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A Li+-flux-homogenizing separator for long-term cycling of Li metal anodes
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2024-03-07 , DOI: 10.1039/d4ee00115j
Yuanpeng Ji 1, 2 , Liwei Dong 1 , Jipeng Liu 1 , Haodong Xie 2 , Shijie Zhong 2 , Chunhui Yang 1, 3 , Jiecai Han 2 , Weidong He 2, 4, 5
Affiliation  

Uneven arrangement of pores and the poor electrolyte affinity of separators made from polyolefins or poly(vinylidene difluoride) result in disordered Li+ flux and rugged deposition layers, triggering continuous consumption of lithium salt and premature expiration of lithium metal batteries (LMBs). Although adjusting the pore structure or modifying the surface of these separators is effective, it is space-occupied and not economically or industrially viable. Herein, we incorporate antistatic agent SN (SN), namely, octadecyl dimethyl hydroxyethyl quaternary ammonium nitrate, into PVDF-HFP matrix to prepare a homogeneous composite separator (PVDF-HFP/SN) for LMBs through a feasible method. The ammonium head of the SN provides numerous anion-friendly sites that absorb PF6 in the electrolyte. This forms the Li-affinity matrix of SN⋯PF6, which allows for the uniform distribution and deposition of Li+ in the SN⋯PF6⋯Li+ structure, and further, reduces the consumption of lithium salt and ensures the formation of a dendrite-free Li anode. Hence, using the PVDF-HFP/SN separator, we achieve exceptional stability of Li‖Li symmetric cells for 1000 hours at 0.5 mA cm−2 with a capacity of 1 mA h cm−2, and the Li‖LiFePO4 cell demonstrates a capacity of 120.4 mA h g−1 with an unparalleled capacity retention of 93.4% after 1000 cycles at 2C (1C = 170 mA g−1).

中文翻译:

用于锂金属阳极长期循环的Li+通量均化分离器

由聚烯烃或聚偏二氟乙烯制成的隔膜的孔排列不均匀和电解液亲和力差,导致Li +通量无序和沉积层凹凸不平,引发锂盐的持续消耗和锂金属电池(LMB)的过早失效。虽然调整孔结构或修饰这些隔膜的表面是有效的,但它占用空间并且在经济或工业上不可行。在此,我们将抗静电剂SN(SN),即十八烷基二甲基羟乙基季铵硝酸盐加入到PVDF-HFP基体中,通过可行的方法制备了用于LMB的均质复合隔膜(PVDF-HFP/SN)。 SN 的铵头提供了许多阴离子友好位点,可吸收电解质中的PF 6 - 。这就形成了SN⋯PF 6 的Li亲和矩阵,使得Li +在SN⋯PF 6 ⋯Li +结构中均匀分布和沉积,进一步减少了锂盐的消耗并保证了锂盐的形成无枝晶的锂负极。因此,使用PVDF-HFP/SN隔膜,我们实现了Li‖Li对称电池在0.5 mA cm -2下1000小时的优异稳定性,容量为1 mA h cm -2,并且Li‖LiFePO 4电池表现出容量为 120.4 mA hg -1,2C 循环 1000 次后容量保持率为 93.4%(1C = 170 mA g -1),无与伦比。
更新日期:2024-03-07
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