Rechargeable aqueous zinc-ion batteries (AZIBs) have received increasing attention on account of their eco-friendliness and low cost. However, the limited capacity and poor rate properties of cathodes remain a major challenge due to the low electrochemical reactivity of cathode materials and sluggish Zn transport kinetics. Herein, we design a 1,5-naphthalenediamine (NAPD) pre-intercalate potassium manganese dioxide (KMO-NAPD) with high capacity and rate capability for AZIBs. The introduction of NAPD can delocalize the d-electrons spin states of the Mn site and activate the reactivity of KMO-NAPD for Zn intercalation. Moreover, the interaction between intercalated Zn and KMO-NAPD is weakened due to the decreased electrostatic interaction force, which promotes the diffusion of Zn. Consequently, the KMO-NAPD cathode exhibits high specific capacity (237 mAh g at 1 A g) satisfying rate capability (129 mAh g at 4 A g), and excellent cycling stability (85 % capacity retention after 1000 cycles). Furthermore, the fabricated AZIBs based on the KMO-NAPD exhibit a high energy density of 294.3 Wh kg and a peak power density of 8.6 kW kg. This study opens up a new path for the development of high-energy organic-inorganic hybrid cathode materials with modulated electronic structures for advanced AZIBs.

中文翻译：

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通过使 Mn 位点的 d 电子自旋态离域，促进水性锌离子电池中锰氧化物中 Zn2+ 的嵌入


可充电水性锌离子电池（AZIB）因其环保和低成本而受到越来越多的关注。然而，由于正极材料的电化学反应性低和锌传输动力学缓慢，正极的有限容量和较差的倍率性能仍然是一个主要挑战。在此，我们设计了一种 1,5-萘二胺 (NAPD) 预插二氧化钾锰 (KMO-NAPD)，其具有高容量和倍率性能，适用于 AZIB。 NAPD的引入可以使Mn位点的d电子自旋态离域并激活KMO-NAPD对Zn嵌入的反应性。此外，由于静电相互作用力减弱，插层Zn与KMO-NAPD之间的相互作用减弱，从而促进了Zn的扩散。因此，KMO-NAPD正极表现出高比容量（1 A g-1下为237 mAh g-1），满足倍率性能（4 A g-1下为129 mAh g-1）和优异的循环稳定性（1000次循环后容量保持率为85%）。此外，基于KMO-NAPD制造的AZIB表现出294.3 Wh kg的高能量密度和8.6 kW kg的峰值功率密度。这项研究为先进AZIBs的具有调制电子结构的高能有机-无机杂化阴极材料的开发开辟了一条新途径。