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 A350 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)
0013-4651/2015/162(3)/A350/13/$31.00 © The Electrochemical Society

A Simulator for System-Level Analysis of Heat Transfer

and Phase-Change in Thermal Batteries
II. Multiple-Cell Simulations
Nir Haimovich,a,∗,z Dario R. Dekel,b and Simon Brandona
a Department of Chemical Engineering, Technion, Haifa 32000, Israel
b CellEra, Caesarea Business and Industrial Park, Caesarea, Israel

We present the application of our thermal battery system-level simulator [J. Electrochem Soc., 156, A442 (2009)] in novel multiple-
cell thermal analyses. Several model batteries are chosen to demonstrate the simulator’s versatility and robustness in developing
advanced thermal battery designs. The heat transfer phase-change model and supporting mass balance are modified to improve
model consistency. Simulation results are presented from several case-studies covering different battery structures and operating
conditions, including low and high current densities, different number of electro-active cells, various internal and external battery
geometrical details, the use of salt buffers, external flanges, and inhomogeneous initial conditions in the battery stack. These results
show the simulator to be a highly user-friendly and powerful tool for development of complex thermal batteries. Investigation of
heat of reactions and joule heating effects unfold insights regarding dominant processes in multiple-cell batteries. Furthermore,
these detailed analyses emphasize the need to track solidification dynamics at the sub-cell level and, at the same time, show that
thermal battery design should include a significant ingredient of multiple-cell analysis. Altogether, this study presents a first-in-its-
kind portable simulator with great flexibility and a capability for supporting the analysis and development of most thermal battery
structures and designs.
© 2014 The Electrochemical Society. [DOI: 10.1149/2.0411503jes] All rights reserved.

Manuscript submitted September 29, 2014; revised manuscript received December 12, 2014. Published December 23, 2014.

Thermal battery modeling efforts can be traced back to the semi-
nal mass transfer - electrochemical study of a single cell by Pollard
and Newman.1 However, despite the importance of thermal manage-
ment of these batteries, significant thermal modeling efforts have
appeared in the literature only during the last decade or so.2–6 More-
over, these studies typically involved reduced or incomplete thermal
models, mostly with a striking lack of consideration for the impact
of electrolyte phase-change on heat transfer, whose importance was
clearly indicated,7 and only recently revisited - though still only at a
single-cell level model.6
As thermal design of thermal batteries is a crucial though experi-
mentally complex process, a reliable and versatile simulation tool is
needed. In a recent publication8 we presented our system-level ther-
mal battery simulator, based on a thermal model, which can capture
geometrical details of most battery parts, unsteady conductive heat
transport, electrolyte phase change, heat of reactions and joule heat-
ing phenomena. Additional features include great flexibility in model
geometrical construction and material property data, thereby turning
this simulator into a viable tool for design and analysis of real systems.
In this manuscript we present the application of our simulator to
the thermal analysis and design of multiple-cell thermal batteries.
We first describe essential features of the latest version of the model
(previously presented in part I of this work8 ) and briefly discuss the re-
lation between the mass transfer resistance coefficient and the current
density drawn. Computational details are next provided, followed by
an extensive results section which, among other things, demonstrates
the model-based simulator’s flexibility in terms of its ability to de-
scribe systems with a rich variety of parameters. Analyzed results
yield a number of insights for the design of thermal batteries and
identification of dominant factors affecting their performance.
Mathematical Model and Computational Approach
Our approach is based on the model described in detail in part
I of this work,8 utilizing the original two-dimensional axisymmetric
geometry, as demonstrated in the 12-cell “base-case” battery structure
plot in Fig. 1. Here, we modify the original analysis for improved
consistency with respect to the definition of current density and the
changing cross-section available for current transport due to solidifi-
cation of electrolyte in the electrodes and separator. Specifically, we
∗
z
Electrochemical Society Active Member.
E-mail: haimovichn@gmail.com
introduce a new measure, ξ, which is the disk-averaged fraction of the
cross-sectional area available for charge transfer in the disk. This mea-
sure is separately tracked and updated throughout model calculations
over time for every disk in every cell in the stack. Using this measure,
together with the understanding that the current density (iA ) is defined
as the disk-averaged current per unit cross-section area available for
charge transfer, the modified equation for change of temperature in
the simulated battery is given by:
∂T ∂w
ρCp = ∇ · (k∇T) − ρχHfus + ξi2A R + (−Qrxn ) , [1]
∂t ∂t
where all symbols in this equation (as well as in all other equa-
tions shown here) are defined in the List of Symbols section of this
manuscript. The time-variation of temperature, on the left-hand-side
(LHS) of Eq. 1, is associated with sensible heat, and the first term
on the right-hand-side (RHS) is due to heat conduction; both of these
terms are present in all parts of the simulated battery. The second term
on the RHS, representing release of latent heat of solidification, is
formulated using a mushy region approach9,10 and is calculated only
in regions of the battery which contain salt. The third and fourth terms
on the RHS respectively account for joule heating and reversible heat
of reactions.1,3,8,11 The former is non-zero in the electrically active
parts of the battery alone, while the latter is only relevant within the
electrodes. This last term is given by:
 
∂U
(−Qrxn ) = ξ |iV | −T , [2]
∂T ρ
where, similar to Eq. 1, this equation was modified to account for ξ
together with the definition of |iV | as the absolute value of the disk-
averaged current density per unit volume available for charge transfer.
As explained in part I of this work,8 the time variation of the
thermal field (given here by Eq. 1) is coupled with the change of
electrolyte composition with time, both due to the dependence of
properties on composition and due to the latent heat of solidification
term (the second term on the RHS of Eq. 1). The previously described8
simplified mass transfer approach, modified to account for consistency
with respect to units of current density, yields a discretized equation
for the mole fraction of the salt’s first species (e.g. LiCl) given by:
 
ρsalt
Z (t) + #F·ρ
M2
· i V (t) · ω · t · ξ · ρ·χ
 .
salt
Z (t + t) = [3]
1 −M2 )
1 − (M#F·ρ salt
· iV (t) · ω · t · ξ · ρρ·χ
salt

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 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015) A351

