Professional Documents
Culture Documents
Nalin A. Chaturvedi
, Reinhardt Klein
,
,
Jake Christensen
, Jasim Ahmed
s
(x, t) in solid electrode, the electric potential
e
(x, t)
in electrolyte, the surface molar ux density j
n
(x, t) at the
surface of the spherical particle, the concentration c
e
(x, t) of
the electrolyte, and the concentration c
s
(x, r, t) of lithium in
the solid electrode particles at a distance r from the center
of a spherical particle located at x at time t [15].
The input to the model is the current that is applied to
the battery given by I(t), and the output of the model is the
corresponding output voltage V given by
V (t) =
s
(0
+
, t)
s
(0
, t), (1)
where 0
+
and 0
s
(x, t)
x
=
i
e
(x, t) I(t)
, (2)
where R
+
is the effective electronic conductivity of
the solid. Equation (2) has no explicit boundary conditions.
However, i
e
= 0 at 0
+
and 0
, and i
e
= I at L
+
and L
.
The third equation relating
e
and i
e
is given by
e
(x, t)
x
=
i
e
(x, t)
+
2RT
F
_
1 t
0
c
_
_
1 +
d ln f
d ln c
e
(x, t)
_
ln c
e
(x, t)
x
, (3)
where F is Faradays constant, R is the universal gas
constant, T is the temperature and f
x=0
=
c
e
x
x=0
+
= 0.
The fth equation relating c
s
and j
n
is described by
diffusion as
c
s
(x, r, t)
t
=
1
r
2
r
_
D
s
r
2
c
s
(x, r, t)
r
_
, (5)
where r is the radial dimension of the particles in the active
material. The boundary and initial conditions for (5) are
given by
c
s
r
r=0
= 0,
c
s
r
r=Rp
=
1
D
s
j
n
, c
s
(x, r, 0) = c
0
s
.
The sixth equation relating i
e
to j
n
is
i
e
(x, t)
x
= aFj
n
(x, t), (6)
where a =
3s
Rp
is a constant. The boundary condition is
i
e
= I at L
+
and L
and i
e
= 0 at 0
+
and 0
.
The seventh and the nal equation relating j
n
to c
e
, c
s
,
s
and
e
is the Butler-Volmer equation [16], [17]
j
n
=
i0
F
_
exp
_
aF
RT
s
_
exp
_
cF
RT
s
_
, (7)
where
a
and
c
are transport coefcients, i
0
is the exchange
current density, and
s
represents the overpotential. The
1998
overpotential
s
represents the change in potential that a
charged species would go through as it passes through the
spherical particle into the electrolyte, and is given as
s
(x) =
s
(x)
e
(x) U(c
ss
(x)) FR
f
j
n
(x), (8)
where for any given t, c
ss
(x) c
s
(x, R
p
). Note that the
equation for the molar ux density j
n
is algebraic. Thus,
all equations need to be solved together to satisfy the
algebraic constraint at every time t. The exchange current
density i
0
in (8) is given by i
0
= r
e
_
c
e
(x, t)(c
s,max
c
ss
(x, t))
_
a
c
ss
(x, t)
c
, where r
e
and c
s,max
are constants.
In summary, given that i
s
+i
e
= I, the six equations (2),
(3), (4), (5), (6) and (7) are solved for with applied current I
as the input and the output given by the voltage V as dened
in (1).
IV. MODEL REDUCTION
In section III, we presented the mathematical equations
describing a Li-ion battery. In this section, we analyze these
equations and present a novel compact structure for the Li-
ion battery model. This reformulation involves changing only
the structure and hence, no information of the model is lost
in the process.
A. Mathematical notation
Let C
r
(a, b) denote the function-space of all real-valued,
r-times continuously differentiable functions with domain
(a, b) R. By abuse of notation, we include 1 value for
r. A function in C
1
(a, b) is discontinuous, but its integral
exists and is continuous. More precisely, this function-space
is the Sobolev space H
1
(R) [18]. Note that C
(R)
C
(R) . . . C
0
(R) C
1
(R), where C
(R) represents
the space of analytic functions.
