Synthesis and Processing by Design of High‐Nickel Cathode Materials

Wang, Feng; Bai, Jianming

doi:10.1002/batt.202100174

Cited by 18 publications

(10 citation statements)

References 70 publications

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“…In situ XRD has widely been used to study the synthesis of NCMbased layered oxides as summarized in a recent review. 24 In our study, we show that the simple blending of binary transition metal oxides and the use of Li 2 CO 3 as Li-source is perfectly suited to obtain SC-NCM83 in the same structural quality as in case of the conventional precursors already after a few hours of calcination at 900 °C. Furthermore, we investigate the influence of synthesis temperature on structure, particle size and electrochemical performance and find that calcination at 975 °C for 9 h yields a particle size of 2-3 μm and good electrochemical performance with a discharge capacity of 199 mAh g −1 in the first cycle at 0.05 C.…”

mentioning

confidence: 62%

Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Rueß

Ulherr

Trevisanello

et al. 2022

J. Electrochem. Soc.

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Single-crystalline Ni-rich LiNi1-x-y Co x Mn y O2 (SC-NCM) cathode active materials promise to increase the lifetime of high energy Li-ion batteries. SC-NCM consist of large primary particles that offer low surface area, limiting detrimental chemical reactions while exhibiting high morphological stability. A typical SC-NCM synthesis starts from the same Ni1-x-y Co x Mn y (OH)2 and LiOH∙H2O precursors commonly used for conventional spherical poly-crystalline NCM (PC-NCM), but requires higher temperatures and additional post-processing. Consequently, the cost and environmental impact of the production of Ni-rich SC-NCM is higher compared to the production of PC-NCM. In this study, we demonstrate a synthesis of SC-NCM that does not require the same highly engineered precursors as used for PC-NCM. We propose a more energy-efficient and cost-effective route that involves simple blending of NiO, MnO, Co3O4 and Li2CO3 which yields single-crystalline LiNi0.83Co0.11Mn0.06O2 with 2–3 μm particle size and good structural quality. It is shown by in situ XRD during synthesis that—while the reaction suffers from slow kinetics—the elevated temperature and longer reaction time, which are in any case required for the crystal growth, are sufficient to also complete the reaction. Furthermore, it is shown that this material is structurally and electrochemically equivalent to the material commonly synthesized from hydroxide-based precursors.

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mentioning

confidence: 62%

Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Rueß

Ulherr

Trevisanello

et al. 2022

J. Electrochem. Soc.

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“…Nickel-manganese-cobalt based cathodes with high Ni content are preferred in Li-ion batteries (LIBs), especially those powering electric vehicles because of their high storage capacity and low cost 1,2 . However, issues persist related to surface reconstruction, oxygen release, transition metal (TM) dissolution, bulk fatigue, and cracking, which precludes their use in practical applications [3][4][5][6][7] . Significant efforts have been made to alleviate these issues over the past decade, with increasing attention paid to high-Ni systemsgenerally represented by LiNi1-x-yMnxCoyO2 and LiNi1-x-yCoxAlyO2 (NMC and NCA, 1-x-y ≥ 0.8) with a layered structure 8,9 .…”

Section: Mainmentioning

confidence: 99%

Stabilizing Cobalt-Free Cathodes with Lithium-Stoichiometry Control for Sustainable Lithium-ion Batteries

Chen

Barai

Kahvecioğlu

et al. 2023

Preprint

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Lithium-ion batteries are essential to decarbonizing transportation and power grids, but their reliance on high-cost earth-scarce cobalt in nickel-manganese-cobalt (NMC) based cathodes raises significant supply chain and sustainability concerns. Despite numerous attempts to address these issues, eliminating Co has remained elusive, yet to be commercially realized because doing so detrimentally affects the layering and cycling stability of NMC cathodes. We report here an alternative solution using Co free high-Ni Li1 xNi0.95Mn0.05O2 (NM9505) with a Li-deficient composite structure that outperforms the stoichiometric layer-structured counterparts. Through correlated synchrotron X-ray characterization and multiscale modeling, we show that Li-deficiency plays a predominant role in hindering crystallization and interparticle fusion during calcination, resulting in intergrown rocksalt and layered phases within the composite. As such, the anisotropic lattice expansion and contraction is suppressed in Li-deficient NM9505 upon cycling, offering 90% first-cycle Coulombic efficiency, 90% capacity retention, and close-to-zero voltage fade for 100 cycles up to 4.4 V. Our findings represent an important step forward in addressing the critical Co-reliance issues, and offer new opportunities for designing high-performing Co-free cathodes for sustainable Li-ion batteries.

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“…In order to unveil the fundamental mechanism of the surface reconstruction in pristine layered oxides, in situ X‐ray diffraction has been carried out. [ 39 ] Through capturing the structures of samples during cooling process, it was found that surface reconstructions on LROs exhibited a rate‐dependent nature. Li 2 CO 3 was first observed on the surface and then the reconstruction happened during the cooling stage (>350 °C), resulting in the formation of a Li‐deficient spinel layer.…”

Section: In Situ Surface Reconstruction Strategiesmentioning

confidence: 99%

In Situ Surface Self‐Reconstruction Strategies in Li‐Rich Mn‐Based Layered Cathodes for Energy‐Dense Li‐Ion Batteries

Gou

Hao

et al. 2022

Adv Funct Materials

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Lithium‐rich manganese‐based layered oxides (LROs) are standing out as cathode materials of lithium‐ion batteries (LIBs) due to merits on both capacity (>250 mAh g−1) and operation voltage (≈3.6 V). However, the applications of LROs are plagued by almost inevitable degradation of structure, in which electrode surface bears the brunt as the primacy barrier for Li+ transport. Plenty of surface modification strategies are proposed to stabilize the structure and in situ self‐reconstruction strategies with atomic level connection to bulk structures provide robust layers to prevent the degradation. Herein, a critical review focusing on in situ surface reconstruction of LROs is summarized. It is started from the overview of LROs and then the surface challenges including lattice oxygen release, phase transformation, transition metal ions dissolution, and interfacial side reactions are further discussed. In situ self‐reconstruction strategies are emphasized to alleviate the performance degradation of LROs, from creating oxygen vacancies to synthesizing layered‐spinel or layered‐rocksalt heterogeneous structures. Among these approaches, synthesis and characterization methods, formation mechanisms and roles to stabilize the structures are highlighted. Finally, the prospects from the aspects of precise/large scale preparations, interphase design between electrolytes and electrodes, and in‐operando characterization approaches for the commercialization of LROs are provided.

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Synthesis and Processing by Design of High‐Nickel Cathode Materials

Cited by 18 publications

References 70 publications

Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Stabilizing Cobalt-Free Cathodes with Lithium-Stoichiometry Control for Sustainable Lithium-ion Batteries

In Situ Surface Self‐Reconstruction Strategies in Li‐Rich Mn‐Based Layered Cathodes for Energy‐Dense Li‐Ion Batteries

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Synthesis and Processing by Design of High‐Nickel Cathode Materials

Cited by 18 publications

References 70 publications

Transition Metal Oxides and Li2CO3 as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Transition Metal Oxides and Li2CO3 as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Stabilizing Cobalt-Free Cathodes with Lithium-Stoichiometry Control for Sustainable Lithium-ion Batteries

In Situ Surface Self‐Reconstruction Strategies in Li‐Rich Mn‐Based Layered Cathodes for Energy‐Dense Li‐Ion Batteries

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Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production

Transition Metal Oxides and Li₂CO₃ as Precursors for the Synthesis of Ni-Rich Single-Crystalline NCM for Sustainable Lithium-Ion Battery Production