Structural Effects of Carbonization of LiFePO
4
Nanoparticles
V. Gariépy
1
, K. Vediappan
1
, P. Hovington
1
,
J. Trottier
1
, C. Gagnon
1
, F. Barray
1
, A. Guerfi
1
,
K. Zaghib
1
, A. Mauger
2
, C.M. Julien
3
1
Energy Storage and Conversion Division, IREQ,
Varennes, QC, Canada J3X 1S1
2
Université Pierre et Marie Curie – Paris6, IMPMC,
4 place Jussieu, 75005 Paris, France.
3
Université Pierre et Marie Curie – Paris6, PECSA,
4 place Jussieu, 75005 Paris, France.
Developing cathode materials with high energy
densities is one of the key challenges for adopting
the lithium-ion battery technology for green
transportation. LiFePO
4
(LFP) is one of the
prominent material used as the active element of the
positive electrode in lithium-ion and/or polymer
batteries. The presence of the poly-anion phosphate
group is of great interest, because it insures that this
compound is considerably more stable at the end of
charging than the close-packed oxide cathode
materials. However, LFP has disadvantages of low
intrinsic electrical conductivity, poor Li
+
-ion
transport and sensitivity to impurities. These major
problems are currently overcome using efficient
synthesis method and coating the particles with
conductive carbon, so that capacities close to the
theoretical predictions can be achieved [1].
In this work, we report the effect of
carbonisation at the surface of LFP cathode
materials prepared by hydrothermal (HT) steering-
assisted method that maintained the solution
agitation during the sample synthesis. The
structural characterization of C-LFP, surface
morphology and electrochemical cycling are
studied as a function of the synthesis conditions.
Carbonisation of LFP nanoparticles was
performed by mixing HTLPF and 10% lactose in
aqueous solution for 5 min. After drying at 95°C
under N
2
atmosphere, the slurries were heated at
different steps of temperature up to 700°C with
purge between each step.
The XRD diagrams of LFP samples before and
after the carbonization are shown in Figs. 1-2. The
carbon coating significantly decreases the amount
of Li
3
PO
4
impurities (Fig. 1). Also, we note for
most of the peaks a shift towards lower d spacing
and, as expected, a small decrease (4.8%) of the
crystallite size after carbonization at 700°C.
Detailed XRD patterns of carbonized nanoparticles
exhibit well-resolved the Bragg lines at ca. 2θ=73-
74°. This is attributed to the better crystallinity of
carbonized LFP nanoparticles. Also, it has been
demonstrated that the carbon coating cures the
disordered surface layer [2]. If the size of the
particles is further reduced, the surface over volume
ratio is increased, and the effect is even more
spectacular.
This effect is simply due to the fact that the
“surface over volume” ratio, i.e. the ratio between
the volumes occupied by the 3 nm-thick surface
layer and the core region, increases when the size of
the particle is reduced. For big particles where this
surface over volume is negligible, the contribution
of the surface layer to the electrochemical
performance is negligible. However, for particles of
diameter 40 nm, this surface over volume ratio is
0.11, which is non-negligible, and the contribution
of the surface layer is responsible for lower specific
capacity.
FIG. 1. XRD patterns showing the decrease of
Li
3
PO
4
impurities for carbonized LFP nanoparticles.
FIG. 2. XRD patterns showing the better
crystallinity of carbonized LFP nanoparticles.
References
[1] N. Ravet, A. Abouimrane and M. Armand, J.
Power Sources 97–98 (2001) 503.
[2] C.M. Julien, A. Mauger, K. Zaghib, J. Mater.
Chem. 21 (2011) 9955.
Abstract #864, 224th ECS Meeting, © 2013 The Electrochemical Society
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