Multielectron Redox-Bipolar Tetranitroporphyrin Macrocycle Cathode for High-Performance Zinc-Organic Batteries.

Angew Chem Int Ed Engl

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 200092 Shanghai, P. R. China.

Published: April 2024


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Article Abstract

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.202401049DOI Listing

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Multielectron Redox-Bipolar Tetranitroporphyrin Macrocycle Cathode for High-Performance Zinc-Organic Batteries.

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.

Article Synopsis
  • - The study introduces a new bipolar organic compound, tetranitroporphyrin (TNP), that enhances zinc-organic batteries (ZOBs) by using a multielectron redox system with both n-type and p-type properties for improved energy capacity.
  • - TNP facilitates efficient charge storage through dual mechanisms: it uses nitro groups to interact with zinc ions at low potential and amine groups with sulfate ions at higher potential, leading to significant increases in battery capacity and voltage.
  • - The TNP-based battery exhibits impressive performance metrics, including a high energy density of 365 Wh/kg and excellent longevity, maintaining 71.6% capacity after 50,000 cycles, marking a notable advancement in the development
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