Surface energy alteration-derived grain size regulation countering capacity deterioration in high-voltage single-crystal Ni-rich cathodes

Guo, Fuqiren; Qiu, Lang; Jiang, Yuandi; Deng, Yuting; Zhou, Junbo; Zheng, Zhuo; Liu, Yang; Sun, Yan; Wu, Zhen; Song, Yang; Guo, Xiaodong

doi:10.1039/d2ta08703k

Cited by 14 publications

(6 citation statements)

References 61 publications

(105 reference statements)

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“…In comparison, SNCM-pure and SNCM-Nb-dry display a consistent capacity decay, showing cycling retentions of 56.8% and 65.1%, respectively. As displayed in Table S3, SNCM-Nb-wet exhibits an obvious advantage on electrochemical performances in comparison with other modified Ni-rich cathodes. ,,− In addition, a comparison of charging/discharging curves of SNCM-Nb-dry and SNCM-Nb-wet from first to 200th cycle at 1 C, as presented in Figure b. It reveals that the in situ doped cathodes significantly suppress the polarization rise and voltage fade during long-term cycling, reflecting the less structural degradation for SNCM-Nb-wet .…”

Section: Resultsmentioning

confidence: 91%

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Wang,

Zhou,

Zhang

et al. 2024

ACS Nano

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Single-crystal Ni-rich cathodes offer promising prospects in mitigating intergranular microcracks and side reaction issues commonly encountered in conventional polycrystalline cathodes. However, the utilization of micrometer-sized single-crystal particles has raised concerns about sluggish Li + diffusion kinetics and unfavorable structural degradation, particularly in high Ni content cathodes. Herein, we present an innovative in situ doping strategy to regulate the dominant growth of characteristic planes in the singlecrystal precursor, leading to enhanced mechanical properties and effectively tackling the challenges posed by ultrahigh-nickel layered cathodes. Compared with the traditional dry-doping method, our in situ doping approach possesses a more homogeneous and consistent modifying effect from the inside out, ensuring the uniform distribution of doping ions with large radius (Nb, Zr, W, etc). This mitigates the generally unsatisfactory substitution effect, thereby minimizing undesirable coating layers induced by different solubilities during the calcination process. Additionally, the uniformly dispersed ions from this in situ doping are beneficial for alleviating the two-phase coexistence of H2/H3 and optimizing the Li + concentration gradient during cycling, thus inhibiting the formation of intragranular cracks and interfacial deterioration. Consequently, the in situ doped cathodes demonstrate exceptional cycle retention and rate performance under various harsh testing conditions. Our optimized in situ doping strategy not only expands the application prospects of elemental doping but also offers a promising research direction for developing high-energy-density single-crystal cathodes with extended lifetime.

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Section: Resultsmentioning

confidence: 91%

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Wang,

Zhou,

Zhang

et al. 2024

ACS Nano

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“…The surface oxygen release and the following reaction with electrolyte contribute to material surface reconstruction and gas production, which are the main causes of performance degradation and safety issues [ 84 , 95 , 96 ]. Introducing transition metal ions that can form strong covalent bonds with oxygen atoms is an effective method to bond oxygen and reduce its reactivity, and the frequently applied transition metal ions include Al, Zr and Nb [ 93 , 94 ]. Guo et al.…”

Section: Performance Enhancement Strategiesmentioning

confidence: 99%

Challenges and approaches of single-crystal Ni-rich layered cathodes in lithium batteries

Hu,

Wang,

Xiao

et al. 2023

National Science Review

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High-energy density and high safety are incompatible with each other in lithium battery, which challenges today's energy storage and power applications. Ni-rich layered transition metal oxides (NMC) have been identified as the primary cathode candidate for powering next-generation electric vehicles and were extensively studied in the last two decades, leading to the fast promotion on its market share including both polycrystalline and single crystal NMC cathodes. Compared to polycrystalline NMC, single crystal NMC appears to be the superior one, especially at low Ni content (≤ 60%). However, the Ni-rich single crystal NMC cathodes experience even faster capacity decay than the polycrystalline one, rendering them unsuitable for practical applications. Accordingly, this work will systematically review the attenuation mechanism of single crystal NMC and generate fresh insights into the valuable research pathway. This perspective is desired to provide an accurate direction for the development of Ni-rich single crystal NMC cathodes.

