Localized concentration reversal of lithium during intercalation into nanoparticles

Zhang, Wei; Yu, Hui -Chia; Wu, Lijun; Liu, Hao; Abdellahi, Aziz; Qiu, Bao; Bai, Jianming; Orvananos, Bernardo; Strobridge, Fiona C.; Zhou, Xufeng; Liu, Zhaoping; Ceder, Gerbrand; Zhu, Yimei; Thornton, Katsuyo; Grey, Clare P.; Wang, Feng

doi:10.1126/sciadv.aao2608

Title: Localized concentration reversal of lithium during intercalation into nanoparticles

Journal Article · Fri Jan 12 00:00:00 EST 2018 · Science Advances

DOI:https://doi.org/10.1126/sciadv.aao2608· OSTI ID:1438434

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^[1]; Orvananos, Bernardo ^[6]; Strobridge, Fiona C. ^[7];

^[5]; Liu, Zhaoping ^[5]; Ceder, Gerbrand ^[8];

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Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of Michigan, Ann Arbor, MI (United States); Michigan State Univ., East Lansing, MI (United States)
Univ. of Cambridge, Cambridge (United Kingdom); Argonne National Lab. (ANL), Argonne, IL (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Chinese Academy of Sciences, Ningbo (People's Republic of China)
Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of Cambridge, Cambridge (United Kingdom)
Univ. of California, Berkeley, CA (United States)

Nanoparticulate electrodes, such as Li_xFePO₄, have unique advantages over their microparticulate counterparts for the applications in Li-ion batteries because of the shortened diffusion path and access to nonequilibrium routes for fast Li incorporation, thus radically boosting power density of the electrodes. However, how Li intercalation occurs locally in a single nanoparticle of such materials remains unresolved because real-time observation at such a fine scale is still lacking. We report visualization of local Li intercalation via solid-solution transformation in individual Li_xFePO₄ nanoparticles, enabled by probing sub-angstrom changes in the lattice spacing in situ. The real-time observation reveals inhomogeneous intercalation, accompanied with an unexpected reversal of Li concentration at the nanometer scale. The origin of the reversal phenomenon is elucidated through phase-field simulations, and it is attributed to the presence of structurally different regions that have distinct chemical potential functions. Furthermore, the findings from this study provide a new perspective on the local intercalation dynamics in battery electrodes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: SC0012704

OSTI ID:: 1438434

Report Number(s):: BNL-203647-2018-JAAM

Journal Information:: Science Advances, Vol. 4, Issue 1; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 50 works

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