重新审视聚（邻苯二胺）作为有机正极材料的结构和电化学性能,ACS Applied Materials & Interfaces

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重新审视聚（邻苯二胺）作为有机正极材料的结构和电化学性能
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-06-08 , DOI: 10.1021/acsami.2c06208
Xi Zhang ₁ , Gaofeng Li ₁ , Junxiao Wang ₁ , Jun Chu ₁ , Feng Wang ₁ , Zijun Hu ₁ , Zhiping Song ₁

Affiliation

聚（邻苯二胺）（PoPDA）已被公认为一种低成本的电活性有机材料，并被研究用作水系锌电池的阴极或非水系锂电池的阳极。然而，对其合成、结构和电化学应用仍然存在很多困惑。特别是之前研究的PoPDA样品大多是在室温下合成的，我们证明它们只是一种二聚体，即2,3-二氨基吩嗪（DAPZ）。通过元素分析和质谱等多种表征方法，我们验证了高温合成的产物PoPDA-H是一种以DAPZ为结构重复单元并带有一些不完全取代物（OH和NH ₃⁺ CH ₃ COO ）的聚合物。^– )。基于吩嗪单元的可逆氧化还原反应和在 1.3-3.8 V vs Li ⁺ /Li 范围内的稳定聚合物结构，PoPDA-H 更适合用作锂电池的正极而不是负极。^{它在 50 mA g –1}下实现了 490 Wh kg ^–1 (2.12 V × 231 mAh g ^–1 ) 的高能量密度，在 500 mA g ^–1下实现了高循环稳定性（79%@1000 次循环），这两者与先前报道的昂贵的吡嗪和羰基聚合物相当。这项工作澄清了对PoPDA的许多误解，这对于其在储能设备中的实际应用的进一步发展具有重要意义。

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

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 × 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.

更新日期：2022-06-08

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