Neutron imaging of lithium concentration in LiNi 0.33 Mn 0.33 Co 0.33 O 2 cathode

Abstract

LiNi_0.33Mn_0.33Co_0.33O₂ (NMC) is a promising substitute for LiCoO₂ because of its good thermal stability and high energy density. In this work, the lithium concentration distributions in an NMC cathode using neutron computed radiography technique at Oak Ridge National Laboratory’s High Flux Isotope Reactor (HFIR) CG-1D Cold Neutron Imaging Facility. Samples with four different state of charge (SOC) were prepared for neutron imaging: 70% SOC, 100% SOC, 105% SOC, and 110% SOC. The neutron tomographic reconstruction of NMC cathode reveals the information of electrochemical transport and spatial Li distribution inside the cathode. The experimental results were explained by a diffusion numerical model which maps the Li concentration evolution during the electrochemical reactions. The study demonstrates that neutron imaging technique can be a very powerful tool to understand the lithium concentrations and evaluate its state of conditions, thus providing information for design of safe lithium ion batteries and estimating their lives.

Keywords

Neutron scattering neutron radiography lithium ion battery concentration modeling

Get full access to this article

View all access options for this article.

References

Amin and

Y.-M.

Chiang, Characterization of electronic and Ionic transport in Li_{1- x}Ni_0.33Mn_0.33Co_0.33O₂ (NMC333) and Li_1-xNi_0.50Mn_0.20Co_0.30O₂ (NMC523) as a function of Li content, Journal of The Electrochemical Society 163(8) (2016), A1512–A1517. doi:10.1149/2.0131608jes.

Capron

et al., On the ageing of high energy lithium-ion batteries – comprehensive electrochemical diffusivity studies of harvested nickel manganese cobalt electrodes, Materials 11 (2018), 176. doi:10.3390/ma11020176.

S.J.

Harris

et al., Direct in situ measurements of Li transport in Li-ion battery negative electrodes, Chemical Physics Letters 485(4) (2010), 265–274. doi:10.1016/j.cplett.2009.12.033.

C.M.

Hayner,

Zhao and

H.H.

Kung, Materials for rechargeable lithium-ion batteries, Annual Review of Chemical and Biomolecular Engineering 3(1) (2012), 445–471. doi:10.1146/annurev-chembioeng-062011-081024.

Lanz

et al., In situ neutron radiography of lithium-ion batteries during charge/discharge cycling, Journal of Power Sources 101(2) (2001), 177–181. doi:10.1016/S0378-7753(01)00706-6.

Nanda

et al., Anomalous discharge product distribution in lithium-air cathodes, The Journal of Physical Chemistry C 116(15) (2012), 8401–8408. doi:10.1021/jp3016003.

Newman and

Tiedemann, Porous-Electrode Theory with Battery Applications, Vol. 21, AIChE Journal, 1975, pp. 25–41. doi:10.1002/aic.690210103.

NIST, X-Ray Mass Attenuation Coefficient s. [cited 2018; Available from: https://physics.nist.gov/PhysRefData/XrayMassCoef/tab3.html. doi:10.18434/T4D01F.

Nitta

et al., Li-ion battery materials: Present and future, Materials Today 18(5) (2015), 252–264. doi:10.1016/j.mattod.2014.10.040.

10.

Santodonato,

Bilheux,

Bailey et al., The CG-1D neutron imaging beamline at the Oak Ridge National Laboratory high flux isotope reactor, Physics Procidia 69 (2015), 104–108. doi:10.1016/j.phpro.2015.07.015.

11.

V.F.

Sears, Neutron scattering lengths and cross sections, Neutron News 3(3) (1992), 26–37. doi:10.1080/10448639208218770.

12.

R.B.

Smith and

M.Z.

Bazant, Multiphase porous electrode theory, Journal of The Electrochemical Society 164(11) (2017), E3291–E3310. doi:10.1149/2.0171711jes.

13.

D.F.

Swinehart, The Beer–Lambert law, Journal of Chemical Education 39(7) (1962), 333. doi:10.1021/ed039p333.

14.

et al., Three-dimensional finite element study on stress generation in synchrotron X-ray tomography reconstructed nickel-manganese-cobalt based half cell, Journal of Power Sources 336 (2016), 8–18. doi:10.1016/j.jpowsour.2016.10.052.

15.

Wu,

Wen and

Zhang, Three-dimensional finite element study on Li diffusion induced stress in FIB-SEM reconstructed LiCoO2 half cell, Electrochimica Acta 222 (2016), 814–820. doi:10.1016/j.electacta.2016.11.042.

16.

Zhang

et al., The nature of electrochemical delithiation of Li–Mg alloy electrodes: Neutron computed tomography and analytical modeling of Li diffusion and delithiation phenomenon, Journal of The Electrochemical Society 164(2) (2017), A28–A38. doi:10.1149/2.0051702jes.