calculated using an assumption of adiabatic heating of the stack dur-

ing the short ignition time,8 while accounting for the heat necessary
to melt the salt in the cells.
igniter top battery disks
top annular disks
bottom annular The mass transfer resistance coefficient.— Recall that in part I of
disks
top external radial insulation
this work8 the mass transfer resistance coefficient ω (see Eq. 3) was
top stack disks
defined to reflect mass transfer effects in each cell component. In
addition, a single value of ω was used for both electrodes of each cell
pyrotechnic internal radial insulation in order to maintain mass conservation at the cell level, based on this
cylinder
external radial insulation
model’s assumptions.8
Consider the relation between the current drawn from the battery
and ω. It is reasonable to believe that high current values cause the
time variation of composition to be dominated by the high rates of ion
12 electro-active cells
generation/consumption within the electrodes, and therefore should
be associated with relatively large values of ω (i.e. close to 1). On the
other hand, at low current values, mass transfer effects of diffusion-
migration are expected to be quantitatively sufficient to balance ion
generation/consumption, leading to a small accumulation or depletion
of the positive ion within the electrodes. It is therefore expected that
case relatively small currents should be associated with relatively small
values of ω.
Following the above discussion, in this manuscript we choose to
bottom stack disks
analyze multiple-cell thermal batteries using either a range of rela-
bottom battery tively low values of ω where relatively smaller current densities are
disks drawn, or a range of large values of ω where relatively high current
densities are drawn from the battery. Still, more exact values of ω
CL could be determined either by calibration versus experimental data, or
preferably by comparison with a validated detailed differential mass-
transfer electrochemical model.
Figure 1. Geometrical model of the 12-cell “base-case” thermal-battery with
an external cell diameter of φ = 30 mm. Details of battery parts are provided
in accordance to the general scheme presented in Ref. 8. Computational details.— All results presented in this manuscript
were generated by the simulator presented in part I of this work,8 with
the model modification suggested above. No other changes in the
It is important to note that iV is defined as the disk-averaged current applied numerical methods, GUI, mesh generation (and its interactive
density per unit volume available for charge transfer (absolute value) refinement via the GUI) or other features were either needed or made.
multiplied by either 0 in the separator, +1 in the anode or −1 in the Finally, note that in all cases the value of T used in calculations,
cathode. As mentioned above, all symbols are defined in the List of within zone 3 of the phase diagram (OEL), is 5◦ C, as in the single cell
Symbols section of this manuscript. simulation presented in Ref. 8.
Boundary conditions for Eq. 1 include symmetry at the centerline We analyze and discuss a number of simulated batteries, differing
(r = 0, see Fig. 1), continuity of heat fluxes and temperatures at inter- one from the other in the number of cells and/or system diameter.
nal boundaries within the battery, and loss of heat to the surroundings In Table I we present details of computations used when simulat-
via convection and radiation at the battery’s external surfaces. Initial ing different batteries depicted in Fig. 2. These include the simu-
conditions involve a single temperature for each battery component lated battery operation time, calculation elapsed time, number of time
(e.g., a separator or specific insulator). Usually, the initial (t = 0) steps, number of elements, number of unknowns and computational
temperature within the stack (cell-stack and pyrotechnic material run- platform. Additional information provided in this table includes rele-
ning through the annular center) is taken to be uniform and elevated vant parameter values (ω, iA , system diameter and number of cells).
compared to the rest of the domain. The value of this temperature is Further battery simulations (e.g., 12-cells with flanges) were executed

Table I. Computational details of the main simulated batteries.

Current
Density Calculation
Drawn Number of Number of Time Number of Elapsed Time Computational
Thermal Battery [A/cm2 ] ω Elements [ ] Unknowns [ ] Simulated [s] Time Steps [ ] [h] Platform
“base-case” 12-cells, 0.1 0.1 96,000 48,000 1200 190 8 8GB DDR2, 6MB
φ = 30 mm 0.3 cache, 2.5 GHz
1.0 0.7 150 145 5 quad-core Xeon
0.9 processor on a Silicon
24-cells, φ = 30 mm 0.1 0.1 177,000 88,900 1320 210 15 Graphics Linux
0.3 workstation
1.0 0.7 150 145 10
0.9
“wide” 12-cells, φ = 0.1 0.1 120,500 60,500 1560 200 14 4GB DDR2, 2MB
42.13 mm 0.3 cache, 3.0 GHz Xeon
1.0 0.7 150 145 9 processor on a
0.9 desktop Linux
machine∗
∗ the same computer used for calculations presented in Ref. 8.

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 A352 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)

Table II. IC Solver computational details of the main simulated batteries.

Calculation
Current Density Number of Number of Elapsed Time
Thermal Battery Drawn [A/cm2 ] ω Elements [ ] Unknowns [ ] [h]
“base-case” 12-cells, 0.1 0.1 30,000 16,000 1.5
φ = 30 mm 0.3
1.0 0.7
0.9
“wide” 12-cells, 0.1 0.1
φ = 42.13 mm 0.3
1.0 0.7
0.9
24-cells, φ = 30 mm 0.1 0.1 44,000 23,000 2
0.3
1.0 0.7
0.9

Results and Discussion

In this section we present various analyses of multiple-cell stack
thermal batteries conducted using our simulator (which is based on the
modified mathematical model presented above). A base-case 12-cell
battery is first analyzed where scenarios involving discharge under low
and high current densities are considered. We next present the analysis
of a battery with twice the number of cells, followed by a discussion
of a 12-cell battery whose cell-stack cross-sectional area is twice that
of the base-case system. In both cases low as well as high current
density discharge scenarios are considered. Finally, the impact of a
number of parameters on system performance is considered. These
include the thickness of insulation, the existence (and size) of flanges,
the insertion of salt buffers into the stack, the form of the initial stack
temperature profile and the heat of reactions and joule heating.

“Base-case” battery.— A model thermal battery consisting of

Figure 2. Geometrical models of the three main batteries tested here:
(a) Twelve-cell “base-case” thermal-battery with an external cell diameter
of φ = 30 mm (b) Twenty-four-cell thermal-battery with an external cell di-
ameter of φ = 30 mm (c) “Wide” 12-cell thermal-battery with an external cell
diameter of φ = 42.13 mm.
using numerical meshes within the range given in Table I and re-
quired similar elapsed times of calculation in accordance to the mesh
size, computational platform involved, and simulated battery opera-
tion time.
The “Initial Condition” (IC) Solver.— Application of the IC solver
(prior to mapping its results onto the full solver and activating the
latter)8 for the cases presented in this manuscript required substantial
calculation time. In Table II we present details of computations used
when applying the IC solver to the different batteries discussed in
Table I (each on the same respective computational platform on which
the full solver was run). These include the calculation elapsed time,
number of elements and number of unknowns. Additional information
provided in this table includes relevant parameter values (ω, iA , system
diameter and number of cells). It is important to note that the IC solver
has proved to be robust in all cases examined, including the case of
inhomogeneous initial conditions in the stack.
twelve serially connected cells was constructed. Other than the cell
stack, the model accounts for surrounding insulators and a sealing
battery case. Specific details of the geometry and material properties
used for this battery are provided in Fig. 1, Fig. 2a and Appendix A.
The stack initial temperature was set equal to 600◦ Cc while the sur-
rounding insulators and sealing case initial temperature was set equal
to 20◦ C (as was the surrounding ambient temperature for the entire
time of simulation). We chose to analyze two different extremes for
the current density per unit area drawn from the battery: 0.1 A/cm2
and 1.0 A/cm2 . These current density values were chosen because
they bracket most of the existing current densities under which ther-
mal batteries are discharged. Consistent with the above discussion,
regarding the relation between ω and the current density, sub-cases of
ω = 0.1 and 0.3 were applied (in all cells) for the case of the smaller
current density (0.1 A/cm2 ), and sub-cases of ω = 0.7 and 0.9 were
applied (in all cells) for the larger current density value (1.0 A/cm2 ).
Discharge under a current density of 0.1 A/cm2 .—Several snapshots
(contour maps at specific times) of the temperature field within the
battery, for the case of iA = 0.1 A/cm2 , are presented in Fig. 3 (with
both ω values simulated) for an operation time of up to 15.0 minutes
where final solidification is completed. The temperature field at any
given time seems almost independent of the value of ω, apart for a
slightly faster solidification process over the eutectic lined in the case
of the larger ω value. Comparison between these two cases is further
clarified by tracking minimum and maximum cell-stack temperatures
throughout battery operation time; see Fig. 4. A maximum temperature
difference between hottest and coldest spots of the cell-stack, of more
than 26◦ C, develops during the first few seconds of discharge. After
1 minute this temperature difference reduces to 15◦ C, after 5 minutes
c
based on calculated adiabatic heating of the stack during instantaneous ignition, while
considering the absorbed electrolyte latent heat of fusion.8
d
Referring to the salt’s phase diagram, as described in Ref. 8.

