A prelithiated carbon anode for lithium-ion battery applications

Jarvis, Cody; Lain, Michael; Yakovleva, M. V.; Gao, Yuan

doi:10.1016/j.jpowsour.2005.07.051

Cited by 156 publications

(156 citation statements)

References 2 publications

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“…Assuming a constant gas volume, as would be the case for a hard-case cell, the pressure buildup can be expressed as 4: p = n CO 2 (total) K H RT V el RTc el + V gas K H [4] On the other hand, in soft pouch cells, gas evolution would typically lead to expansion (or bulging) of the cell. This volume expansion at a given pressure can be calculated by 5: V = RT n CO 2 (total) p − V el c el K H [5] To assess how much pressure buildup or volume expansion would actually occur in a commercial-scale cell containing 2.5 wt% lithium oxalate in the cathode electrode, we use a similar approximation for a commercial-scale 3 Ah cell as shown in ref. 16, where the weight for cathode active material and electrolyte solution were taken from Wagner et al 57 Furthermore, we also calculate the expected volume expansion for a 180 mAh pouch cell containing ∼ 0.75 mL electrolyte solution as used by Xia et al, 58 assuming a constant pressure of 1 bar in the cell.…”

Section: Discussionmentioning

confidence: 99%

Lithium Oxalate as Capacity and Cycle-Life Enhancer in LNMO/Graphite and LNMO/SiG Full Cells

Solchenbach

Wetjen

Pritzl

et al. 2018

J. Electrochem. Soc.

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In the present study, we explore the use of lithium oxalate as a "sacrificial salt" in combination with lithium nickel manganese spinel (LNMO) cathodes. By online electrochemical mass spectrometry (OEMS), we demonstrate that the oxidation of lithium oxalate to CO 2 (corresponding to 525 mAh/g) occurs quantitatively around 4.7 V vs. Li/Li + . LNMO/graphite cells containing 2.5 or 5 wt% lithium oxalate show an up to ∼11% higher initial discharge capacity and less capacity fade over 300 cycles (12% and 8% vs. 19%) compared to cells without lithium oxalate. In LNMO/SiG full-cells with an FEC-containing electrolyte solution, lithium oxalate leads to a better capacity retention (45% vs 20% after 250 cycles) and a higher coulombic efficiency throughout cycling (∼1%) compared to cells without lithium oxalate. When CO 2 from lithium oxalate oxidation is removed after formation, a similar capacity fading as in LNMO/SiG cells without lithium oxalate is observed. Hence, we attribute the improved cycling performance to the presence of CO 2 in the cells. Further analysis (e.g., FEC consumption by 19 F-NMR) indicate that CO 2 is an effective SEI-forming additive for SiG anodes, and that a combination of FEC and CO 2 has a synergistic effect on the lifetime of full-cells with SiG anodes. Lithium nickel manganese spinel (LiNi 0.5 Mn 1.5 O 4 , LNMO) is a promising cathode material for high energy lithium ion batteries due to its high operating potential around 4.7 V vs. Li/Li + , its high rate capability, structural stability and the absence of cobalt. However, its lower specific capacity (146 mAh/g LNMO ) compared to layered oxide materials (e.g. lithium nickel manganese cobalt oxide (NMC), specific capacity 150-250 mAh/g NMC ) 1 is regarded as a major drawback. In full-cells, the practically achievable capacity of LNMO is even lower, as the formation of the solid-electrolyte interphase (SEI) on the graphite anode consumes active lithium. For many layered oxide cathodes, however, the first cycle irreversible capacity of the cathode is similar to the capacity needed for SEI formation (∼20 mAh/g NMC ), and hence the practical discharge capacity of the cathode and the remaining active lithium are more or less balanced again. 2,3 In contrast, the first cycle irreversible capacity of LNMO (∼6 mAh/g LNMO ) is much lower than the capacity needed for SEI formation. This leads to a mismatch between active lithium and practical cathode capacity, i.e., there is not enough active lithium available to fully discharge the LNMO cathode during subsequent cycling.In cells with silicon-based anodes, active lithium losses on the anode are even higher compared to graphite, as the expansion of the silicon particles during the first lithiation leads to a continuous exposure of fresh, unpassivated silicon surface. 4 On this new surface, electrolyte reduction occurs instantaneously, which reduces the total lithium reservoir in the cell. Therefore, different ideas to increase the amount of active lithium in lithium ion full-cells have been suggested, ...

