrolytes depend on whether they are synthesized from organometallic or inorganic reagents. Additionally, electrolyte properties vary depending on the electrolyte preparation method, either in situ electrolyte formation or salt isolation. To improve electrolyte performance, we explore two approaches: additional salt isolation steps and the use of a scavenging additive. Salt precipitation results in a modest improvement in the coulombic efficiency of Mg plating/stripping, while a scavenging additive significantly reduces overpotentials and enhances coulombic efficiency, especially in electrolytes synthesized from inorganic reagents. Finally, investigated syntheses are evaluated in terms of their practical applicability through procedure complexity and costs of used chemicals. Based on this, we propose a synthesis procedure that strikes a balance between the electrochemical performance of Mg electrolyte and its costs. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs) are crystalline porous organic polymers that have recently emerged as promising electrode materials for rechargeable batteries. Herein, we present an approach to improve the electrochemical performance of an anthraquinone-based COF (DAAQ-TFP-COF) cathode material in metal anode (Li, Mg) based batteries through proper selection of the electrolyte and binder. Our results show that the combination of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in tetraethylene glycol dimethyl ether (TEGDME) as electrolyte and poly(tetrafluoroethylene) (PTFE) as binder led to the best electrochemical performance with high utilisation efficiency of the redox sites and specific capacities close to the theoretical value. Using such electrolyte and binder, cyclable symmetric cells consisting of two DAAQ-TFP-COF organic electrodes exemplify 79% capacity retention after 2000 cycles at a high current density of 500 mA h g−1. The high reversibility and stability of the COF electrode material upon cycling were confirmed by ex situ IR spectroscopy. In addition, DAAQ-TFP-COF was explored as a cathode in magnesium cells using two different Mg electrolytes; one based on MgCl2 and one containing weakly coordinating anions. Electrochemical characterisation reveals significant differences in the performance of COF in terms of achievable capacities and voltage profiles, pointing towards hindered transport. Our findings demonstrate that the appropriate choice of electrolyte and binder is crucial to maximise the performance of COF-based materials in different post-lithium-ion metal anode batteries. [ABSTRACT FROM AUTHOR]

Multivalent batteries are often hyped as a next‐generation high‐energy density battery technology, but in reality, both literature reports and practical research are plagued by poor reproducibility of electrochemical results. Within the present work, we take a look at the electrochemical testing of organic cathodes that can be used with a variety of mono‐ and multivalent cations and propose a cyclable symmetric cell approach, already applied to the field of lithium‐ion batteries. By using a model organic system based on poly(anthraquinonyl sulfide) (PAQS) active material, we demonstrate that the symmetric cell approach elegantly removes the limitations of multivalent metal anodes, and for the first time, reveals the full potential of organic cathodes in multivalent batteries. Furthermore, symmetric cells enable reliable EIS measurements on organic cathodes and open a pathway to optimize electrochemical/transport parameters through the design of next‐generation organic cathode materials and advanced electrode design(s). We suggest that the cyclable symmetric cell approach should be generally applicable in multivalent and all other batteries where electrochemical characterization requires the elimination of the counter electrode contribution. [ABSTRACT FROM AUTHOR]