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Bipolar organics fuse the merits of n/p-type redox reactions for better Zn-organic batteries (ZOBs), but face the capacity plafond due to low density of active units and single-electron reactions. Here we report multielectron redox-bipolar tetranitroporphyrin (TNP) with quadruple two-electron-accepting n-type nitro motifs and dual-electron-donating p-type amine moieties towards high-capacity-voltage ZOBs. TNP cathode initiates high-kinetics, hybrid anion-cation 10e charge storage involving four nitro sites coordinating with Zn ions at low potential and two amine species coupling with SO ions at high potential. Consequently, Zn||TNP battery harvests high capacity (338 mAh g), boosted average voltage (1.08 V), and outstanding energy density (365 Wh kg ). Moreover, the extended π-conjugated TNP macrocycle achieves anti-dissolution in electrolytes, prolonging the battery life to 50,000 cycles at 10 A g with 71.6 % capacity retention. This work expands the chemical landscape of multielectron redox-bipolar organics for state-of-the-art ZOBs.
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http://dx.doi.org/10.1002/anie.202401049 | DOI Listing |
Angew Chem Int Ed Engl
April 2024
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 200092 Shanghai, P. R. China.