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Section: Discussionmentioning

confidence: 99%

Lithium Oxalate as Capacity and Cycle-Life Enhancer in LNMO/Graphite and LNMO/SiG Full Cells

Solchenbach

Wetjen

Pritzl

et al. 2018

J. Electrochem. Soc.

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“…The size of the SLMP particles ranges from ≈10-100 µm. The stabilized Li metal powder ( Figure 8) can be handled safely in dry air, in contrast to "normal" (non-treated) Li metal powder which is only stable under inert gas conditions [67]. Other Li products producing companies like Rockwood Lithium (now: Albemarle Corporation, Charlotte, NC, USA) have developed their own Li powder, i.e., coated lithium powder (CLiP) [69,70].…”

Section: Pre-lithiation By Direct Contact To Lithium Metalmentioning

confidence: 99%

Pre-Lithiation Strategies for Rechargeable Energy Storage Technologies: Concepts, Promises and Challenges

et al. 2018

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Abstract:In order to meet the sophisticated demands for large-scale applications such as electro-mobility, next generation energy storage technologies require advanced electrode active materials with enhanced gravimetric and volumetric capacities to achieve increased gravimetric energy and volumetric energy densities. However, most of these materials suffer from high 1st cycle active lithium losses, e.g., caused by solid electrolyte interphase (SEI) formation, which in turn hinder their broad commercial use so far. In general, the loss of active lithium permanently decreases the available energy by the consumption of lithium from the positive electrode material. Pre-lithiation is considered as a highly appealing technique to compensate for active lithium losses and, therefore, to increase the practical energy density. Various pre-lithiation techniques have been evaluated so far, including electrochemical and chemical pre-lithiation, pre-lithiation with the help of additives or the pre-lithiation by direct contact to lithium metal. In this review article, we will give a comprehensive overview about the various concepts for pre lithiation and controversially discuss their advantages and challenges. Furthermore, we will critically discuss possible effects on the cell performance and stability and assess the techniques with regard to their possible commercial exploration.

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“…In the past two decades, the first-cycle Coulombic efficiency of graphite anodes has increased from o80% to 90-95% through optimization of material quality, electrolyte and additives [11][12][13][14] . Further improvement is likely to result from pre-compensation or prelithiation of the electrodes 15 .…”

mentioning

confidence: 99%

“…In addition, prelithiation of a thick electrode with Li foil is time consuming, as it requires the diffusion of Li ions across the entire anode. Another approach is to use stabilized lithium metal powder (SLMP), which is effective to pre-compensate the first-cycle irreversible capacity loss of different anode materials, such as graphite and silicon-carbon nanotube (Si-CNT) composite 15,[42][43][44] . It is thus far the only prelithiation reagent in the powder form that can potentially be adopted during battery manufacturing, although practical challenges still exist to be addressed 45 .…”

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confidence: 99%

Dry-air-stable lithium silicide–lithium oxide core–shell nanoparticles as high-capacity prelithiation reagents

et al. 2014

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Rapid progress has been made in realizing battery electrode materials with high capacity and long-term cyclability in the past decade. However, low first-cycle Coulombic efficiency as a result of the formation of a solid electrolyte interphase and Li trapping at the anodes, remains unresolved. Here we report Li x Si-Li 2 O core-shell nanoparticles as an excellent prelithiation reagent with high specific capacity to compensate the first-cycle capacity loss. These nanoparticles are produced via a one-step thermal alloying process. Li x Si-Li 2 O core-shell nanoparticles are processible in a slurry and exhibit high capacity under dry-air conditions with the protection of a Li 2 O passivation shell, indicating that these nanoparticles are potentially compatible with industrial battery fabrication processes. Both Si and graphite anodes are successfully prelithiated with these nanoparticles to achieve high first-cycle Coulombic efficiencies of 94% to 4100%. The Li x Si-Li 2 O core-shell nanoparticles enable the practical implementation of high-performance electrode materials in lithium-ion batteries.

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A prelithiated carbon anode for lithium-ion battery applications

Cited by 156 publications

References 2 publications

Lithium Oxalate as Capacity and Cycle-Life Enhancer in LNMO/Graphite and LNMO/SiG Full Cells

Lithium Oxalate as Capacity and Cycle-Life Enhancer in LNMO/Graphite and LNMO/SiG Full Cells

Pre-Lithiation Strategies for Rechargeable Energy Storage Technologies: Concepts, Promises and Challenges

Dry-air-stable lithium silicide–lithium oxide core–shell nanoparticles as high-capacity prelithiation reagents

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