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2. π-Conjugated redox-active two-dimensional polymers as organic cathode materials

   https://doi.org/10.1039/D1SC07157B  

   Jin, Zexin; Cheng, Qian; Evans, Austin M.; Gray, Jesse; Zhang, Ruiwen; Bao, Si Tong; Wei, Fengkai; Venkataraman, Latha; Yang, Yuan; Nuckolls, Colin (March 2022, Chemical Science)

   Redox-active two-dimensional polymers (RA-2DPs) are promising lithium battery organic cathode materials due to their regular porosities and high chemical stabilities. However, weak electrical conductivities inherent to the non-conjugated molecular motifs used thus far limit device performance and the practical relevance of these materials. We herein address this problem by developing a modular approach to construct π-conjugated RA-2DPs with a new polycyclic aromatic redox-active building block PDI-DA. Efficient imine-condensation between PDI-DA and two polyfunctional amine nodes followed by quantitative alkyl chain removal produced RA-2DPs TAPPy-PDI and TAPB-PDI as conjugated, porous, polycrystalline networks. In-plane conjugation and permanent porosity endow these materials with high electrical conductivity and high ion diffusion rates. As such, both RA-2DPs function as organic cathode materials with good rate performance and excellent cycling stability. Importantly, the improved design enables higher areal mass-loadings than were previously available, which drives a practical demonstration of TAPPy-PDI as the power source for a series of LED lights. Collectively, this investigation discloses viable synthetic methodologies and design principles for the realization of high-performance organic cathode materials. 

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   Bighin, G.; Burchianti, A.; Minardi, F.; Macrì, T. (August 2022, Physical Review A)
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   Schramm, Brandon; Gray, Montgomery; Herbert, John M (January 2025, Journal of the American Chemical Society)