Meng Yahan, Wang Mingming, Xu Jingwen, Xu Kui, Zhang Kai, Xie Zehui, Zhu Zhengxin, Wang Weiping, Gao Pengfei, Li Xiangyang, Chen Wei
Department of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
Interdisciplinary Center for Fundamental and Frontier Sciences, Nanjing University of Science and Technology, Jiangyin, Jiangsu 214443, China.
Angew Chem Int Ed Engl. 2023 Oct 2;62(40):e202308454. doi: 10.1002/anie.202308454. Epub 2023 Aug 29.
Metallic zinc (Zn) is considered as one of the most attractive anode materials for the post-lithium metal battery systems owing to the high theoretical capacity, low cost, and intrinsic safety. However, the Zn dendrites and parasitic side reaction impede its application. Herein, we propose a new principle of regulating p-band center of metal oxide protective coating to balance Zn adsorption energy and migration energy barrier for effective Zn deposition and stripping. Experimental results and theoretical calculations indicate that benefiting from the uniform zincophilic nucleation sites and fast Zn transport on indium tin oxide (ITO), highly stable and reversible Zn anode can be achieved. As a result, the I-Zn symmetrical cell achieves highly reversible Zn deposition/stripping with an extremely low overpotential of 9 mV and a superior lifespan over 4000 h. The Cu/I-Zn asymmetrical cell exhibits a long lifetime of over 4000 cycles with high average coulombic efficiency of 99.9 %. Furthermore, the assembled I-Zn/AC full cell exhibits an excellent lifetime for 70000 cycles with nearly 100 % capacity retention. This work provides a general strategy and new insight for the construction of efficient Zn anode protection layer.
金属锌（Zn）因其高理论容量、低成本和本质安全性，被认为是锂金属电池系统之后最具吸引力的负极材料之一。然而，锌枝晶和寄生副反应阻碍了其应用。在此，我们提出了一种调节金属氧化物保护涂层p带中心的新原理，以平衡锌的吸附能和迁移能垒，实现有效的锌沉积和剥离。实验结果和理论计算表明，得益于氧化铟锡（ITO）上均匀的亲锌成核位点和快速的锌传输，可以实现高度稳定且可逆的锌负极。结果，I-Zn对称电池实现了高度可逆的锌沉积/剥离，过电位极低，仅为9 mV，并且具有超过4000 h的优异寿命。Cu/I-Zn非对称电池表现出超过4000次循环的长寿命，平均库仑效率高达99.9 %。此外，组装的I-Zn/AC全电池在70000次循环中表现出优异的寿命，容量保持率接近100 %。这项工作为构建高效的锌负极保护层提供了一种通用策略和新见解。
