Huang Chenghao, Guo Baiyu, Wang Xiaodong, Cao Qingping, Zhang Dongxian, Huang Jianyu, Jiang Jian-Zhong
International Center for New-Structured Materials (ICNSM), State Key Laboratory of Silicon Materials, and School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, P.R. China.
Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004, P. R. China.
Adv Mater. 2024 Jan;36(4):e2309732. doi: 10.1002/adma.202309732. Epub 2023 Dec 1.
Gallium-based metallic liquids, exhibiting high theoretical capacity, are considered a promising anode material for room-temperature liquid metal alkali-ion batteries. However, electrochemical performances, especially the cyclic stability, of the liquid metal anode for alkali-ion batteries are strongly limited because of the volume expansion and unstable solid electrolyte interphase film of liquid metal. Here, the bottleneck problem is resolved by designing carbon encapsulation on gallium-indium liquid metal nanoparticles (EGaIn@C LMNPs). A superior cycling stability (644 mAh g after 800 cycles at 1.0 A g ) is demonstrated for lithium-ion batteries, and excellent cycle stability (87 mAh g after 2500 cycles at 1.0 A g ) is achieved for sodium-ion batteries by carbon encapsulation of the liquid metal anode. Morphological and phase changes of EGaIn@C LMNPs during the electrochemical reaction process are revealed by in situ transmission electron microscopy measurements in real-time. The origin for the excellent performance is uncovered, that is the EGaIn@C core-shell structure effectively suppresses the non-uniform volume expansion of LMNPs from ≈160% to 127%, improves the electrical conductivity of the LMNPs, and exhibits superior electrochemical kinetics and a self-healing phenomenon. This work paves the way for the applications of room-temperature liquid metal anodes for high-performance alkali-ion batteries.
具有高理论容量的镓基金属液体被认为是室温液态金属碱离子电池很有前景的负极材料。然而,由于液态金属的体积膨胀和不稳定的固体电解质界面膜,碱离子电池液态金属负极的电化学性能,尤其是循环稳定性受到很大限制。在此,通过在镓铟液态金属纳米颗粒(EGaIn@C LMNPs)上设计碳包覆解决了这一瓶颈问题。对于锂离子电池,在1.0 A g-1下循环800次后展现出优异的循环稳定性(644 mAh g-1),对于钠离子电池,通过对液态金属负极进行碳包覆,在1.0 A g-1下循环2500次后实现了出色的循环稳定性(87 mAh g-1)。通过原位透射电子显微镜实时测量揭示了EGaIn@C LMNPs在电化学反应过程中的形态和相变。揭示了优异性能的来源,即EGaIn@C核壳结构有效地将LMNPs的不均匀体积膨胀从≈160%抑制到127%,提高了LMNPs的电导率,并展现出优异的电化学动力学和自修复现象。这项工作为高性能碱离子电池室温液态金属负极的应用铺平了道路。