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Phys Chem Chem Phys. 2013 Jul 7;15(25):10402-12. doi: 10.1039/c3cp51662h. Epub 2013 May 17.

Reactive surface area of the Li(x)(Co(1/3)Ni(1/3)Mn(1/3))O2 electrode determined by μ(+)SR and electrochemical measurements.

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  • 1Toyota Central Research & Development Laboratories, Inc., 41-1 Yokomichi, Nagakute, Aichi 480-1192, Japan.


The self-diffusion coefficient of Li(+) ions (D(Li)) in the positive electrode material Li(x)(Co(1/3)Ni(1/3)Mn(1/3))O2 has been estimated by muon-spin relaxation (μ(+)SR) using powder samples with x = 1-0.49, which were prepared by an electrochemical reaction in a Li-ion battery. Here, since the implanted muons sense a slight change in the internal magnetic field due to Li-diffusion, μ(+)SR provides an intrinsic D(Li) through the temperature dependence of the nuclear field fluctuation rate (ν) [Sugiyama et al., Phys. Rev. Lett., 2009, 103, 147601]. Both D(Li) at 300 K and activation energy (E(a)) were estimated to be ∼2.9 × 10(-12) cm(2) s(-1) and 0.074 eV for the x = 1 sample, ∼11.0 × 10(-12) cm(2) s(-1) and 0.097 eV for x = 0.70, and ∼8.9 × 10(-12) cm(2) s(-1) and 0.062 eV for x = 0.49, assuming that the diffusing Li(+) ions mainly jump from a regular occupied site to a regular vacant site. The estimated D(Li) was smaller by roughly one order of magnitude than those for Li(x)CoO2 in the whole x range measured. Furthermore, by making comparison with D(Li) obtained by electrochemical measurements, the reactive surface area of the Li(x)(Co(1/3)Ni(1/3)Mn(1/3))O2 electrode in a liquid electrolyte was found to strongly depend on x particularly at x > 0.8.

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