Qiu Meijia, Ma Liang, Sun Peng, Wang Zilong, Cui Guofeng, Mai Wenjie
Key Laboratory for Polymeric Composite & Functional Materials of Ministry of Education, School of Chemistry, Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, Sun Yat-Sen University, Guangzhou, 510275, People's Republic of China.
Siyuan Laboratory, Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University, Guangdong, 510632, People's Republic of China.
Nanomicro Lett. 2021 Dec 13;14(1):31. doi: 10.1007/s40820-021-00777-2.
The stability of Zn anode in various Zn-based energy storage devices is the key problem to be solved. Herein, aromatic aldehyde additives are selected to modulate the interface reactions between the Zn anode and electrolyte. Through comprehensively considering electrochemical measurements, DFT calculations and FEA simulations, novel mechanisms of one kind of aromatic aldehyde, veratraldehyde in inhibiting Zn dendrite/by-products can be obtained. This additive prefers to absorb on the Zn surface than HO molecules and Zn, while competes with hydrogen evolution reaction and Zn plating/stripping process via redox reactions, thus preventing the decomposition of active HO near the interface and uncontrollable Zn dendrite growth via a synactic absorption-competition mechanism. As a result, Zn-Zn symmetric cells with the veratraldehyde additive realize an excellent cycling life of 3200 h under 1 mA cm/1 mAh cm and over 800 h even under 5 mA cm/5 mAh cm. Moreover, Zn-Ti and Zn-MnO cells with the veratraldehyde additive both obtain elevated performance than that with pure ZnSO electrolyte. Finally, two more aromatic aldehyde additives are chosen to prove their universality in stabilizing Zn anodes.
锌阳极在各种锌基储能装置中的稳定性是亟待解决的关键问题。在此，选择芳香醛添加剂来调节锌阳极与电解质之间的界面反应。通过综合考虑电化学测量、密度泛函理论（DFT）计算和有限元分析（FEA）模拟，可以得出一种芳香醛（藜芦醛）抑制锌枝晶/副产物生成的新机制。这种添加剂比水分子和锌更倾向于吸附在锌表面，同时通过氧化还原反应与析氢反应以及锌的电镀/剥离过程竞争，从而通过协同吸附-竞争机制防止界面附近活性水分子的分解以及不可控的锌枝晶生长。结果，添加藜芦醛的锌-锌对称电池在1 mA cm²/1 mAh cm²条件下实现了3200小时的优异循环寿命，甚至在5 mA cm²/5 mAh cm²条件下也能达到800多小时。此外，添加藜芦醛的锌-钛和锌-二氧化锰电池的性能均比使用纯硫酸锌电解质时有所提高。最后，选择另外两种芳香醛添加剂来证明它们在稳定锌阳极方面的通用性。
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