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 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015) A353

200 250 250

temperature of the ω = 0.1 sub-case as compared to that of the ω = 0.3
150
50 250
50
50 250 50 300 50 300 sub-case is less than 4◦ C. The same is true when comparing the
350 coldest cell stack temperatures, thus demonstrating the low sensitivity
350
40 40 450 40 40 of thermal fields to the value of ω in the range chosen.
In Fig. 5 we present time-temperature and molar fraction-
z [mm]

z [mm]

z [mm]

z [mm]
30 30 30 30 temperature plots at the center of all three electro-active disks be-
longing to the lowest (and in this case, coldest) cell in the stack. It
20 20 20 20
is obvious again that final process termination is due to solidification
10 550 10 10 350 10 over the eutectic line (assuming an excess of active material at the
350
450 electrodes throughout battery operation time8 ). Moreover, it seems
0 0 0 0 that mass transfer, reflected by the chosen range of values for ω,
0 10 20 0 10 20 0 10 20 0 10 20 does not significantly affect the temperature transient until this stage
r [mm] r [mm] r [mm] r [mm]
(OEL). This is despite the fact that, for the case of ω = 0.3, a complete
(a) (b) (c) (d)
depletion of Li+ ions at the anode takes place within zone 2 of the
salt’s phase diagram8 (BEL)e .
250 250
50
250
200
300 Battery operation time is typically determined by either a drop
50 250 150 50 50 50 300
350 below a specified voltage threshold, or due to a complete current
450
40 40 40 40 cutoff. The time it takes to reach both of these events is listed in
Table III. More specifically, these time-measures are the time in which
z [mm]

z [mm]

z [mm]

z [mm]

30 30 30 30 the coldest cell (average) temperature reaches 400◦ C, the time for
complete solidification OEL and the time for complete ion depletion
20 20 20 20 at the cathode. The first time measure is derived from the fact that the
350
cell’s electrical resistivity significantly increases when the tempera-
10 550 10 10 10
450 350
350
ture is decreased below 400◦ C (as can be deduced from the material
0 0 0 0 property data described in part I of this work8 ), therefore causing a
0 10 20 0 10 20 0 10 20 0 10 20 significant drop in battery voltage. It is important to stress that while
r [mm] r [mm] r [mm] r [mm] a drop below 400◦ C will impair the battery’s performance, complete
(e) (f) (g) (h) current cut off will be caused either by solidification OEL or by cath-
ode ion depletion (whichever occurs earlier). Having said that, there
Figure 3. Temperature field contours [◦ C] during simulated discharge of the are two more mechanisms (beyond the scope of our analysis) which
12-cell “base-case” battery at different times with a drawn current density of
may impact battery operation time. First of all, changes in molar con-
0.1 A/cm2 . For the case of ω = 0.1: (a) 1.0 [min] (b) 5.0 [min] (c) 10.0 [min]
(d) 15.0 [min], and for the case of ω = 0.3: (e) 1.0 [min] (f) 5.0 [min] (g) 10.0 centration may lead to increased electrical resistivity to a point where
[min] (h) 15.0 [min]. battery performance is compromised. In addition, complete current
cut off can occur due to the system reaching a percolation threshold
for ion transfer even before complete salt solidification.
to 8◦ C; after 10 minutes (and later on during final solidification) it An additional important set of data for analysis is the disk averaged
reduces to 5◦ C (for both ω = 0.1 and ω = 0.3 sub-cases). Therefore, current density per unit area as a function of time for the lowest
in this case of relatively small temperature gradients across the cell- (coldest) electro-active cell, presented in Fig. 6. As explained in part
stack there should be no significant spatial variations in electrical I of our work,8 the current density is sensitive to the narrowing cross-
resistivity (see material property data used, as published in part I of sectional area for charge transfer in the cell-component (disk) due to
this work8 ). It is also important to note that until phase change over salt solidification. Not only does this plot show (again) that complete
the eutectic line occurs, the difference between the hottest cell stack current cutoff is a result of the salt freezing process, it also reveals that
the separator, holding the largest percentage of electrolyte, dominates
this process, as seen in single cell simulations with the same current
density drawn.8 Finally, note that the same analysis for each of the
electro-active cells reveals that it is indeed the lowest cell in the stack
in which current cutoff first occurs, thus determining battery operation
time.
We next compare this battery’s thermal performance with that of
a single cell, with similar measures, materials, and conditions of op-
eration. This is the same single cell battery presented in part I of this
work,8 except for the external cell radius which, in this case, is equal
to 15.0 mm rather than the value of 17.5 mm used in Ref. 8; the thick-
ness of the surrounding insulation, perpendicular to the cell’s axis of
symmetry, as well as that of the (battery) case are identical to what
was used in Ref. 8. Time-temperature and molar fraction-temperature
plots of the single cell battery, displayed in Fig. 7, reveal that while the
cause for complete current cutoff is the same (freezing over the eutec-
tic line), the multiple-cell battery performance differs substantially in
several aspects. A system level effect related to the increased 12-cell
stack volume relative to its surface area is unfolded, as the time for
process termination is significantly larger than in the case of a single-
cell battery. While this may be attributed partly to the configuration
of insulations in the single cell battery, note that the 12-cell battery
exhibits a much larger Z (mole-fraction) span over the phase diagram
(for a given value of ω). The increased Z span in the 12-cell battery
Figure 4. Minimum and Maximum temperatures in the cell-stack as a function
of discharge time for the 12-cell “base-case” battery, at 0.1 A/cm2 current
density drawn with different ω values. e
As Z = 1 is reached in this zone (BEL) all LiCl is solidified as a pure salt

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 A354 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)

Figure 5. Trajectories of simulation results corresponding to the lowest electro-active cell in the 12-cell “base-case” battery for 0.1 A/cm2 current density drawn
and with different ω values: (a) Trajectories of molar composition and temperature at the center of each of the electro-active cell disks as viewed within the eutectic
salt phase diagram; the horizontal dotted line below the eutectic line displays the lower boundary of the artificial mushy region for the “over the eutectic line”
sub-model; T = 5◦ C (b) Temperature trajectories, as viewed in a temperature-time plot, at the same points as in (a).

Table III. Summary of measures for thermal battery operation time for each case-study presented.

