Yang Qi, Li Liang, Hussain Tanveer, Wang Donghong, Hui Lan, Guo Ying, Liang Guojin, Li Xinliang, Chen Ze, Huang Zhaodong, Li Yongjun, Xue Yurui, Zuo Zicheng, Qiu Jieshan, Li Yuliang, Zhi Chunyi
Hong Kong Center for Cerebro-Cardiovascular Health Engineering, Hong Kong SAR, 999077, China.
Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Hong Kong SAR, 999077, China.
Angew Chem Int Ed Engl. 2022 Feb 1;61(6):e202112304. doi: 10.1002/anie.202112304. Epub 2021 Dec 20.
Zn dendrite issue was intensively studied via tuning zinc ion flux. pH change seriously influences dendrite formation, while its importance has not been revealed. Here, we construct a N-modification graphdiyne interface (NGI) to stabilize pH by mediating hydrated zinc ion desolvation. Operando pH detection reveals pH stabilization by NGI. This works with pores in NGI to achieve dendrite-free Zn deposition and an increased symmetric cell lifespan by 116 times. Experimental and theoretical results owe pH stabilization to desolvation with a reduced activation energy achieved by electron transfer from solvation sheath to N atom. The efficient desolvation ensures that electron directly transfers from substrate to Zn (rather than the coordinated H O), avoiding O-H bond splitting. Hence, Zn-V O battery achieves a long lifespan at 20.65 mA cm and 1.07 mAh cm . This work reveals the significance of interface pH and provides a new approach to address Zn dendrite issue.
通过调节锌离子通量对锌枝晶问题进行了深入研究。pH值变化严重影响枝晶形成，但其重要性尚未得到揭示。在此，我们构建了一个氮修饰的石墨炔界面（NGI），通过介导水合锌离子去溶剂化来稳定pH值。原位pH检测揭示了NGI对pH值的稳定作用。这与NGI中的孔隙协同作用，实现了无枝晶锌沉积，并使对称电池寿命延长了116倍。实验和理论结果表明，pH值的稳定归因于去溶剂化，通过从溶剂化鞘层到氮原子的电子转移降低了活化能。高效的去溶剂化确保电子直接从基底转移到锌（而不是配位的水分子），避免了O-H键的断裂。因此，锌-五氧化二钒电池在20.65 mA cm²和1.07 mAh cm²的条件下实现了长寿命。这项工作揭示了界面pH值的重要性，并提供了一种解决锌枝晶问题的新方法。