We next introduce the concept of a function-space map-
ping. In this article, we dene a function-map F as a mapping
that takes an element of C
r
(a, b) to C
q
(a, b) where r and q
are some integers. In other words, F : C
r
(a, b) C
q
(a, b) is
a function-map. We also introduce the notion of restriction of
a function by means of an example. Suppose g(x, t) R is a
function, that is, g : RR R. Then, the t-restriction of the
function g is dened as g
t
(x) g(x, t). Hence, g
t
: R R
denotes the value of g for some xed t.
B. Reduction of PDE system
We begin by reducing the system of ve PDEs and one
algebraic equation to two PDEs with time derivatives and
algebraic constraints. We focus on any one of the positive or
negative electrodes for this purpose. The spatial domain is
assumed to run from 0 to L. Thus, for the positive electrode
and the negative electrode, the corresponding domains are
[0
, L
] and [0
+
, L
+
], respectively (see Figure 1).
Consider equation (6). For a sufciently regular I(t) R,
we have j
t
n
(x) C
1
[0, L] for each time t R. Note that
I
t
= I(t) is a scalar for each t R. Now, we can solve
(6) as i
e
(x, t) =
_
x
0
aFj
n
(, t)d + i
e0
(I(t)). Dene the
function-map F
ie
: C
1
[0, L] R C
0
[0, L] as
F
ie
(g, ) (x)
_
x
0
aFg()d + i
e0
(). (9)
Then it is clear that a solution of the PDE in (6) for each t
is
i
e
(x, t) = i
t
e
(x) = F
ie
(j
t
n
, I
t
) (x). (10)
Here we have absorbed the constant of integration in F
ie
as the boundary condition of the PDE is known. Indeed, the
constant of integration is obtained by setting i
e
to either zero
or I(t) at one of the boundaries (x = 0 or x = L) of the
domain. Since the value of i
t
e
(x) is known at both x = 0 and
x = L, there are in fact two boundary conditions to satisfy.
Depending on whether it is the positive or negative electrode
or the separator, it is
{i
t
e
(0), i
t
e
(L)} =
_
{0, I(t)} (electrodes),
{I(t), I(t)} (separator).
(11)
For now, we choose any one of the above boundary
conditions (at x = 0 or x = L) to determine i
e0
in (9).
Similarly, we solve PDE in (2) for each t as
s
(x, t) =
t
s
(x) = F
s
(j
t
n
, I
t
) (x) +
s0
(t), (12)
where F
s
: C
1
[0, L] R C
1
[0, L] is dened as
F
s
(g, ) (x)
1
_
x
0
(F
ie
(g, ) (w) ) dw, (13)
w is a dummy variable, and
s0
(t) is an integration constant
that depends on boundary condition. Note that unlike F
ie
, we
do not absorb the integration constant in F
s
. This is because
we do not know a priori what the boundary condition is.
As we show later, the boundary condition appears implicitly
through the ux density j
n
(x, t) and the Butler-Volmer
equation. For now, we write
s0
(t) as a boundary condition
that is unknown.
Similarly, assuming a constant t
0
c
and performing some
manipulations, we solve for the PDE in (3) as
e
(x, t) =
t
e
(x) = F
e
(j
t
n
, c
t
e
, I
t
) (x), (14)
where F
e
: C
1
[0, L] C
0
[0, L] R C
1
[0, L] is
F
e
(g, h, ) (x)
_
x
0
F
ie
(g, ) (w)
(h(w))
dw
+
2RT
F
_
1 t
0
c
_
ln(f
h(x)) +
e0
(g, h, ), (15)
w is a dummy variable and f
s
(x, t) = F
s
(j
t
n
, I
t
) (x) +
t
s0
F
e
(j
t
n
, c
t
e
, I
t
) (x) U(c
t
ss
(x)) R
f
j
t
n
(x)F. (16)
1999
Equation (16) suggests that we can express
s
as a function
of j
n
, c
e
, c
ss
, I and
s0
for every x and t. Note that
t
s0
=
s0
(t) in (16) is the unknown boundary condition
or constant of integration for the
s
-equation, and that the
exchange current density is also a function of c
e
and c
ss
.