Complete Current Cut-Off [min]

Current Density Drop below 400◦ C[min]
Thermal Battery Drawn [A/cm2 ] ω (drop below a specified voltage threshold) Solidification OEL Cathode Ion-Depletion
1-cell, φ = 30 mm 0.1 0.1 2.083 3.75 –
0.3 2.083 3.75 –
1.0 0.7 – – 0.8333
0.9 – – 0.5833
“base-case” 12-cells, 0.1 0.1 8.0 14.0 –
φ = 30 mm 0.3 8.5 15.0 –
1.0 0.7 – – 0.8333
0.9 – – 0.5833
24-cells, φ = 30 mm 0.1 0.1 9.5 19.0 –
0.3 10.5 – 18.0
1.0 0.7 – – 0.7500
0.9 – – 0.5833
“wide” 12-cells, 0.1 0.1 12.1 22.0 –
φ = 42.13 mm 0.3 13.5 – 18.0
1.0 0.7 – – 0.7500
0.9 – – 0.5833
12-cells, φ = 26 mm, 0.1344 0.1 8.64 14.0 –
increased radial
insulation
12-cells, φ = 30 mm, 0.1 0.1 8.75 17.0 –
with salt-buffers
12-cells, φ = 30 mm, 0.1 0.1 7.2 12.0 –
with (small) flange
12-cells, φ = 30 mm, 0.1 0.1 6.5 11.0 –
with larger flange
12-cells, φ = 30 mm, 0.1 0.1 7.3 12.0 –
inhomogeneous stack
IC’s
“base-case” 12-cells, 0.1 0.1 9.4 18.0 –
φ = 30 mm, no heat 1.0 0.9 – – 0.5833
of rxn’s
1-cell, φ = 30 mm, no 0.1 0.1 2.083 3.75 –
heat of rxn’s 1.0 0.9 – – 0.5833
“base-case” 12-cells, 0.1 0.1 7.9 13.0 –
φ = 30 mm, no
joule-heating 1.0 0.9 – – 0.5833
1-cell, φ = 30 mm, no 0.1 0.1 2.083 3.75 –
joule-heating 1.0 0.9 – – 0.5833

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 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015) A355

Figure 6. Disk-averaged current density per unit area

simulation results as a function of time for the lowest
electro-active cell in the 12-cell “base-case” battery (cur-
rent density drawn from the battery is equal to 0.1 A/cm2 )
with (a) ω = 0.1 and (b) ω = 0.3.

may be a result of the slower cooling rate, which is associated with
the stack overall thermal mass and smaller surface-to-volume ratio.
Longer times of discharge are then enabled, thus promoting the de-
velopment of significant variations in concentration in each cell even
under conditions of small current density and low resistance to mass
transfer. This is another system level effect emphasizing that thermal
design cannot rely on single cell simulation/testing alone.
Discharge under a current density of 1.0 A/cm2 .— Time-
temperature and molar fraction-temperature plots at the center of all
three electro-active disks belonging to the lowest (and in this case,
coldest) cell in the stack for this case are displayed in Fig. 8. As can
be seen there, the maximum battery operation time in this case ap-
pears to be much shorter than in the previous case, due to an enhanced
change in molar fractions as compared to heat loss rate, leading to pro-
cess termination by depletion of LiCl (Li+ ions) in the cathode regime
where its presence is mandatory for the electrochemical reaction. Not
Surprisingly, the chosen values of ω in this case, reflecting increased
resistance to mass transfer in the cells, have a larger effect on pre-
dicted maximum operation times than in the previous case of smaller
current densities (see Table III and Fig. 8b). The time dependence
of minimum and maximum cell-stack temperatures for this case is
exhibited in Fig. 9. A maximum temperature difference of more than
26◦ C builds up in the first few seconds across the whole cell-stack,
reducing to ∼15◦ C after just 15 seconds (for both ω = 0.7 and ω
= 0.9). The sudden “drop” in stack minimum temperature following
ignition (from 600◦ C to ∼575◦ C), suggests that the initial temperature
of the coldest spot in the stack is largely controlled by adjacent battery
insulators. This phenomenon is observed for a wide range of current
densities and ω values (see e.g. Fig. 4) as well as in the “dummy”
thermal analysis presented in part I of this work.8 Despite this phe-
nomenon, at these relatively high temperatures and relatively small
temperature differences, electrical resistivity across the stack should
be quite spatially uniform throughout battery operation time (i.e., the
electrical performance in this case is not sensitive to sensible heat
effects). Finally, note the strong effect of latent heat within the BEL
zone during battery operation in this case (Fig. 8a), which “holds” the
temperature at almost the same value during this fast-rate solidifica-
tion process; this seems to be dominated by the (large) current-driven
changes in molar fraction of LiCl in both electrodes.
Examining the disk averaged current density per unit area over
time for the lowest electro-active cell (Fig. 10), it is evident that for
both ω values, a significant degree of KCl solidification takes place in
the cathode. These results represent increasing local current densities
followed by an associated increased cell electrical resistance that may
finally lead to a drop below the specified voltage threshold.
Comparing this case with that of a single cell battery whose struc-
ture is described above, reveals the same cause for complete process
termination in both cases (Fig. 11). Moreover, it is most remarkable
to observe, in these simulation results, an identical operation time (re-
lated to complete current-cut off by cathode ion depletion) for both the
single cell battery and the 12-cell “base-case” battery (see Table III).
This observation is consistent with a system entirely controlled by

Figure 7. Trajectories of simulation results corresponding to the single cell battery (of an electro-active cell similar to those of the 12-cell “base-case” battery)
for 0.1 A/cm2 current density drawn and with different ω values: (a) Trajectories of molar composition and temperature at the center of each of the electro-active
cell disks as viewed within the eutectic salt phase diagram; the horizontal dotted line below the eutectic line displays the lower boundary of the artificial mushy
region for the “over the eutectic line” sub-model; T = 5◦ C (b) Temperature trajectories, as viewed in a temperature-time plot, at the same points as in (a).

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 A356 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)

Figure 8. Trajectories of simulation results corresponding to the lowest electro-active cell in the 12-cell “base-case” battery for 1.0 A/cm2 current density drawn
and with different ω values: (a) Trajectories of molar composition and temperature at the center of each of the electro-active cell disks as viewed within the eutectic
salt phase diagram; the horizontal dotted line below the eutectic line displays the lower boundary of the artificial mushy region for the “over the eutectic line”
sub-model; T = 5◦ C (b) Temperature trajectories, as viewed in a temperature-time plot, at the same points as in (a).

