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Prolonged lifespan of initial-anode-free lithium-metal battery by pre-lithiation in Li-rich Li2Ni0.5Mn1.5O4 spinel cathode
Authors:Leiyu Chen  Chao-Lung Chiang  Xiaohong Wu  Yonglin Tang  Guifan Zeng  Shiyuan Zhou  Baodan Zhang  Haitang Zhang  Yawen Yan  Tingting Liu  Hong-Gang Liao  Xiaoxiao Kuai  Yan-Gu Lin  Yu Qiao  Shi-Gang Sun
Abstract:Anode-free lithium metal batteries (AF-LMBs) can deliver the maximum energy density. However, achieving AF-LMBs with a long lifespan remains challenging because of the poor reversibility of Li+ plating/stripping on the anode. Here, coupled with a fluorine-containing electrolyte, we introduce a cathode pre-lithiation strategy to extend the lifespan of AF-LMBs. The AF-LMB is constructed with Li-rich Li2Ni0.5Mn1.5O4 cathodes as a Li-ion extender; the Li2Ni0.5Mn1.5O4 can deliver a large amount of Li+ in the initial charging process to offset the continuous Li+ consumption, which benefits the cycling performance without sacrificing energy density. Moreover, the cathode pre-lithiation design has been practically and precisely regulated using engineering methods (Li-metal contact and pre-lithiation Li-biphenyl immersion). Benefiting from the highly reversible Li metal on the Cu anode and Li2Ni0.5Mn1.5O4 cathode, the further fabricated anode-free pouch cells achieve 350 W h kg−1 energy density and 97% capacity retention after 50 cycles.

Benefiting from highly reversible structure evolution of pre-lithiated Li-rich Li2Ni0.5Mn1.5O4 cathode, the corresponding anode-free pouch cell delivers a considerable energy density of 350 W h kg−1 and 97% capacity retention after 50 cycles.
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