Li‐Rich Li₂[Ni_0.8Co_0.1Mn_0.1]O₂ for Anode‐Free Lithium Metal Batteries

Abstract

Anode-free lithium metal batteries can maximizethe energy density at the cell level. However,w ithout the Li compensation from the anode side,i tf aces muchm ore challenging to achieve al ong cycling life with ac ompetitive energy density than Li metal-based batteries.Here,weprolong the lifespan of an anode-free Li metal battery by introducing Li-rich Li 2 [Ni 0.8 Co 0.1 Mn 0.1 ]O 2 into the cathode as aL i-ions extender.T he Li 2 [Ni 0.8 Co 0.1 Mn 0.1 ]O 2 can release al arge amount of Li-ions during the first charging process to supplement the Li loss in the anode,then convert into NCM811, thus extending the lifespan of the battery without the introduction of inactive elements.B yt he benefit of Li-rich cathode and high reversibility of Li metal on Cu foil, the anode-free pouchcells enable to achieve 447 Wh kg À1 energy density and 84 % capacity retention after 100 cycles in the condition of limited electrolyte addition (E/C ratio of 2gAh À1).

A Review of Performance Attenuation and Mitigation Strategies of Lithium‐Ion Batteries

“…[ 160 ] Therefore, how to improve the cycle life while maintaining high energy density is the biggest challenge faced by AFLMBs. [ 161–163 ]…”

Opportunities and Challenges of Li2C4O4 as Pre‐Lithiation Additive for the Positive Electrode in NMC622||Silicon/Graphite Lithium Ion Cells

“…In the first charge/discharge cycles of a LIB cell, the amount of irreversible capacity can be directly correlated with the active lithium loss, as reported previously. [ 5,12b ] The amount of additional lithium needed to compensate for ALL due to SEI formation was thus calculated from the irreversible capacity in the first cycle of NMC622||Si/graphite LIB cell (0 wt% Li 2 C 4 O 4 ), and was estimated to be ≈40 mAh g −1 . Therefore, based on the theoretical discharge capacity of Li 2 C 4 O 4 , the amount of pre‐lithiation additive needed to fully compensate for ALL should be ≈9.4 wt%.…”

“…[ 7a,b ] Over‐lithiation of the cathode material can be conducted electrochemically in a lithium metal cell [ 11 ] or chemically using reactive compounds such as n‐butyl‐lithium, lithium naphthalene, or lithium metal. [ 12 ] While many of the early studies on over‐lithiated cathode materials focused on the over‐lithiation of spinel oxides, such as Li 1+ x Mn 2 O 4 and Li 1+ x Ni 0.5 Mn 1.5 O 4 , [ 12b–e ] recent works have also reported the possible over‐lithiation of SOTA LiNi x Mn y Co z O 2 (NMC‐ xyz , x + y + z = 1) layered oxides, yet precise control is required to avoid irreversible phase transitions. [ 11b,12a,13 ] In both cases, either an additional production step is necessary or the use of an inert atmosphere is needed to handle the utilized chemicals and reaction conditions, raising safety concerns.…”

Highly Reversible Li‐Ion Full Batteries: Coupling Li‐Rich Li1.20Ni0.28Mn0.52O2 Microcube Cathodes with Carbon‐Decorated MnO Microcube Anodes

“…[9][10][11][12] However, these cathode materials are insufficient to satisfy the required performances for electric vehicles since the charge/discharge capacity about 120-200 mAh g À 1 was achieved. [13][14][15][16][17] Therefore, it is important to develop alternative cathodes having high energy-and power-density. Recently, Li-rich materials with the chemical formula of xLi 2 MnO 3 • (1-x)LiMO 2 (M = Ni, Mn, Co, etc.)…”

“…In the case of the cathode materials, layered LiCoO 2 , LiNi 0.33 Co 0.33 Mn 0.33 O 2 , olivine LiFePO 4 , spinel LiMn 2 O 4 were used widely in the commercialized LIB cathodes [9–12] . However, these cathode materials are insufficient to satisfy the required performances for electric vehicles since the charge/discharge capacity about 120–200 mAh g −1 was achieved [13–17] . Therefore, it is important to develop alternative cathodes having high energy‐ and power‐density.…”