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“…Understanding and controlling the morphology of particles produced through coprecipitation in batch mode is essential for comprehending the synthesis parameters that influence the particle morphology and characteristics. Crystallinity and the morphology/size of primaries are important parameters for cathodes and are known to influence electrochemical performance. ,− A deep, comprehensive, and fundamental understanding of synthetic mechanisms and kinetics will be helpful for further optimization and better control of the processing and more effectively fine-tuning methodologies, ensuring desired morphology and ultimately leading to enhancements in the final product’s performance and consistency. In this study, the aim is to explore the coprecipitation processes employed in synthesizing the more complex, Ni-containing carbonate cathode precursors, focusing on the evolution of crystalline structures, TM distribution, and morphological attributes during synthesis as well as the impact on particle morphology of x in Ni x Mn 1– x CO 3 .…”

Section: Introductionmentioning

confidence: 99%

Unveiling Morphology and Crystallinity Dynamics in Ni_xMn_1–xCO₃ Cathode Precursors through Batch-Mode Coprecipitation

Chen,

Gutierrez,

Sultanov

et al. 2024

ACS Appl. Energy Mater.

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This study delves into the synthesis and control of Ni x Mn 1−x CO 3 , a critical class of Mn-rich, Co-free precursors vital for cathode-oxide materials in energy storage and conversion technologies. Employing batch-mode coprecipitation, we systematically generated samples with varying Ni concentrations (x = 0, 0.1, 0.3, 0.5, 0.7, and 0.9) and conducted a comprehensive analysis of their compositions, crystallinities, transition-metal distributions, and particle morphologies through both experimental and computational methods. A significant variation in particle size and crystallinity was observed, contingent on the Ni content. A pivotal transition emerged at Ni concentrations above x = ∼0.5, transforming uniform morphologies, such as spherical, monodisperse, pseudo-single-crystalline particles, into bimodal, polycrystalline structures. Furthermore, the study highlights the role of Ni−ammonia complexes leading to Ni-deficient precipitates and underscores the importance of ammonia concentration in achieving precise Ni content control. This study unveils critical reaction conditions governing Mn-rich precursor properties that are vital for cathode-oxides, emphasizing the need for meticulous synthetic control and offering the potential for practical applications in advanced energy storage and conversion systems.

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Surface energy alteration-derived grain size regulation countering capacity deterioration in high-voltage single-crystal Ni-rich cathodes

Abstract: Single-crystal Ni-rich cathodes possess prominent structural integrity and thermal stability compared to the poly-crystal counterparts, yet their application at high-voltage is hampered by the intragranular cracks which remain intractable to...

Cited by 14 publications

References 61 publications

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Challenges and approaches of single-crystal Ni-rich layered cathodes in lithium batteries

Unveiling Morphology and Crystallinity Dynamics in Ni_xMn_1–xCO₃ Cathode Precursors through Batch-Mode Coprecipitation

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Surface energy alteration-derived grain size regulation countering capacity deterioration in high-voltage single-crystal Ni-rich cathodes

Abstract: Single-crystal Ni-rich cathodes possess prominent structural integrity and thermal stability compared to the poly-crystal counterparts, yet their application at high-voltage is hampered by the intragranular cracks which remain intractable to...

Cited by 14 publications

References 61 publications

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Optimized In Situ Doping Strategy Stabling Single-Crystal Ultrahigh-Nickel Layered Cathode Materials

Challenges and approaches of single-crystal Ni-rich layered cathodes in lithium batteries

Unveiling Morphology and Crystallinity Dynamics in NixMn1–xCO3 Cathode Precursors through Batch-Mode Coprecipitation

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Unveiling Morphology and Crystallinity Dynamics in Ni_xMn_1–xCO₃ Cathode Precursors through Batch-Mode Coprecipitation