Thus, equation (7) can be expressed as
j
n
(x, t) = j
t
n
(x) = F
jn
(j
t
n
, c
t
e
, c
t
ss
, I
t
,
t
s0
) (x), (17)
where F
jn
: C
1
[0, L] C
0
[0, L] C
0
[0, L] R R
C
1
[0, L] is
F
jn
(f, g, h, , ) (x)
i
0
(x)
F
_
exp
_
a
F
RT
s
(x)
_
exp
_
c
F
RT
s
(x)
__
, (18)
i
0
(x) r
e
_
g(x)
_
a
_
c
s,max
h(x)
_
a
_
h(x)
_
c
, (19)
s
(x) F
s
(f, ) (x) F
e
(f, g, ) (x)
U(h(x)) R
f
f(x)F + . (20)
Note that (17) is an algebraic equation that has to hold
for every x and time t. Given the electrolyte concentration
c
t
e
(x), the surface concentration of the solid particle c
t
ss
(x) =
c
s
(x, R
p
, t), and the current I
t
, we need to nd j
t
n
(x) and
t
s0
that satisfy (17). However, there are two unknowns
j
n
(x, t) and
s0
(t) and only one equation (17). To solve
for j
n
and
s0
together, we now use the second boundary
condition on i
e
. Suppose to derive F
ie
in (9), we used
i
e
(0, t) = 0. Then, the other boundary condition on i
e
at the
separator-electrode interface is i
e
(L, t) = I(t). Thus, from
(10) it follows that
i
e
(L, t) = i
t
e
(L) = F
ie
(j
t
n
, I
t
) (L) = I(t), (21)
which is an algebraic constraint on j
n
(, t). Then, (17) and
(21) are solved together to obtain the current density j
n
(x, t)
and the boundary condition on
s
given by
s0
(t), for a
given electrolyte concentration c
e
(x, t), surface concentra-
tion of the electrode c
ss
(x, t) and current I(t).
The full Li-ion battery model is given by (2), (3), (4), (5),
(6) and (7). In this section, we have reduced these equations
to solving the dynamical equations (involving time) given by
(4) and (5) while satisfying the algebraic constraints in space
given by (17) and (21) at all times t.
V. SIMPLEST DISCRETIZATION OF THE MODEL
In the last section, we studied the equations for the model
given by PDEs (2), (3), (4), (5), (6) and (7), and reduced
them to a compact form given by (4) and (5), and the
algebraic constraint (17) and (21). In general, the equations
obtained from discretization of (17) and (21) along the
spatial dimension cannot be solved analytically. However,
it is possible to solve these equations analytically for the
case where the coarsest discretization is chosen. This yields
a model related to the single particle model (SPM) [13], [14].
A. Assumptions involving coarse discretization
Suppose we choose the lowest order of discretization for
the X-domain. Then, we have one node for the positive
electrode and one node for the negative electrode (and a
node at the separator; see Figure 2) with quantities at this
node representing their average over the whole electrode. Let
us consider the positive electrode. Assume that
ce
x
0 and
ce
t
0. This approximation holds if we assume that I is
small or is large. Then c
e
(x, t) c
0
e
R
+
is a constant.
Also, (4) yields that i
e
(x, t) = cnst(t), yielding that within a
domain (positive electrode, negative electrode, or separator),
i
e
remains a constant or that it does not vary in x. Then we
can express i
e
for the entire electrode by one value in each
of the electrode in the cell.
Fig. 2. Schematic showing variables for the approximate model.
B. Solution for the coarse discretization
Since only one node exists in the electrode, we express
the corresponding variables as scalar functions of time de-
noted as j
+
n
(t), i
+
e
(t),
+
s
(t),
+
e
(t), c
+
e
(t), c
+
s
(r, t), and
similarly for the negative electrode, as shown in Figure 2.
The function-maps in this case are easily solved as follows.
From (9) and (10), we obtain
0 = i
e
(0
+
, t) = i
+
e
(t) = F
ie
(j
t
n
, I
t
) (0
+
)
_
0
0
a
+
Fj
+,t
n
d + i
e0
(I
t
) = i
e0
(I
t
).
