Kang Tuo, Zhao Jianghui, Guo Feng, Zheng Lei, Mao Yayun, Wang Cheng, Zhao Yanfei, Zhu Jinghui, Qiu Yejun, Shen Yanbin, Chen Liwei
Shenzhen Engineering Lab of Flexible Transparent Conductive Films, School of Materials Science and Engineering , Harbin Institute of Technology , Shenzhen 518055 , China.
i-Lab, CAS Center for Excellence in Nanoscience , Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences , Suzhou 215123 , China.
ACS Appl Mater Interfaces. 2020 Feb 19;12(7):8168-8175. doi: 10.1021/acsami.9b19655. Epub 2020 Feb 5.
Li metal is considered the most promising anode for high energy density secondary batteries due to its high theoretical capacity and low redox potential. However, lithium is prone to form dendrites which will not only cause internal short-circuits but also bring accumulation of "dead Li" and result in fast capacity decay, thus its large-scale application is challenging. In this work, we demonstrate that the commonly used metal corrosion inhibitor, benzotriazole (BTA), can be used to modify the Cu foil surface and guide homogeneous Li plating/stripping due to the lithiophilic nature of the N atom in the BTA molecule. As a result, the lithium plated on the BTA modified Cu (BTA-Cu) substrate is free of dendrites, and a Coulombic efficiency (CE) as high as 99.0% was achieved for Li plating/stripping on the BTA-Cu substrate at a current density of 1 mA/cm. Furthermore, the BTA-Cu foil can be used as an anode to assemble an anode-free cell (BTA-Cu∥LFP), and ∼73.3% of the initial capacity can be obtained after 50 cycles. Last but not the least, a BTA-Cu@Li electrode prepared by plating of Li on the BTA-Cu substrate can serve as a stable Li anode in a BTA-Cu@Li∥LFP cell and display an average cycled CE of 98.5% at a depth of discharge (DOD) of 33%. This simple method of Li plating/stripping behavior regulation could inspire researchers on the development of highly stable lithium metal anodes for high energy density batteries.
锂金属因其高理论容量和低氧化还原电位,被认为是用于高能量密度二次电池最有前景的负极材料。然而,锂易于形成枝晶,这不仅会导致内部短路,还会造成“死锂”的积累并导致快速的容量衰减,因此其大规模应用具有挑战性。在这项工作中,我们证明了常用的金属腐蚀抑制剂苯并三唑(BTA)可用于修饰铜箔表面,并由于BTA分子中N原子的亲锂性来引导均匀的锂沉积/剥离。结果,沉积在BTA修饰的铜(BTA-Cu)基底上的锂没有枝晶,并且在1 mA/cm²的电流密度下,在BTA-Cu基底上进行锂沉积/剥离时实现了高达99.0%的库仑效率(CE)。此外,BTA-Cu箔可作为负极组装无负极电池(BTA-Cu∥LFP),在50次循环后可获得约73.3%的初始容量。最后但同样重要的是,通过在BTA-Cu基底上镀锂制备的BTA-Cu@Li电极可作为BTA-Cu@Li∥LFP电池中稳定的锂负极,并在33%的放电深度(DOD)下显示出98.5%的平均循环CE。这种调节锂沉积/剥离行为的简单方法可能会激发研究人员开发用于高能量密度电池的高度稳定的锂金属负极。