mass-transfer effects, in which heat transfer plays only a marginal
role in determining battery operation time. Furthermore, note that
temperature transients are moderated throughout operation by the re-
lease of latent heat of solidification, which in itself is accelerated by
mass-transfer controlled rapid changes in molar concentrations. This
effect is more pronounced in the 12-cell “base-case” battery as com-
pared to the single cell battery (see Figs. 8 and 11), seemingly due
to the enlarged thermal mass of the multiple-cell stack (and smaller
surface-to-volume ratio), representing a system-level effect.
Twenty four-cell battery.— A battery consisting of twenty four
serially connected cells was virtually assembled, similar in all aspects
to the 12-cell base-case battery presented above except for the number
of electro-active cells vertically assembled. Specific details of the
geometry and material properties used for this battery are detailed in
Fig. 2b and Appendix A. This case study involves current densities
drawn from the battery of (again) 0.1 and 1.0 A/cm2 , with mass
transfer resistance coefficient values of (again) ω = 0.1,0.3 and ω =
0.7, 0.9, respectively. The goal of this case-study is to examine the
performance of a battery producing twice the voltage with the same
currentf (and, also, at the same current density) as compared to using
two of the “base-case” batteries connected in series.
Discharge under a current density of 0.1 A/cm2 .—Generally, the 24-
cell battery performance qualitatively resembles that of the “base-
case” 12-cell system (see Table III). The cause for a complete current
cutoff in the case of ω = 0.1 is the solidification of salt over the
eutectic line only (OEL, zone 3), where in the case of ω = 0.3 cathode
ion-depletion occurs first, though it takes place just when reaching the
eutectic line. Therefore, the latter case does not indicate a departure
from the overall heat-transfer controlled nature of the system (seen
with ω = 0.1 and in the 12-cell battery for both ω values). Temperature
variations across the stack are identical to those observed in the 12-
cell battery (in respective points in time) to within a difference of 2◦ C
between the two cases. Finally, it is important to note that, consistent
with the slight decrease of surface to volume ratio in this system’s
stack as compared to the base case, we see (Table III) a slight increase
in measures of battery operation time.
Discharge under a current density of 1.0 A/cm2 .—In this case of a
larger current density drawn, battery performance is seen to resemble
the 12-cell battery even more than in the case of a lower current
density. Temperature variations across the stack are identical to those
observed in the 12-cell battery (in respective points in time) to within
a difference of 2◦ C between the two cases. Time-temperature and
molar fraction-temperature plots for this case (not presented here)
are almost identical to those of the 12-cell battery shown in Fig. 8.
Process termination, induced by positive ion depletion at the cathode,
is at the exact same time as in the 12-cell battery when ω = 0.9, and
a few seconds earlier when ω = 0.7 (see Table III). This remarkable
similarity suggests that the stack’s temperature-time characteristics
are largely controlled by the endothermic heat of reaction, latent heat
of fusion, and the cell-stack’s thermal massg , rather than heat transfer
from the stack to the surroundings (which is sensitive to geometry).
The obvious qualitative difference in battery thermal history during its
operation, between low and high current density cases (observed in 1,
12 and 24 cell batteries), suggests that thermal battery design for high
current density discharge should focus on mass transfer optimization.

Figure 9. Minimum and Maximum temperatures in the cell-stack as a function
of time for the 12-cell “base-case” battery simulation with 1.0 A/cm2 current
density drawn and with different ω values.
f
Alternatively this battery can be thought of as producing the same voltage with twice the
current, achieved by electrically dividing the cell stack in half, placing 3 current collectors
instead of 2, and electrically connecting the 2 halves of the cell stack in parallel.
g
And possibly also joule heating as is further detailed below.

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 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015) A357

Figure 10. Disk-averaged current density per unit area

simulation results as a function of time for the lowest
electro-active cell in the 12-cell “base-case” battery (cur-
rent density drawn from the battery is equal to 1.0 A/cm2 )
with (a) ω = 0.7 and (b) ω = 0.9.

Figure 11. Trajectories of simulation results corresponding to the single cell battery (with an electro-active cell similar to those of the 12-cell “base-case” battery)
for 1.0 A/cm2 current density drawn and different ω values: (a) Trajectories of molar composition and temperature at the center of each of the electro-active cell
disks as viewed within the eutectic salt phase diagram; the horizontal dotted line below the eutectic line displays the lower boundary of the artificial mushy region
for the “over the eutectic line” sub-model; T = 5◦ C (b) Temperature trajectories, as viewed in a temperature-time plot, at the same points as in (a).

“Wide” twelve-cell battery.—Following the 12-cell and the 24-cell
batteries, we now discuss the simulated discharge of an additional
12-cell battery identical to the base-case configuration except for the
cell-stack’s cross-sectional area that is doubled in value. Details of the
geometry and material properties used for this battery are provided
in Fig. 2c and Appendix A. Again, current densities drawn from the
battery were set to 0.1 A/cm2 and 1.0 A/cm2 , with mass transfer
resistance coefficient values of (again) ω = 0.1, 0.3 and ω = 0.7,
0.9, respectively. This battery is thus comparable and serves as an
alternative to the previous case of the 24-cell battery in a situation
where the latter’s cell stack is electrically divided in two thereby
producing twice the current of the “base-case” battery (with the same
voltage). In addition, this case study is useful for the analysis of
possible heat transfer effects in the radial direction.
Discharge under a current density of 0.1 A/cm2 .—As previously stated,
maximum operation time is estimated to be reached via one of three
possible scenarios: (1) the coldest cell average temperature reaching
400◦ C, (2) complete solidification of the electrolyte salt over the eu-
tectic line, (3) cathode ion-depletion; relevant times are provided in
Table III. Interestingly, the maximum operation time for this battery
is significantly longer than that of the 24-cell battery (see Table III),
especially when mass transfer resistance is small enough, so that a
scenario of cathode ion depletion (as occurs in the case of ω = 0.3) is
avoided.
It is interesting to note that, for this “wide” battery, the case of
ω = 0.3 is advantageous compared to that of the lower mass trans-
fer resistance (ω = 0.1) in terms of a slower cooling rate, as indi-
cated when looking at times it takes these batteries to reach 400◦ C
(Table III). This is probably due to the heat of fusion dissipated there
due to a somewhat enhanced change in molar composition, which
brings the system into zone 2 over the salt’s phase diagram (BEL)
earlier than in the case of ω = 0.1, and within it drives a faster change
in molar compositions.
The above mentioned advantage of the “wide” battery as compared
to the 24-cell system brings to light the importance of the cell-stack
surface area to volume ratio: 0.181, 0.159, and 0.142 [mm−1 ] for
the “base-case” 12-cell battery, 24-cell battery, and “wide” 12-cell
battery, respectively. As observed earlier, this significantly impacts
the stack’s cooling rate: note that the stack’s thermal mass in this
case of the “wide” 12-cell battery is the same as that of the 24-cell
battery and should therefore have no influence on differences between
cooling rates of these two batteries. Furthermore, this result supports
the earlier suggestion that the 24-cell battery operation time could
be dramatically extended with an optimized thermal design of heat
loss from the stack. Therefore, this “wide” 12-cell battery is clearly
superior to the 24-cell battery in terms of thermal performance in this
scenario in which its stack is electrically divided in two. However,
larger changes in Z toward the end of the “wide” 12-cell battery
operationh may compromise electrical performance and diminish the
advantage of the “wide” battery. Finally, note that the temperature
h
a maximum of 0.05 additional change in Z until final solidification in the case of ω =
0.1, compared with the 24-cell battery, as would be displayed in figures such as Fig. 5 for
each of these 2 cases (not shown here).