Thus, i
e0
(I
t
) = 0 is obtained from the boundary condition
that i
e
(0
+
, t) = i
+
e
(t) = 0. Next, substituting this boundary
condition in F
ie
and solving (21) implies that
I(t) = i
sep
e
(t) = i
e
(L
+
, t) = F
ie
(j
t
n
, I
t
) (L
+
)
=
_
L
+
0
a
+
Fj
+,t
n
d = j
+,t
n
L
+
a
+
F,
where i
sep
e
(t) is the current in the separator and hence,
j
+
n
(t) = j
+,t
n
=
I(t)
Fa
+
L
+
. (22)
Next, it follows from (12) and (13) that
+
s
(t) =
1
_
0
0
_
i
+
e
(t) I(t)
_
dw +
+
s0
(t) =
+
s0
(t). (23)
2000
Similarly, it can be shown that
+
e
(t) = 0 since
+
e0
(t) =
0 from the boundary condition that
e
= 0 at the current
collector of the positive electrode.
Finally, applying the last algebraic constraint (17) to (22),
and choosing
a
=
c
=
1
2
, it follows that
I(t)
2a
+
L
+
= r
e
_
c
0
e
c
+
ss
(t)(c
+
s,max
c
+
ss
(t)) sinh(
+
), (24)
+
=
F
2RT
_
+
s0
(t) U
+
(c
+
ss
(t)) +
R
+
f
I(t)
a
+
L
+
_
, (25)
where U
+
() is the OCP of the positive electrode and is
usually known from experiments.
Similarly, for the negative electrode, i
e0
(I(t)) = 0 is
obtained from the boundary condition that i
e
(0
, t) =
i
e
(t) = 0. Substituting this boundary condition in F
ie
and
solving (21) yields
j
n
(t) = j
,t
n
=
I(t)
Fa
. (26)
Equations (12) and (13) imply that
s
(t) =
1
_
0
0
_
i
e
(t) I(t)
_
dw +
s0
(t) =
s0
(t). (27)
Also (15) with the boundary condition that
e
= 0 at
the current collector of the positive electrode yields that
+
e0
(t) = 0 and hence
e
(t) =
1
_
0
0
+
i
e
(x, t)dx 0.
The above follows since i
e
(x, t) = I(t) in the separator and
I(t)/ 1 from the assumption for SPM that I(t) is small
or the conductance is large. Lastly, (17), along with the
assumption that
a
=
c
=
1
2
, yields
I(t)
2a
= r
e
_
c
0
e
c
ss
(t)(c
s,max
c
ss
(t)) sinh(
), (28)
=
F
2RT
_
s0
(t) U
(c
ss
(t))
R
f
I(t)
a
_
, (29)
where U
+
s0
(t) and (28) and (29) for
s0
(t) yielding
+
s
(t) from (23)
and
s
(t) from (27). Note that we need to compute c
+
ss
(t) =
c
+
s
(R
p
, t) and c
ss
(t) = c
s
(R
p
, t) by solving the PDE (4)
where j
n
(x, t) = j
+
n
(t) and j
n
(x, t) = j
n
(t), respectively.
Then, the output voltage V (t) =
+
s0
(t)
s0
(t).
VI. SIMULATION RESULTS
In section IV, we presented a compact form of the model
that is subsequently used to derive an approximation of
the electrochemical model (SPM) in section V. Since SPM
is an approximation, its applicability is only valid over
certain regimes. In this section, we illustrate some of these
limitations by means of simulation results. We present a brief
comparison of the full model given by (4) and (5), and the
algebraic equations (17) and (21) with SPM. In particular, we
consider cells that correspond to a high energy conguration
with applications in EVs.
To compare model performance, we compare output volt-
ages and surface concentrations computed from the two
models. The comparison of surface concentration c
ss
can be
used as an indicator of when the approximate model starts to
fail. We present a comparison between SPM and full model
for a high energy cell conguration with a nominal capacity
of 3.5 A-h. The applied currents are a constant discharge at
rates of C/25, C/2, 1 C and 2 C, where 1 C corresponds to
3.5 A.
0 1 2 3 4
2.5
3
3.5
4
4.5
V
o
l
t
a
g
e
[
V
]
C/25
0 1 2 3 4
2.5
3
3.5
4
4.5
C/2
0 1 2 3 4
2.5
3
3.5
4
4.5
V
o
l
t
a
g
e
[
V
]
Discharge Capacity [Ah]
1C
0 1 2 3 4
2.5
3
3.5
4
4.5
Discharge Capacity [Ah]
2C
Full Model
SPM
Full Model
SPM
Full Model
SPM
Full Model
SPM
Fig. 3. Comparison of the full model and the single particle model (SPM)
for a high-energy cell conguration.
