In Situ Observation of Single-Phase Lithium Intercalation in Sub-25-nm Nanoparticles

Zhong, Li; Liu, Yang; Han, Wei-Qiang; Huang, Jian Yu; Mao, Scott X.

doi:10.1002/adma.201700236

Title: In Situ Observation of Single-Phase Lithium Intercalation in Sub-25-nm Nanoparticles

Journal Article · Fri May 05 00:00:00 EDT 2017 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201700236· OSTI ID:1399872

Zhong, Li ^[1]; Liu, Yang ^[2]; Han, Wei-Qiang ^[3]; Huang, Jian Yu ^[4]; Mao, Scott X. ^[1]

Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
Zhejiang Univ., Hangzhou (China). School of Materials Science and Engineering
Yanshan Univ., Qin Huang Dao, Hebei Province (China). Nano Energy Center, State Key Lab. of Metastable Materials Science and Technology

Although a non-equilibrium single-phase reaction, with the absence of nucleation and growth of a second phase, is believed to be a key factor for high-rate performance of lithium-ion batteries, it is thermodynamically unfavorable and usually proceeds in electrode materials with small particle sizes (tens of nanometers). Unfortunately, the phase evolutions inside such small particles are often shrouded by the macroscopic inhomogeneous reactions of electrodes containing millions of particles, leading to intensive debate over the size-dependent microscopic reaction mechanisms. Here, we provide a generally applicable methodology based on in-situ electron diffraction study on a multi-particle system to track the lithiation pathways in individual nanoparticles, and unambiguously reveal that lithiation of anatase TiO₂, previously long believed to be biphasic, converts to a single-phase reaction when the particle size is below ~25 nm. Our results imply the prevalence of such a size-dependent transition in lithiation mechanism among intercalation compounds whose lithium miscibility gaps are associated with a prominent size effect, and therefore provide important guidelines for designing high-power electrodes, especially cathodes.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC04-94AL85000; SC0001160; DESC0001160

OSTI ID:: 1399872

Alternate ID(s):: OSTI ID: 1401791

Report Number(s):: SAND-2016-7630J; 646434; TRN: US1702855

Journal Information:: Advanced Materials, Vol. 29, Issue 26; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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