In Situ Construction of Anode–Molecule Interface via Lone-Pair Electrons in Trace Organic Molecules Additives to Achieve Stable Zinc Metal Anodes,Advanced Energy Materials

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In Situ Construction of Anode–Molecule Interface via Lone-Pair Electrons in Trace Organic Molecules Additives to Achieve Stable Zinc Metal Anodes
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-04-25 , DOI: 10.1002/aenm.202300550
Huaming Yu ₁ , Dongping Chen ₁ , Quanyu Li ₁ , Chunshuang Yan ₂ , Zihao Jiang ₃ , Liangjun Zhou ₁ , Weifeng Wei ₁ , Jianmin Ma ₄ , Xiaobo Ji ₁ , Yuejiao Chen ₁ , Libao Chen ₁

Affiliation

The practical application of aqueous zinc batteries (AZBs) is significantly limited by the poor reversibility of the zinc anodes, including rampant dendrite growth and severe interfacial side-reactions. Herein, trace hexamethylenetetramine (HMTA) additive with a lone-pair-electron containing heterocycle is introduced for Zn metal anode protection. Specifically, the trace added HMTA can change the solvated structure by strong interaction with zinc ions, and preferentially absorb on the anode surface to in situ establish an unique anode–molecule interface. Such an interface not only shows strong affinity to promote the dynamic transmission and deposition of Zn²⁺ ions but also displays a role in suppressing parasitic reactions. Consequently, a zinc anode in an electrolyte with trace HMTA achieves a high Coulombic efficiency of 99.75%, and delivers a remarkable lifespan over 4000 h at 5 mA cm⁻² and 1 mAh cm⁻² in a Zn//Zn symmetric cell. Even under a deep plating/stripping condition (5 mA cm⁻² and 5 mAh cm⁻²), it can still run almost for 600 h. Additionally, the Zn//V₂O₅ full cell with HMTA retains a high capacity retention of 61.7% after 4000 cycles at 5 A g⁻¹. Such an innovative strategy is expected to be of immediate benefit to design low-cost AZBs with ultra-long lifespan.

中文翻译：

通过微量有机分子添加剂中的孤对电子原位构建阳极-分子界面以获得稳定的锌金属阳极

水性锌电池 (AZB) 的实际应用受到锌阳极不良可逆性的显着限制，包括枝晶生长猖獗和界面副反应严重。在此，引入了含有孤对电子杂环的痕量六亚甲基四胺 (HMTA) 添加剂用于锌金属阳极保护。具体来说，微量添加的HMTA可以通过与锌离子的强相互作用改变溶剂化结构，优先吸附在阳极表面，原位建立独特的阳极-分子界面。这样的界面不仅表现出很强的亲和力，还能促进Zn ^{2+的动态传输和沉积}离子，但也显示出抑制寄生反应的作用。因此，在含有痕量 HMTA 的电解质中的锌阳极可实现 99.75% 的高库仑效率，并在 Zn//Zn 对称电池中在 5 mA cm -2 和 1 mAh cm ^-2 下^{提供超过 4000 小时的卓越寿命。}即使在深电镀/剥离条件下（5 mA cm ^-2 和5 mAh cm ^-2），它仍然可以运行近600小时。此外，具有 HMTA 的 Zn//V ₂ O ₅ 全电池在 5 A g ^-1下经过 4000 次循环后仍保持 61.7% 的高容量保持率。这种创新策略有望对设计具有超长寿命的低成本 AZB 产生立竿见影的好处。

更新日期：2023-04-25

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