The corresponding voltages for the full model and the
SPM are compared in Figure 3. As seen in the gure, SPM
is accurate until C, /2 where the discharge curves are almost
indistinguishable.
As seen in Figure 4, the surface concentration in an SPM
is the average surface concentration in the electrode. This
averaging follows from the fact that variables in an SPM
represent spatial average over electrodes. At higher discharge
rates of 1 C and 2 C, the uniformity in the concentration is
lost and SPM is no longer valid since concentrations cannot
be effectively represented by its spatial average due to large
variance. This failure of the approximation is noted in the
corresponding rate plots in Figure 3. In fact, even at C/2,
the variance in the surface concentrations shown in Figure 4
is large suggesting that SPM may have signicant errors in
its prediction of states of the full model.
VII. CURRENT STATUS ON BMS AND FUTURE WORK
Earlier in the paper, we mentioned that a BMS has to
perform certain tasks that are critical to the operation of
the battery. In particular for vehicle electrication, a sample
of these tasks include prediction of maximum available
power and energy, safe charging and discharging to meet
regenerative braking and load bearing requirements, tracking
the state of health of the battery pack as it ages, and updating
the BMS to maintain accuracy of its tasks throughout its life.
The importance of prediction of maximum available power
and energy is self-evident since this knowledge allows the
electronic control unit (ECU) to compute the vehicles all-
battery range in miles and the power it can deliver to
accelerate, if demanded. Though ideally, it is desirable to
have the ability to charge or discharge the battery as quickly
as possible, such processes can dangerously stress the battery
2001
0 1 2 3 4
0
0.5
1
c
s
s
/
c
m
a
x
C/25
0 1 2 3 4
0
0.5
1
C/2
0 1 2 3 4
0
0.5
1
Discharge Capacity [Ah]
c
s
s
/
c
m
a
x
1C 1C
0 1 2 3 4
0
0.5
1
Discharge Capacity [Ah]
2C 2C
c
ss
(x=0
)
c
ss
(x=L
)
c
ss
(SPM)
c
ss
(x=0
)
c
ss
(x=L
)
c
ss
(SPM)
c
ss
(x=0
)
c
ss
(x=L
)
c
ss
(SPM)
c
ss
(x=0
)
c
ss
(x=L
)
c
ss
(SPM)
Fig. 4. Surface concentrations over the electrode computed from SPM and
the full model for a high-energy cell conguration.
and accelerate aging. Thus, a BMS has to monitor overpoten-
tials and other relevant states that indicate potential damage
to the battery [19]. Finally, as the battery ages, a BMS
needs to track model parameters to maintain accuracy of
power and energy prediction throughout the life of the battery
pack. Each of the above BMS tasks, reects an estimation
or control problem.
We now briey mention some of the contemporary re-
search work on design of a BMS. A large section of the
research work on batteries uses a simple equivalent circuit
model for design of the BMS [2], [6], [3], [5], [7], [8]. This
choice stems from the fact that existing BMS for portable
electronics mostly models the battery as an equivalent circuit
and hence, its use in modeling is naturally extended to Li-ion
batteries for high-energy applications.
In contrast to equivalent circuit approach, [19], [20], [21],
[22], [23] study estimation problems using other models,
including electrochemical-based models. In particular, they
use approximations of electrochemical models and other
physics-based models to improve accuracy of estimation
algorithms for BMS. With this picture in mind, we mention
the future work that needs to be addressed for design of
improved and sophisticated BMS.
Referring to our earlier discussion in this section, the
future challenges are characterization of an approximation or
reduction of the full electrochemical model given by (4) and
(5), and the algebraic equations (17) and (21) such that the
model is accurate over a large range of operation and simple
enough that it is analytically tractable. Retaining the physical
signicance of the parameters is important since it helps in
characterizing aging phenomena in batteries. Next, the design
of simple algorithms for observing states of this model is an
open problem, especially when applied to the whole battery
pack and not just one cell. Finally, the estimation of all
parameters of the model to maintain accuracy of the model
and to identify age of the battery pack by tracking relevant
physical parameters is also an open problem.
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