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

Wang, Wei; Zhou, Yanan; Zhang, Bao; Huang, Weiyuan; Cheng, Lei; Wang, Jing; He, Xinyou; Yu, Lei; Xiao, Zhiming; Wen, Jianguo; Liu, Tongchao; Amine, Khalil; Ou, Xing

doi:10.1021/acsnano.3c10986

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

Journal Article · Thu Mar 07 00:00:00 EST 2024 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.3c10986· OSTI ID:2498372

Wang, Wei ^[1]; Zhou, Yanan ^[2]; Zhang, Bao ^[3]; Huang, Weiyuan ^[4]; Cheng, Lei ^[2]; Wang, Jing ^[4]; He, Xinyou ^[1]; Yu, Lei ^[5]; Xiao, Zhiming ^[1]; ^[5]; ^[4]; ^[4]; ^[1]

Central South University, Changsha (China)
Zhejiang Power New Energy Co. Ltd., Zhuji (China)
Central South University, Changsha (China); Zhejiang Power New Energy Co. Ltd., Zhuji (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

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). Further, 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: National Natural Science Foundation of China; Natural Science Foundation of Hunan Province; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2498372

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 11 Vol. 18; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
improved Li+ diffusion kinetics
precursors engineering
single-crystal
ultrahigh-nickel layered cathodes
uniform in situ doping

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

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