A new approach for compensating the irreversible capacity loss of high-energy Si/C|LiNi0.5Mn1.5O4 lithium-ion batteries

Gabrielli, Giulio; Marinaro, Mario; Mancini, Marilena; Axmann, Peter; Wohlfahrt‐Mehrens, Margret

doi:10.1016/j.jpowsour.2017.03.051

Cited by 86 publications

(80 citation statements)

References 57 publications

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“…This property makes LNMO an interesting candidate for high voltage applications [139]. Gabrielle et al and Mancini et al investigated different degrees of over-lithiated LNMO materials against graphite and Si/C composite anodes [140,141]. The over-lithiated Li1+xNi0.5Mn1.5O4 was synthesized by mixing the pristine compound with a reductive lithium-containing compound at 600 °C.…”

Section: Over-lithiated Positive Electrode Materialsmentioning

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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Section: Over-lithiated Positive Electrode Materialsmentioning

confidence: 99%

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

et al. 2018

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“…Therefore, different ideas to increase the amount of active lithium in lithium ion full-cells have been suggested, for example via prelithiation of silicon anodes with metallic lithium. [5][6][7][8] Recently, Gabrielli et al 9 successfully used LNMO that had been chemically overlithiated to compensate for the initial lithium loss in LNMO/silicon-carbon full cells. Alternatively, Shanmukaraj et al 10 proposed "sacrificial salts" as an additional source of lithium ions: A lithium salt is incorporated in the active material/carbon black matrix of the cathode.…”

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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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“…Those samples when compared to the 10 % SL paste printed samples (used in this study as CO‐3D), demonstrated that the areal capacity could be improved by over 25 % to 75 % to obtain a high areal capacity. This result exhibited a higher areal capacity (3.48 mAh/cm 2 ) for LMNO than the records in recent five years, due to its high active material mass loading (approximately 25 mg/cm 2 ) and high specific capacity (approximately 135 mAh/g) which benefited from the 3D structure and ALD coating (Figure h and S5).…”

Section: Figurementioning

confidence: 70%

Ultra‐Thin Coating and Three‐Dimensional Electrode Structures to Boosted Thick Electrode Lithium‐Ion Battery Performance

Gao

Liu

et al. 2018

Batteries & Supercaps

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This paper reports a multiscale controlled three‐dimensional (3D) electrode structure to boost the battery performance for thick electrode batteries with LiMn1.5Ni0.5O4 as cathode material, which exhibits a high areal capacity (3.5 mAh/cm2) along with a high specific capacity (130 mAh/g). This excellent battery performance is achieved by a new concept of cell electrode fabrication, which simultaneously controls the electrode structure in a multiscale manner to address the key challenges of the material. Particles with ultrathin conformal coating layers are prepared through atomic layer deposition followed by a nanoscale‐controlled, thermal diffusion doping. The particles are organized into a macroscale‐controlled 3D hybrid‐structure. This synergistic control of nano‐/macro‐structures is a promising concept for enhancing battery performance and its cycle life. The nanoscale coating/doping provides enhanced fundamental properties, including transport and structural properties, while the mesoscale control can provide a better network of the nanostructured elements by decreasing the diffusion path between. Electrochemical tests have shown that the synergistically controlled electrode exhibits the best performance among non‐controlled and selectively‐controlled samples, in terms of specific capacity, areal capacity, and cycle life.

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A new approach for compensating the irreversible capacity loss of high-energy Si/C|LiNi0.5Mn1.5O4 lithium-ion batteries

Cited by 86 publications

References 57 publications

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

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

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

Ultra‐Thin Coating and Three‐Dimensional Electrode Structures to Boosted Thick Electrode Lithium‐Ion Battery Performance

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