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 A358 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)
Figure 12. Minimum and Maximum temperatures in the cell-stack as a func-
tion of time for the 12-cell “wide” battery simulation for 1.0 A/cm2 current
density drawn and with (a) ω = 0.7 and (b) ω = 0.9.
differences within the stack in this case are observed to be even slightly
smaller than in the two previous case studies despite the increased
radial dimension associated with this battery.
Discharge under a current density of 1.0 A/cm2 .—The cause for pro-
cess termination remains unchanged in this case of large current den-
sity drawn, and battery thermal performance resembles that of the
12-cell “base-case” and 24-cell batteries with the same estimated bat-
tery operation time (see Table III). Looking at Fig. 12 as compared
with Fig. 9, only slightly bigger temperature gradients develop across
the cell (perhaps due to radial heat transfer). In addition, tempera-
tures are elevated throughout (the same) time of operation by a few
degrees Celsius; this could be attributed to the decreased stack sur-
face to volume ratio. As there were practically no differences between
the “base-case” 12 and 24-cell batteries in the event of large current
densities, it is reasonable to believe that the differences observed here
are due to the change in cell and stack geometry in the radial direc-
tion. Finally, note the sudden “drop” in stack minimum temperature
following ignition also in this case, supporting the previous claim it
is mostly related to the battery’s initially colder parts.
The base-case battery with special variations.— In this section,
we examine the impact of variations in design parameters and other
system variables on the discharge characteristics of the base-case 12-
cell thermal battery.
Thermal insulation thickness.—A significant advantage of using com-
puter simulations in thermal design of thermal batteries lies in the
ability to easily test changes in system geometry in a cost-effective
manner. This is especially relevant when considering changes in the
diameter of cell-stack disks, which are both time consuming and ex-
pensive to manufacture. To test this approach, we (virtually) assemble
and discharge a battery similar to the “base-case” 12-cell battery oper-
ated under a current density of 0.1 A/cm2 and with ω = 0.1. The only
difference involves the radial measures of the battery’s components.
Specifically, the thermal insulation wrapping the stack is increased
in thickness by 2 mm, at the expense of the stack’s exterior diameter
(which is decreased to 26 mm) (see Appendix A). To electrically com-
pensate for this change, the current density drawn from this battery is
enlarged by an appropriate factor in order to maintain the same over-
all current this battery supplies. Such a change in the design could be
considered in a case where one wishes to extend the battery operation
time while maintaining the same electrical performance. The trade-
off between an increased radial insulation thickness and an increased
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Figure 13. Temperature Trajectories, as viewed in a temperature-time plot,
of simulation results corresponding to the lowest electro-active cell cath-
ode center in the 12-cell “base-case” battery and variations (as described in
Table III) with 0.1 A/cm2 (except for “increased radial insulation”, 0.1344
A/cm2 ) current density drawn and with ω = 0.1; T = 5◦ C.
current densityi is to be investigated, with the constraint of keeping
the exterior measures of the battery unchanged. Results for this case
are displayed in Fig. 13 and Table III, and are further discussed below.
Salt-buffers.—“Salt-buffers” is a term used for non-electro-active so-
lidifying disks combined in the cell-stack in order to improve thermal
behavior and increase battery operation time.12 It is highly advisable
not to increase the stack’s initial temperature (using pyrotechnic ma-
terials) beyond a certain point due to material stability limitations. It
is however possible to increase the battery’s thermal energy density
(and thus its operation time) using salt-buffers which absorb energy
in the form of latent heat of fusion to be dissipated back into the
battery when it reaches these salts freezing points during battery cool-
ing. The energy required for melting the salt within the salt-buffers at
ignition is supplied by additional pyrotechnic disks combined in the
stack.
Here, we choose to use salt-buffers whose salt melts at 450◦ C
(about 100◦ C higher than the salts used in the electrochemical cells).
Remember that, in the specific materials systems considered here,
electrical resistivity may begin to increase significantly as the temper-
ature falls below 400◦ C, thus possibly decreasing the battery voltage
beneath a specified minimum threshold value. As demonstrated above,
this scenario is most relevant for thermal batteries with a relatively
low current density drawn (where heat transfer effects dominate bat-
tery operation time); it is for this reason that a current density of
0.1 A/cm2 and ω = 0.1 was chosen for this study.
The “base-case” 12-cell thermal battery model was altered by an
addition of 2 salt buffer disks at the bottom of the stack (the coldest
part by the analysis above) and 1 at the top, at the expense of thermal
insulation there (thus preserving overall battery volume). Additional
pyrotechnic disks were added to balance the extra heat required for
melting of the salt in the buffers and for keeping the cell stack’s initial
temperature (assumed homogeneous) as in the base case. Last, in
order to keep the battery exterior dimensions (as would be required by
product specifications) one other insulation above the cell stack was
also removed. All details for the battery involved in this case study
may be found in Appendix A. It is important to note that the model
described here (for the virtual batteries described above) was used
i
mostly accelerating battery cooling; see also the effect of heat of reactions and joule
heating below.
 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)
for the salt-buffers too, with the relevant material data, zero current
density applied within, and using T = 5◦ C. Results for this case are
displayed in Fig. 13 and Table III and are further discussed below.
External case design (flanges).—Additional metal flanges are some-
times required for mechanical support of the battery or as an interface
with the immediate environment. To test the possible impact of these
on heat transfer and resultant battery performance we simulate the
discharge of a modified version of the 12-cell “base-case” battery to
which an asymmetric (to the cell stack) external flange is added. The
impact of two different sized-flanges, both placed at the same loca-
tion, is examined. Similar to the previous two studies, we examine the
heat-transfer dominated case involving a current density drawn of 0.1
A/cm2 with ω = 0.1; full details of the batteries involved in this case
study are to be found in Appendix A. Results for these cases are also
displayed in Fig. 13 and Table III, and are further discussed below.
Stack initial conditions.—An important design goal is to have the
entire stack, including the thermal insulation disks on top and at the
bottom of electro-active disks within the main cylinder at a uniform
elevated temperature right after ignition. Failing to do so is suspected
to result in a much faster cooling than usual of these two cells, leading
to a decreased operation time. To examine this issue, we simulate
discharge of the “base-case” 12-cell battery with a current density
drawn of 0.1 A/cm2 and ω = 0.1, and with the pyrotechnic disks at
the bottom and top of the stack replaced by thermal insulators of the
same size (further details are given in Appendix A).
We estimate the impact of this change in the stack configuration to
lead to a decreased initial temperature (500◦ C) in the insulators below
and above the electro-active cells, where the rest of the stack remains
at 600◦ C as in all previous cases discussed here. It is important to note
that the IC solver combined in the simulator8 has enabled calculation
of this case of inhomogeneous initial conditions in the stack smoothly
and without any need for re-adjusting numerical parameters. Results
for this case are also displayed in Fig. 13 and Table III, and are further
discussed below.
The base-case battery with special variations.— results and
discussion.—The results for these variations of the “base-case” 12-
cell battery at low current density, presented in Fig. 13 and Table III,
reveal a number of design possibilities and considerations to be taken
into account.
First, it is shown that an imbalanced stack in terms of initial tem-
peratures may significantly reduce battery operation time. Therefore,
it is evident that combining pyrotechnic materials at the stack’s top
and bottom (exterior to the electro-active cells) is required to ther-
mally balance the different sections of the cell stack. Next, it is very
interesting to notice that the addition of a single and quite ordinary
metal flange may cause the same effect as that of an imbalanced stack,
emphasizing that simulation and/or experimental testing of a battery
must consider such features. Reviewing this case of an ordinary flange
together with that of an enlarged flange shows how a critical heat loss
could occur due to this design feature, leading to the suggestion that it
may be worthwhile to apply thermal insulation to the flanges. More-
over, since the flange’s tip is usually fastened onto a larger colder
device, thus causing a thermal “short-circuit”, thermally insulating
the flange’s tip may be of extreme importance. The benefit of proper
thermal design is also demonstrated when looking at the addition of
even a minimal set of “salt-buffers” to a low current-density battery.
A truly significant enhancement of the battery’s thermal performance
is obtained when using this attractive design feature.
Finally, it is most interesting to observe how increasing the thermal
insulation in the radial direction at the expense of the cells’ diame-
ter positively impacts heat transfer in the battery. Even though this
