Dendrite-Free and Stable Lithium Metal Battery Achieved by a Model of Stepwise Lithium Deposition and Stripping

Abstract

Highlights A facile method is adopted to obtain cucumber-like lithiophilic composite skeleton. Massive lithiophilic sites in cucumber-like lithiophilic composite skeleton can promote and guide uniform Li depositions. A unique model of stepwise Li deposition and stripping is determined. Abstract The uncontrolled formation of lithium (Li) dendrites and the unnecessary consumption of electrolyte during the Li plating/stripping process have been major obstacles in developing safe and stable Li metal batteries. Herein, we report a cucumber-like lithiophilic composite skeleton (CLCS) fabricated through a facile oxidation-immersion-reduction method. The stepwise Li deposition and stripping, determined using in situ Raman spectra during the galvanostatic Li charging/discharging process, promote the formation of a dendrite-free Li metal anode. Furthermore, numerous pyridinic N, pyrrolic N, and CuxN sites with excellent lithiophilicity work synergistically to distribute Li ions and suppress the formation of Li dendrites. Owing to these advantages, cells based on CLCS exhibit a high Coulombic efficiency of 97.3% for 700 cycles and an improved lifespan of 2000 h for symmetric cells. The full cells assembled with LiFePO4 (LFP), SeS2 cathodes and CLCS@Li anodes demonstrate high capacities of 110.1 mAh g−1 after 600 cycles at 0.2 A g−1 in CLCS@Li|LFP and 491.8 mAh g−1 after 500 cycles at 1 A g−1 in CLCS@Li|SeS2. The unique design of CLCS may accelerate the application of Li metal anodes in commercial Li metal batteries.

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

“…LMA possesses unique superiority in energy density because it owns the lowest molar mass and reduction potential among metallic elements [ 49 , 50 ]. However, notorious dendrite propagation gives rise to large volume expansion, low reversibility and potential safety hazards [ 51 ].…”

Construction of a N,P doped 3D dendrite-free lithium metal anode by using silicon-containing lithium metal

“…At about 180 h, the discharge voltage rises sharply, indicating an internal circuit caused by the continuous collapse of SEI layers and unfettered Li dendrite penetration. 59,60 At the three highlighted locations during the first cycle (I, II, and III), the DLi/LiSi x CA||DLi/LiSi x CA cell (19 mV) also showed a small overpotential because of the low energy barrier at each stage. During the charging procedure (I), two large overpotentials resulted from a substantial blocking of Li + transport and the spontaneous development of SEI layers on the Li surface ( pure Li for 150 mV and Li-CC for 62 mV in Fig.…”

Multidimensional Co3O4/NiO heterojunctions with rich‐boundaries incorporated into reduced graphene oxide network for expanding the range of lithiophilic host

“…17 While normal 3D self-supporting matrixes can be effective for the electrochemical cycle, the uneven regulation of Li-ions is still a major issue. 16,[18][19][20] The construction of host structures with lithiophilic species modification has been supposed to form the isolated and randomly distributed nucleation sites for Li deposition, such as functional groups, [21][22][23] heteroatom-doped carbon, [24][25][26][27] and X-Li based alloy. [28][29][30][31] Now, a lot of 3D hosts have been developed to achieve excellent lithiophilicity and stable structure.…”