Facile Synthesis of Polyphenothiazine as a High-Performance p-Type Cathode for Rechargeable Lithium Batteries

ChemSusChem. 2021 Aug 9;14(15):3174-3181. doi: 10.1002/cssc.202101008. Epub 2021 Jun 23.

Abstract

p-Type electroactive polymers are promising cathodes for dual-ion batteries but cost-effective candidates are still lacking. In this study, the p-type polymer polyphenothiazine (PPTZ) is synthesized by a facile one-step oxidation polymerization from the low-cost phenothiazine (PTZ) monomer. As a cathode for rechargeable lithium batteries, PPTZ shows superior electrochemical performance to previously reported PTZ-based polymers with complicated structures and syntheses. For example, PPTZ has a high reversible capacity of 157 mAh g-1 within 2.5-4.3 V vs. Li+ /Li with an average discharge voltage of 3.5 V, and a high capacity retention of 77 % after 500 cycles. The highly reversible one-electron redox mechanism of PPTZ is also investigated in detail by electrochemical testing, ex situ FT-IR and X-ray photoelectron spectroscopy, and DFT calculations. PPTZ has the potential to serve as an attractive p-type cathode material for practical applications and the facile synthesis may be also extended to other polymer cathodes based on N-heteroaromatic units.

Keywords: N heterocycles; electrode materials; lithium; organic batteries; polymerization.