requires (as explained above) the drawing of an increased current
density from the battery, thus causing an increased heat consumption
per volume due to the endothermic heat of reactions, the increased
radial thermal resistance more than compensates for it. Furthermore,
this battery shows the best thermal performance above 400◦ C, where
below this temperature it is second only to the salt-buffer enhanced
battery. Finally, we emphasize that all these results were obtained for
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A359
Figure 14. Trajectories of simulation results corresponding to the lowest
electro-active cell cathode center in the 12-cell “base-case” battery for 0.1
A/cm2 current density drawn and with ω = 0.1 with/without (endothermic)
heat of reactions and with/without joule heating; T = 5◦ C.
cases involving a low current density, where heat transfer effects have
been shown to be crucially important.
Heat of reactions and joule heating.— Our last study involves the
“base-case” 12-cell battery structure with which we seek to investigate
the importance of heat dissipation in the stack caused by joule heating,
as well as battery cooling due to the endothermic heat of reactions.
The emphasis is on comparing results obtained for this multi-cell
system with those calculated for the case of a single cell battery. Two
extreme cases were studied: small current density drawn with low
mass transfer resistance (0.1 A/cm2 with ω = 0.1), and large current
density with a large mass transfer resistance coefficient (1.0 A/cm2
with ω = 0.9).
In the case of the low current density, time-temperature plots pre-
sented in Fig. 14 (and values noted in Table III) reveal a negligible
effect of the joule heating in the multiple-cell battery. On the other
hand, endothermic heat of reactions seems to play an important role
in the thermal performance of the battery, having a significant quan-
titative effect on its operation time. This is in contrast to the single
cell battery, which seems to be indifferent to both these phenomena in
terms of operation time measures as they are reflected in Table III. We
can conclude that heat loss from the surface of the single cell battery
dominates its rate of cooling, as compared with the multi-cell system
whose volumetric heat generation and consumption mechanisms are
more pronounced due to the difference in surface to volume ratio be-
tween the two systems. Finally, notice that during the last stage of
solidification (in zone 3 over the phase diagram, OEL) the latent heat
of fusion entirely dominates heat transfer in both single (not shown
here) and multi-cell systems, rendering the cell/stack temperature un-
changed throughout this stage.
Simulating the multiple-cell battery’s performance with large cur-
rent density drawn (and therefore large mass transfer resistance) yields
the temperature trajectories shown at Fig. 15. These reveal that in this
case joule heating does have some (albeit minimal) influence on the
battery’s thermal history. However, as process termination here is
determined by ion depletion at the cathode, the influence of joule
heating is only through decreased electrical resistivity, probably not
significant with the small gains in temperature observed in Fig. 15.
Heat of reactions again has a marked impact on heat transfer in
the full-scale battery, but as battery operation time (controlled by
mass transfer) is the same for all relevant cases (see in Fig. 15 and
 A360 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)
Figure 15. Trajectories of simulation results corresponding to the lowest
electro-active cell cathode center in the 12-cell “base-case” battery for 1.0
A/cm2 current density drawn and with ω = 0.9 with/without (endothermic)
heat of reactions and with/without joule heating; T = 5◦ C.
Table III), the effect is (again) through a reduced electrical resistivity
due to elevated temperatures throughout battery discharge. Finally, it
is important to note that results from the single-cell battery simulation
(see Table III) reveals similar behavior including the same cause for
process termination. Moreover, the single cell battery seems to be
completely indifferent to these phenomena in this case of large current
density drawn, too.
Conclusions
Our validated simulator for thermal design of high-temperature
molten-salt batteries, based on a two-dimensional mathematical heat
transfer model including the electrolyte phase-change and a simplified
supporting mass balance (presented in Ref. 8 and slightly modified
in this manuscript for improved consistency), has been used for the
analysis of a variety of case-studies of thermal battery designs. These
case studies demonstrate the simulator’s importance as a robust and
flexible tool for thermal design of multiple-cell batteries exhibiting
a considerable range of geometrical measures, current density drawn
and other scenarios.
Results presented in this manuscript lead to a set of useful conclu-
sions regarding the design of full scale, multiple-cell thermal batteries:
r Comparing single-cell and multiple-cell batteries, it is evident
that a multiple-cell battery design cannot rely on single cell analysis
alone, due to system level effects. Moreover, we demonstrate that
solidification dynamics are different in each of the electro-active disks
(i.e., anode, cathode, and separator) within a cell, thus requiring that
multiple cell analysis should also include details at the sub-cell level.
r At low current densities drawn, battery operation time is gov-
erned by heat loss of the cell-stack to the surroundings, which is found
to be dominated by the stack’s thermal mass and area to volume ratio.
A common scenario associated with the end of discharge at low cur-
rent density is the release of latent heat of solidification at the eutectic
temperature (OEL –zone 3), dominating heat transfer to the extent
that it renders the cell practically isothermal during this phase-change
process. Examining the effect of additional fundamental phenomena
in thermal batteries at small current densities, it seems that the heat
of reactions significantly impacts the cooling of the stack, while the
contribution of joule-heating to heat transfer is negligible.
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r At large current densities the system is dominated by mass
transfer effects leading to a battery operation time determined by ion
depletion in the cathode. This suggests that, under such conditions
(large iA values), thermal battery design should focus on mass trans-
fer optimization. During discharge, the latent heat of fusion has a
noticeable effect on heat transfer within the intermediate (BEL – zone
2) stage across the phase-diagram of the electrolyte. This, in turn,
slows the battery’s cooling process, thus moderating the associated
rate of electrical resistivity rise. In addition, the endothermic heat of
reactions in this case has a small (yet noticeable) effect on the thermal
behavior, though much larger than that of joule heating.
r In both cases of low and high current density drawn from the
battery, results show little sensitivity to the choice of the value for
ω within a reasonable range: small (close to 0) values of ω for low
current-densities, and large (close to 1) values of ω for high current-
densities. This is very useful in terms of using our model-based sim-
ulator for thermal design of thermal batteries, potentially making it
easier to estimate the value of ω (per current-density) via comparison
with either more exact mass-transfer electrochemical models or with
actual battery tests and measurements.
r When performing scale-up of a multiple-cell thermal battery in
terms of the voltage and/or current to be supplied, design parameters
are subject to certain constraints (e.g. battery geometry and weight).
It seems that under conditions of small current densities, a reduced
surface to volume ratio of the cell-stack (at the same thermal mass) is
a desirable design feature, as seen in the “base-case” 12-cell battery,
24-cell battery and “wide” 12-cell battery models analyzed in this
manuscript. In the case of large current densities, as noted, thermal
battery design should mainly lean toward mass transfer optimization.
In this case, only some marginal gain can be expected when increasing
stack geometry in the radial direction. This is because heat loss to the
surroundings is not as dominant as other phenomena in this scenario.
r Special variations/additions to a specific thermal battery design
may prove to significantly impact its performance. During discharge
at low current density, it was found that:
– A non-uniform initial temperature field in the stack may com-
promise thermal design.
– Radial heat transfer effects are significant.
– “Salt buffers” are an efficient feature useful in extending thermal
battery operation time.
– Addition of external case objects such as flanges has a crucial
effect on heat loss from the battery (and, thus, its operation time),
suggesting that selective thermal insulation of these objects should
significantly enhance battery performance. This is especially im-
portant when such an object (e.g. a flange) is attached to an external
cold object thus thermally short circuiting the battery.
Finally, to the best of our knowledge, this is the first time in which
such a comprehensive analysis, accounting for extensive thermal de-
sign parameters, is being presented for thermal batteries. We believe
that this is enabled due to the use of verified mathematical models,
involving the significant physical phenomena for thermal analysis and
design of thermal batteries. Of no less importance is the fact that these
models are incorporated into a versatile, portable and robust simu-
lation tool, easily applicable for the analysis and design of thermal
batteries.
Acknowledgments
N. Haimovich thank the Sylvia Rose Fine fellowship, the George
Feldenkreis and family fellowship, and the Irwin and Joan Jacobs
fellowship for their kind financial support.
Appendix A: Thermal Batteries Geometrical and Material
Property Data Details
The 12-cell “base-case” battery model of external cell diameter of φ = 30 mm
presented in Fig. 1 (and, also, in Fig. 2a) involves 12 electro-active 4-disk cells, of the
 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015) A361

