Supramolecular design as a route to high-performing organic electrodes.

Organic electrodes may someday replace transition metals oxides, the current standard in electrochemical energy storage, including those with severe issues of availability, cost, and recyclability. To realize this more sustainable future, a thorough understanding of structure-property relationships and design rules for organic electrodes must be developed. Further, it is imperative that supramolecular interactions between organic species, which are often overlooked, be included in organic electrode design. In this review, we showcase how molecular and polymeric electrodes that host non-covalent interactions outperform materials without these features. Using select examples from the literature, we emphasize how dispersion forces, hydrogen-bonding, and radical pairing can be leveraged to improve the stability, capacity, and energy density of organic electrodes. Throughout this review, we identify potential next-generation designs and opportunities for continued investigation. We hope that this review will serve as a catalyst for collaboration between synthetic chemists and the energy storage community, which we view as a prerequisite to achieving high-performing supramolecular electrode materials.

Cooperative crosslinking in polyvinyl alcohol organogels.

Manipulating and optimizing the properties of gels is important for practical applications but can be both synthetically difficult and expensive. In this work, we report an easily tunable polyvinyl alcohol (PVA) organogel formed with boric acid (BA) and 1,4-benzenediboronic acid (1,4-BDBA) as crosslinkers. While PVA and BA alone form weak aggregations in DMSO, adding small amounts of 1,4-BDBA dramatically improves the material properties and gelation. PVA organogels made with mixtures of BA and 1,4-BDBA have improved thermal properties, lower CGCs, and higher G' than those with either crosslinker alone. We propose that these enhanced material properties are the result of cooperative PVA crosslinking between 1,4-BDBA and BA. As the properties of this system can be improved by simply varying the ratio of crosslinkers, these organogels are highly adjustable and are a practical alternative to PVA hydrogels.