4.8 Article

Revisiting the Structure and Electrochemical Performance of Poly(o-phenylenediamine) as an Organic Cathode Material

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 24, 页码 27968-27978

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c06208

关键词

organic cathode material; rechargeable lithium battery; poly(o-phenylenediamine); phenazine; diaminophenazine

资金

  1. National Natural Science Foundation of China [21975189, 22179102]
  2. Recruitment Program of Global Experts
  3. Fundamental Research Funds for the Central Universities [2042017kf0028]
  4. Wuhan University

向作者/读者索取更多资源

Poly(o-phenylenediamine) has been identified as a promising cathode material for lithium batteries, with PoPDA-H synthesized at high temperature showing better performance and potential for practical application in energy storage devices.
Poly(o-phenylenediamine) (PoPDA) has been recognized as a low-cost electroactive organic material and studied as a cathode for aqueous zinc batteries or as an anode for nonaqueous lithium batteries. However, there remains a lot of confusion about its synthesis, structure, and electrochemical application. Especially, the previously studied PoPDA samples were mostly synthesized at room temperature, which were proved by us to be just a dimer, that is, 2,3-diaminophenazine (DAPZ). By various characterization methods including elemental analysis and mass spectrometry, we verified that the product synthesized at high temperature, PoPDA-H, was a polymer based on DAPZ as the structural repeat unit and with some imperfect substitutes (OH and NH3+CH3COO-). Based on the reversible redox reaction of phenazine units and the stable polymer structure within 1.3-3.8 V vs Li+/Li, PoPDA-H was more appropriate to be applied as a cathode rather than as an anode for lithium batteries. It achieved a high energy density of 490 Wh kg(-1) (2.12 V x 231 mAh g(-1)) at 50 mA g(-1) and a high cycling stability (79%@1000th cycle) at 500 mA g(-1), both of which were comparable to previously reported expensive pyrazine- and carbonyl-based polymers. This work clarifies many misunderstandings of PoPDA, which is important to its further development toward practical application in energy-storage devices.

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