Redox-active conjugated microporous polymers (RCMPs) polymerized by conventional methods are commonly obtained as irregular insoluble solid particles making the electrode processing difficult. In this work, the synthesis of RCMP based on anthraquinone moieties (IEP-11) is developed via a two-step pathway combining miniemulsion and solvothermal techniques that results in polymer nanostructures that are much easier to disperse in solvents facilitating the fabrication of electrodes. Interestingly, this synthetic approach is also found to have an important impact on the inherent morphology of IEP-11 that exhibits a dual porosity combining micro and mesopores with a specific surface area as high as 2200 m 2 g −1 , which is one of the highest values reported for RCMPs. Moreover, the compactness of the electrodes is also improved, the resulting electrodes have triple the density than those obtained with conventional methods. Consequently, when these electrodes are tested as cathodes in Li-ion battery, they deliver high gravimetric capacities (≈100 mAh g −1 ) and extraordinary rate capability keeping 76% of discharge capacity when charged-discharged in only 12 min (@5 C). Moreover, the insoluble and robust conjugated porous structure provides IEP-11-E12 with an unprecedented cycling stability retain ≈90% and ≈60% of its initial capacity after 5000 (@2 C) and 80 000 cycles (@30 C), respectively.

DFT calculations reveal interesting structure–property relationships of the redox potentials of phenazines in non-aqueous media.

Redox-active organic compounds have become promising electrode materials for the development of more sustainable, economical, and safer batteries. However, their high electrochemical performance is inherently associated with the use of low mass-loading electrodes with high carbon content, which collectively hinders their applicability in real batteries. This work presents an innovative approach for developing high-performance and practical organic electrodes through the synthesis of anthraquinone-based conjugated microporous polymers in the presence of carbon nanostructures and further processing into self-supported buckypaper electrodes. This effective method enables high-mass-loading hybrid electrodes (up to 60 mg cm–2) with low carbon content (20 wt %), which attained high gravimetric capacity (83.7 mAh gelectrode –1), high areal capacity (6.3 mAh cm–2), good rate capability (0.8 mAh cm–2 at 10C), and remarkable cycle stability (>80% capacity retention over 1000 cycles). These are the highest values reported for an organic electrode, constituting a great leap forward in the development of practical organic batteries.

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