Hua Kang, Ma Quanwei, Liu Yangyang, Xiong Peng, Wang Rui, Yuan Libei, Hao Junnan, Zhang Longhai, Zhang Chaofeng
Institutes of Physical Science and Information Technology, Leibniz Research Center of Materials Sciences of Anhui Province, Anhui University, Hefei 230601, China.
Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, New South Wales 2522, Australia.
ACS Nano. 2025 Apr 15;19(14):14249-14261. doi: 10.1021/acsnano.5c00833. Epub 2025 Apr 3.
Organic small-molecules with redox activity are promising cathode candidates for aqueous zinc-ion batteries (AZIBs) due to their low cost, high safety and high theoretical capacity. However, their severe dissolution leads to unsatisfactory electrochemical performance. Here, a dihydro-octaaza-pentacene (DOP) compound is synthesized as a cathode for AZIBs by extending its N heterocyclic molecular structure. The extended N heterocyclic structure provides dual active sites of n-type (C═N) and p-type (-NH-) redox reactions while reducing dissolution through enhanced π-conjugation. Hence, the Zn//DOP battery demonstrates improved performance, e.g., an enhanced capacity of 360 mAh g at 0.05 A g. Even under extended temperature conditions of - 50 and 50 °C, the batteries still maintain the capacities of 172 and 312 mAh g, respectively. In/ spectroscopy provide a thorough understanding of the storage mechanisms of cations and anions (Zn/H and ClO) through multielectron transfer process occurring at dual electroactive sites. This strategy offers a promising approach to designing high-performance zinc-organic batteries for sustainable energy storage.
具有氧化还原活性的有机小分子因其低成本、高安全性和高理论容量，有望成为水系锌离子电池（AZIBs）的正极材料。然而，它们的严重溶解导致电化学性能不尽人意。在此，通过扩展其二氢八氮并五苯（DOP）化合物的N杂环分子结构，合成了一种用于AZIBs的正极材料。扩展的N杂环结构提供了n型（C═N）和p型（-NH-）氧化还原反应的双活性位点，同时通过增强π共轭减少了溶解。因此，Zn//DOP电池表现出了改进的性能，例如在0.05 A g下容量提高到360 mAh g。即使在-50和50°C的扩展温度条件下，电池仍分别保持172和312 mAh g的容量。In/光谱通过在双电活性位点发生的多电子转移过程，深入了解了阳离子和阴离子（Zn/H和ClO）的存储机制。该策略为设计用于可持续储能的高性能锌有机电池提供了一种有前景的方法。
