Dual-Redox-Center Conjugated Microporous Polymers as Durable p-Type Cathode Enabling Hybrid Kinetics in Lithium Batteries.

Jiao, Wenyu; Chen, Yuze; Huang, Wanhong; Song, Xiaowei; Sun, Libo; Liang, Zhiqiang · Nano Lett · 2026

basic_science · Level V

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Abstract

p-Type organic cathodes offer high operating voltages but are often limited by poor cyclability. To overcome this, herein, we successfully integrate two p-type redox centers, triphenylamine and phenazine, into conjugated microporous polymers (CMPs), denoted as CMP-TBDA-Pz and CMP-TBA-Pz. These materials demonstrate high voltages (>3.5 V vs Li<sup>+</sup>/Li), superior capacity, and excellent stability. Notably, the dual-redox centers endow the system with hybrid charge storage kinetics, balancing diffusion-controlled and pseudocapacitive behavior. As a result, CMP-TBDA-Pz delivers specific capacities of 219.4 mAh g<sup>-1</sup> (0.1 A g<sup>-1</sup>) and 135.7 mAh g<sup>-1</sup> (5 A g<sup>-1</sup>), corresponding to energy densities of 633 and 417 Wh kg<sup>-1</sup>, respectively. In graphite//CMP-TBDA-Pz full-cells, 97% capacity retention is achieved after 500 cycles at 2 A g<sup>-1</sup>. This work establishes a strategy for high-performance p-type cathodes via dual-site architecture to regulate hybrid kinetics.