Magnesium Substitution in Ni‐Rich NMC Layered Cathodes for High‐Energy Lithium Ion Batteries (Adv. Energy Mater. 8/2022)

Gómez-Martín, Aurora; Reissig, Friederike; Frankenstein, Lars; Heidbüchel, Marcel; Winter, Martin; Placke, Tobias; Schmuch, Richard

doi:10.1002/aenm.202270029

Cited by 12 publications

(17 citation statements)

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“…State‐of‐the‐art (SOTA) cathode active materials (CAMs) are LiFePO 4 (LFP) and layered oxides such as LiNi 1‐ x‐y Co x Mn y O 2 (referred to as NCM xyz ; x + y + z =1) [3,4] . By increasing the Ni content within NCM materials, the energy density on material level can be gradually increased [1,5] .…”

Section: Introductionmentioning

confidence: 99%

Enabling Aqueous Processing of Ni‐Rich Layered Oxide Cathode Materials by Addition of Lithium Sulfate

et al. 2022

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Aqueous processing of Ni‐rich layered oxide cathode materials is a promising approach to simultaneously decrease electrode manufacturing costs, while bringing environmental benefits by substituting the state‐of‐the‐art (often toxic and costly) organic processing solvents. However, an aqueous environment remains challenging due to the high reactivity of Ni‐rich layered oxides towards moisture, leading to lithium leaching and Al current collector corrosion because of the resulting high pH value of the aqueous electrode paste. Herein, a facile method was developed to enable aqueous processing of LiNi0.8Co0.1Mn0.1O2 (NCM811) by the addition of lithium sulfate (Li2SO4) during electrode paste dispersion. The aqueously processed electrodes retained 80 % of their initial capacity after 400 cycles in NCM811||graphite full cells, while electrodes processed without the addition of Li2SO4 reached 80 % of their capacity after only 200 cycles. Furthermore, with regard to electrochemical performance, aqueously processed electrodes using carbon‐coated Al current collector outperformed reference electrodes based on state‐of‐the‐art production processes involving N‐methyl‐2‐pyrrolidone as processing solvent and fluorinated binders. The positive impact on cycle life by the addition of Li2SO4 stemmed from a formed sulfate coating as well as different surface species, protecting the NCM811 surface against degradation. Results reported herein open a new avenue for the processing of Ni‐rich NCM electrodes using more sustainable aqueous routes.

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Section: Introductionmentioning

confidence: 99%

Enabling Aqueous Processing of Ni‐Rich Layered Oxide Cathode Materials by Addition of Lithium Sulfate

et al. 2022

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“…Although NMC 750 °C shows good cycling stability, the achieved discharge capacity of 185 mAh/g at 20 °C and 0.1 C (18 mA/g), in a voltage window of 3.0‐4.3 V, is low compared to earlier reported results. Initial capacities above 200 mAh/g at 19–25 °C have been reported for Ni‐rich layered oxides with 85–90 at% Ni‐content [3,6,43,64,65] . Higher capacities have also been reported with lower Ni‐contents as well, such as above 190 mAh/g at 80 at% Ni [3,37,66–69] .…”

Section: Resultsmentioning

confidence: 96%

“…Several studies have observed that incorporating Al 3+ in NMC to form NMCA has improved the cycle life, [36–38] and Al 3+ has been reported to suppress the H2‐H3 phase transition associated anisotropic volume change [39,40] . Nb 5+ and Mg 2+ are other doping elements that have been explored to counteract the instability issues of Ni‐rich NMC [41–43] . As the Ni‐content increases there is correspondingly less substitutional freedom, and which supporting elements to include should be carefully considered due to their differing properties.…”

Section: Introductionmentioning

confidence: 99%

A Single‐Pot Co‐Precipitation Synthesis Route for Ni‐Rich Layered Oxide Materials with High Cycling Stability

