نبذة مختصرة : 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. ; Funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 715087) is gratefully acknowledged. ICMAB-CSIC members are grateful for funding through PTI+ TRANSENER+: “Alta Tecnología clave en la transición en el ciclo energético”, part of the CSIC program for the Spanish Recovery, Transformation and Resilience Plan funded by the Recovery and Resilience Facility of the European Union, established by the Regulation (EU) 2020/2094 and thank the Spanish Agencia Estatal de Investigación Severo Ochoa Programme for Centres of Excellence in R&D (CEX2019-000917-S). ; With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S). ; Peer reviewed
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