Nitroxyl radical triggered the construction of a molecular protective layer for achieving durable Zn metal anodes,Journal of Colloid and Interface Science

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Nitroxyl radical triggered the construction of a molecular protective layer for achieving durable Zn metal anodes
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2024-03-12 , DOI: 10.1016/j.jcis.2024.03.085
Xipo Ma ₁ , Huaming Yu ₁ , Chunshuang Yan ₁ , Qihao Chen ₂ , Zheng Wang ₂ , Yuejiao Chen ₃ , Gang Chen ₁ , Chade Lv ₁

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The issues of dendrite growth, hydrogen evolution reaction, and zinc anode corrosion have significantly hindered the widespread implementation of aqueous zinc-ion batteries (AZIBs). Herein, trace amounts of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) additive is introduced into AZIBs to protect the zinc metal anode. Trace amounts of the TEMPO additive with nitroxyl radical can provide fast Zn transport and anode protection ability by forming an adsorbed molecular layer via Zn-O bond. This interface not only provides strong interfacial compatibility and promotes dynamic transport of Zn, but also induces deposition of Zn along Zn (002) plane. Additionally, the molecular protective layer significantly inhibits hydrogen evolution reaction (HER) and corrosion. The Zn anodes achieve high Coulombic efficiency of up to 99.75 % and long-term plating/stripping of more than 1400 h at 1 mA cm and 0.5 mAh cm. The Zn//Zn symmetric cell can operate continuously for 2500 h at a current density of 1 mA cm and 1 mAh cm, and it can still last for nearly 1400 h even when the current density is increased to 5 mA cm. Furthermore, the Zn//VO full cell using TEMPO/ZnSO electrolyte effectively maintains a maximum capacity retention rate of 53.4 % even after 1500 cycles at 5 A/g. This innovative strategy introduces trace additive with free radicals into the electrolyte, which may help to achieve large-scale, ultra-long-life, and low-cost AZIBs.

中文翻译：

硝酰基引发了分子保护层的构建，以实现耐用的锌金属阳极

枝晶生长、析氢反应和锌阳极腐蚀等问题严重阻碍了水系锌离子电池（AZIB）的广泛应用。在此，将痕量的2,2,6,6-四甲基哌啶-1-氧基（TEMPO）添加剂引入到AZIB中以保护锌金属阳极。微量的具有硝酰自由基的TEMPO添加剂可以通过Zn-O键形成吸附分子层来提供快速的Zn传输和阳极保护能力。该界面不仅提供了很强的界面相容性并促进了Zn的动态传输，而且还诱导了Zn沿着Zn（002）面沉积。此外，分子保护层可显着抑制析氢反应（HER）和腐蚀。锌阳极的库仑效率高达 99.75%，在 1 mA cm 和 0.5 mAh cm 下的长期电镀/剥离时间超过 1400 小时。 Zn//Zn对称电池在1 mA cm和1 mAh cm的电流密度下可连续运行2500 h，即使电流密度增加到5 mA cm，仍可持续运行近1400 h。此外，使用TEMPO/ZnSO电解质的Zn//VO全电池即使在5 A/g下循环1500次后仍能有效保持53.4%的最大容量保持率。这种创新策略将含有自由基的微量添加剂引入电解质中，这可能有助于实现大规模、超长寿命和低成本的AZIB。

更新日期：2024-03-12

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