Stable Cycling of All‐Solid‐State Batteries with Sacrificial Cathode and Lithium‐Free Indium Layer

Choi, Hwa-Jung; Yoo, Yiseul; Lim, Hyeon‐Sook; Park, Jun‐Woo; Lee, Yoojin; Ha, Yoon‐Cheol; Lee, Sang‐Min; Kim, Byung Gon

doi:10.1002/adfm.202108203

Cited by 29 publications

(19 citation statements)

References 53 publications

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“…This has been demonstrated as an effective strategy for fabricating practical Li metal full cells [ 39 – 43 ]. However, the currently reported sacrificial agents, such as Li 2 O and Li 3 N, are air-sensitive and not suitable for actual productions [ 44 , 45 ]. An ideal cathode prelithiation reagent should possess excellent air stability, high charge specific capacity, low charge/discharge reversibility, reasonable operating voltage range and harmless decomposition products.…”

Section: Resultsmentioning

confidence: 99%

Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode

Lin

Xu²,

Qin

et al. 2022

Nano-Micro Lett.

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The energy density of commercial lithium (Li) ion batteries with graphite anode is reaching the limit. It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent. However, the poor reversibility and infinite volume change of Li metal hinder the realistic implementation of Li metal in battery community. Herein, a commercially viable hybrid Li-ion/metal battery is realized by a coordinated strategy of symbiotic anode and prelithiated cathode. To be specific, a scalable template-removal method is developed to fabricate the porous graphite layer (PGL), which acts as a symbiotic host for Li ion intercalation and subsequent Li metal deposition due to the enhanced lithiophilicity and sufficient ion-conducting pathways. A continuous dissolution-deintercalation mechanism during delithiation process further ensures the elimination of dead Li. As a result, when the excess plating Li reaches 30%, the PGL could deliver an ultrahigh average Coulombic efficiency of 99.5% for 180 cycles with a capacity of 2.48 mAh cm−2 in traditional carbonate electrolyte. Meanwhile, an air-stable recrystallized lithium oxalate with high specific capacity (514.3 mAh g−1) and moderate operating potential (4.7–5.0 V) is introduced as a sacrificial cathode to compensate the initial loss and provide Li source for subsequent cycles. Based on the prelithiated cathode and initial Li-free symbiotic anode, under a practical-level 3 mAh capacity, the assembled hybrid Li-ion/metal full cell with a P/N ratio (capacity ratio of LiNi0.8Co0.1Mn0.1O2 to graphite) of 1.3 exhibits significantly improved capacity retention after 300 cycles, indicating its great potential for high-energy-density Li batteries.

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Section: Resultsmentioning

confidence: 99%

Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode

Lin

Xu²,

Qin

et al. 2022

Nano-Micro Lett.

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“…Inspired by the concept of prelithiation strategies, Park et al first reported lithium nitride (Li 3 N) as the sacrificial cathode material to assemble all-solid-state batteries with Li-free In layer (Figure 4d). [62] In this study, Li 6 PS 5 Cl was used as solid electrolyte due to its high room-temperature ionic conductivity (10 À2 À10 À3 S cm À1 ). [63] It can be observed from the charging curve that a voltage plateau appeared at 2.4 V (%3.0 V vs Li/Li þ ), which was ascribed to the decomposition of Li 3 N (Figure 4e).…”

Section: The Solid Electrolytementioning

confidence: 99%

Challenges, Strategies, and Prospects of the Anode‐Free Lithium Metal Batteries

Shao

Tang

Zhang

et al. 2022

Adv Energy and Sustain Res

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The anode‐free lithium metal batteries (AF‐LMB), eliminating the use of host anode, can exploit the full potential of the lithium‐containing cathode system in terms of the highest retrievable gravimetric/volumetric energy densities, simplified processing of the anode coating, as well as the reduced cost of cell production and maintenance. However, the issues of interfacial contact resistance, curtailed ion pathway, as well as the dead lithium formation coherently lead to the unsatisfactory cation utilization upon repetitive cycling, which impairs the performance endurance of the practical relevance. Hitherto, a plethora of optimization strategies for the electrolyte and deposition substrate are proposed to extend the cell lifespan. Most of the methods, however, are still based on empirical attempts and lack of systematic diagnosis tools to elucidate the interplay between the structural evolution of the cathode and Li deposition behavior. Herein, the recent research process is summarized and the current development dilemma from multiple perspectives is probed, aiming to highlight the key features of the system that dedicate the cycling endurance. In addition, prospects of the operando characterizations that can be used to accelerate the mechanism elucidation of the AF‐LMB configuration are systematically commented.

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“…Combined, the B doping and the B coating protect the interior and exterior of a Ni-rich layered cathode to afford an ASSB that demonstrates superior long-term cycling stability. Finally, Figure S9 compares the cycling performance of the ASSB featuring a BCD-NCM90 cathode with those of recently reported ASSBs. − None of the reported ASSBs features a Ni-rich layered cathode with Ni contents ≥0.9; as a result, the ASSB featuring a BCD-NCM90 cathode and Li 6 PS 5 Cl SE demonstrates a much higher specific discharge capacity. The ASSB featuring a BCD-NCM90 cathode also outperforms other reported ASSBs in terms of areal capacity without compromising cycling stability.…”

mentioning

confidence: 96%

Microstructure- and Interface-Modified Ni-Rich Cathode for High-Energy-Density All-Solid-State Lithium Batteries

Kim

Lee

et al. 2023

ACS Energy Lett.

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Electric vehicles powered by Li-ion batteries pose a potential safety risk because the flammable liquid electrolytes can, under certain conditions, cause explosions. All-solid-state batteries (ASSBs) are safe alternative battery technologies. However, realizing high-energy-density ASSBs by employing Ni-rich layered cathodes is difficult because of the detrimental volume contraction near charge end. This study shows that the simultaneous B doping and coating of a Ni-rich Li[Ni 0.9 Co 0.05 Mn 0.05 ]-O 2 cathode, which modifies the cathode microstructure and cathode−solid electrolyte interface, respectively, afford an ASSB that cycles stably for 300 cycles with minimal capacity fading. An ASSB featuring the B-doped, B-coated Li[Ni 0.9 Co 0.05 Mn 0.05 ]O 2 cathode demonstrates a discharge capacity of 214 mAh g −1 , which represents one of the highest discharge capacities achieved by an ASSB; moreover, the ASSB retains 91% of its initial capacity after 300 cycles and easily outperforms previously reported ASSBs in terms of energy density without compromising cycling stability.

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Stable Cycling of All‐Solid‐State Batteries with Sacrificial Cathode and Lithium‐Free Indium Layer

Cited by 29 publications

References 53 publications

Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode

Commercially Viable Hybrid Li-Ion/Metal Batteries with High Energy Density Realized by Symbiotic Anode and Prelithiated Cathode

Challenges, Strategies, and Prospects of the Anode‐Free Lithium Metal Batteries

Microstructure- and Interface-Modified Ni-Rich Cathode for High-Energy-Density All-Solid-State Lithium Batteries

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