Monti Damien, Patil Nagaraj, Black Ashley P, Raptis Dionysios, Mavrandonakis Andreas, Froudakis George E, Yousef Ibraheem, Goujon Nicolas, Mecerreyes David, Marcilla Rebeca, Ponrouch Alexandre
Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Campus UAB, 08193 Bellaterra, Catalonia, Spain.
Electrochemical Processes Unit, IMDEA Energy, Avda. Ramón de La Sagra 3, 28935 Móstoles, Spain.
ACS Appl Energy Mater. 2023 Jun 27;6(13):7250-7257. doi: 10.1021/acsaem.3c00969. eCollection 2023 Jul 10.
Ca- and Mg-based batteries represent a more sustainable alternative to Li-ion batteries. However, multivalent cation technologies suffer from poor cation mass transport. In addition, the development of positive electrodes enabling reversible charge storage currently represents one of the major challenges. Organic positive electrodes, in addition to being the most sustainable and potentially low-cost candidates, compared with their inorganic counterparts, currently present the best electrochemical performances in Ca and Mg cells. Unfortunately, organic positive electrodes suffer from relatively low capacity retention upon cycling, the origin of which is not yet fully understood. Here, 1,4,5,8-naphthalenetetracarboxylic dianhydride-derived polyimide was tested in Li, Na, Mg, and Ca cells for the sake of comparison in terms of redox potential, gravimetric capacities, capacity retention, and rate capability. The redox mechanisms were also investigated by means of operando IR experiments, and a parameter affecting most figures of merit has been identified: the presence of contact ion-pairs in the electrolyte.
钙基和镁基电池是锂离子电池更具可持续性的替代品。然而，多价阳离子技术存在阳离子传质较差的问题。此外，开发能够实现可逆电荷存储的正极目前是主要挑战之一。有机正极除了是最具可持续性且可能成本较低的候选材料外，与无机正极相比，目前在钙和镁电池中展现出最佳的电化学性能。不幸的是，有机正极在循环过程中容量保持率相对较低，其原因尚未完全明确。在此，为了在氧化还原电位、重量容量、容量保持率和倍率性能方面进行比较，对1,4,5,8 - 萘四甲酸二酐衍生的聚酰亚胺在锂、钠、镁和钙电池中进行了测试。还通过原位红外实验研究了氧化还原机制，并确定了一个影响大多数品质因数的参数：电解质中接触离子对的存在。