et al. 2022

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In this work we report variations of LiNi 0.88 Mn 0.06 Co 0.06 O 2 synthesised through a single-pot oxalic acid co-precipitation route, in which all cation precursors were added in the same step. The effects of Al-doping, heat-treatment temperature and Li precursor excess were investigated with physicochemical and electrochemical characterisation. Phase pure and well-ordered polycrystalline materials were successfully synthesised for all Aldoped and undoped compositions. Undoped LiNi 0.88 Mn 0.06 Co 0.06 O 2 prepared at 750 °C with 4 at% excess Li precursor showed excellent cycling stability in NMC j j LTO cells with an initial capacity of 201 mAh/g at 0.1 C at 20 °C, and a capacity retention of 81 % after 415 cycles. The Al-doped variations LiNi 0.88 Mn 0.04 Co 0.06 Al 0.02 O 2 and LiNi 0.88 Mn 0.06 Co 0.04 Al 0.02 O 2 were synthesised, and they showed similar initial electrochemical performance to undoped LiNi 0.88 Mn 0.06 Co 0.06 O 2 , but Aldoping via the oxalic acid co-precipitation route resulted in shorter cycle life. The study outlines the importance of the processing parameters to achieve Ni-rich layered oxides with a long cycle life without further surface modifications.

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“…This helps explain the slightly larger presence of shattered particles from the LNO samples compared to the NBM samples, as continual cycling of these cracked particles can cause further mechanical pulverization from anisotropic lattice distortions typically seen with high‐Ni cathodes. [ 48,65 ]…”

Section: Resultsmentioning

confidence: 99%

“…The choice of Mg and B as dopants stems from the current understanding of Mg 2+ functioning as an inert pillaring ion in the Li layer to mitigate lattice collapse due to anisotropic distortions coupled with B promoting a robust microstructure and cathode‐electrolyte interphase (CEI) formation during cycling. [ 37,40–49 ] The NBM cathode exhibits a notable improvement in cycling stability with a 20% capacity retention increase over the baseline LNO cathode after long‐term cycling in pouch full cells. Hybrid pulse power characterization (HPPC) tests coupled with postmortem electrochemical, X‐ray diffraction (XRD), and scanning electron microscopy (SEM) analyses indicate more severe active Li loss present in the LNO cathode and less utilization in the graphite anode.…”

Section: Introductionmentioning

confidence: 99%

Stabilizing the Interphase in Cobalt‐Free, Ultrahigh‐Nickel Cathodes for Lithium‐Ion Batteries

Manthiram

2023

Adv Funct Materials

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High-nickel layered oxide cathodes, such as LiNi 1-x-y Mn x Co y O 2 (NMC) and LiNi 1-x-y Co x Al y O 2 (NCA), are at the forefront for implementation in highenergy-density lithium-ion batteries. The presence of cobalt in both cathode chemistries, however, largely deters their application due to fiscal and humanitarian issues affiliated with cobalt sourcing. Increasing the Ni content drives down the Co content, but introduces additional structural and electrochemical problems attributed to high-Ni cathodes. Herein a dually modified cobalt-free ultrahigh-nickel cathode 0.02B-LiNi 0.99 Mg 0.01 O 2 (NBM) is presented with 1 mol% Mg and 2 mol% B that exhibits a high initial 1C discharge capacity of 210 mA h g -1 with a 20% capacity retention improvement over 500 cycles when benchmarked against LiNiO 2 (LNO) in pouch full cell configurations with graphite anode. Postmortem analyses reveal the enhanced performance stems from reduced active lithium inventory loss and localized surface reactivity in the NBM cathode. The stabilized cathode-electrolyte interphase subsequently reduces transition-metal dissolution and ensuing chemical crossover to the graphite anode, which prevents further catalyzed parasitic reactions that harmfully passivate the anode surface. Altogether, this study aims to highlight the importance of electrode characterization and analysis from an interphasial viewpoint and to push the ongoing research to stabilize cobalt-free ultrahigh-Ni cathodes for industrial feasibility.

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Magnesium Substitution in Ni‐Rich NMC Layered Cathodes for High‐Energy Lithium Ion Batteries (Adv. Energy Mater. 8/2022)

Cited by 12 publications

References 0 publications

Enabling Aqueous Processing of Ni‐Rich Layered Oxide Cathode Materials by Addition of Lithium Sulfate

Enabling Aqueous Processing of Ni‐Rich Layered Oxide Cathode Materials by Addition of Lithium Sulfate

A Single‐Pot Co‐Precipitation Synthesis Route for Ni‐Rich Layered Oxide Materials with High Cycling Stability

Stabilizing the Interphase in Cobalt‐Free, Ultrahigh‐Nickel Cathodes for Lithium‐Ion Batteries

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