Table AI. Additional Material Property Data of non-electrochemically active materials.

Battery Part Property Data

Pyrotechnic Disk k 6.65685E-03-3.19476E-05×T+8.26475E-08×T2 –9.12458E-11×T3 +3.62392E-14×T4
ρ 3.40600E-03+0.00000E+00×T+0.00000E+00×T2 +0.00000E+00×T3 +0.00000E+00×T4
Cp 5.45707E-01-1.11251E-03×T+4.95898E-06×T2 –6.59480E-09×T3 +3.22165E-12×T4
R (irrelevant in the case studies involved in this manuscript)
Insulation Layer B k 1.21287E-04-7.34383E-07×T+2.10356E-09×T2 -2.55184E-12×T3 +1.13554E-15×T4
ρ 3.30000e-4+0.00000E+00×T+0.00000E+00×T2 +0.00000E+00×T3 +0.00000E+00×T4
Cp 1.19009E+00–1.48771E-03×T+2.74005E-06×T2 -1.29849E-09×T3 +0.00000E+00×T4
Insulation Layer C k 1.17483E-04-3.67789E-07×T+6.67190E-10×T2 –4.30562E-13×T3 +1.24181E-16×T4
ρ 1.76000e-4 +0.00000E+00×T+0.00000E+00×T2 +0.00000E+00×T3 +0.00000E+00×T4
Cp 1.13000E+00+0.00000E+00×T+0.00000E+00×T2 +0.00000E+00×T3 +0.00000E+00×T4

same geometrical details and material property data discussed in Ref. 8, except for an
external cell radius of 15.0 mm (instead of 17.5 mm in Ref. 8).
The “bottom stack disks” (see Fig. 1) include 5 non-electro-active disks (in which
electrical current does not flow) of the same internal and external radius. These disks’
axial thicknesses, from bottom to top, are:
1. Insulation Layer A – 1.0 mm.
2. Pyrotechnic Disk– 0.75 mm.
3. Insulation Layer A– 1.0 mm.
4. Pyrotechnic Disk– 0.75 mm.
5. Insulation Layer A – 1.0 mm.
Material Property Data temperature/concentration dependent correlations used in
the simulations for “Insulation Layer A” are the same as those used for the insulation
layers in Ref. 8 whereas Material Property Data for the “Pyrotechnic Disk(s)” is given in
Table AI; note that the latter are different from the disks combined in the electro-active
cells (where metal is combined at their bottom). Units used in this table are: [T] = [K];
[k] = [W/mK]; [ρ] = [kg/m3 ]; [Cp ] = [J/kgK].
The “top stack disks”" (see Fig. 1) consist of 2 non-electro-active disks of the same
internal and external radius as the previous group also. These disks’ axial thicknesses,
from bottom to top, are:
containing 24 serially connected similar electro-active cells in the axial direction instead
of 12.
The “wide” 12-cell battery of external cell diameter of φ = 42.13 mm is similar to the
12-cell “base-case” battery of external cell diameter of φ = 30 mm, except for the external
stack diameter (i.e., all disks within, including the “top” and “bottom stack disks” which
are non electro-active) and resultant changes in the geometrical measures of the insulation
layers and sealing case so that their original thicknesses perpendicular to the stack in each
of the axis (r,z,) remain unchanged. For further clarity, this battery’s geometrical model
is displayed in Fig. 2c.
The thermal battery geometrical model for the 12-cell “base-case” battery special
variation: “thermal insulation thickness effect” involves the same geometrical and material
property data details as in the 12-cell “base-case” battery model (shown in Fig. 1), except
for two changes. The “internal radial insulation” layer radial thickness is increased by
2.0 mm, and therefore the stack (and all disks within) external diameter is set to 26.0 mm
(its radius decreased by 2.0 mm).
The thermal battery geometrical model for the 12-cell “base-case” battery special
variation: “salt buffers” involves the same geometrical and material property data details
as in the 12-cell “base-case” battery model (shown in Fig. 1), except for three changes.
The “bottom stack disks” (as in Fig. 1) is replaced with the following configuration of 7
non-electro-active disks of the same internal and external diameter as the rest of the stack
(φ = 30 mm), and with disks’ axial thicknesses from bottom to top:

1. Insulation Layer A – 1.0 mm. 1. Insulation Layer A – 0.5 mm.

2. Pyrotechnic Disk– 0.75 mm.
Material Property Data used in model calculations for these disks is the same as that
used for the “bottom stack disks”, respectively.
The “bottom annular disks” marked in Fig. 1 involve 2 non-electro-active disks of the
same internal radius as of the stacks’ disks (2.5 mm), and an external radius of 16.0 mm.
These disks’ axial thicknesses, from bottom to top, are:
1. Insulation Layer B – 0.6 mm.
2. Insulation Layer A – 1.0 mm.
Material Property Data for “Insulation Layer B” is also summed in Table AI.
The “top annular disks” within this battery configuration (see Fig. 1) consist of 3 non-
electro-active disks of the same internal radius as of the stacks’ disks (2.5 mm), and an
external radius of 17.5 mm; all 3 disks are of an axial thickness of 1.0 mm each, and utilize
Material Property Data of “Insulation Layer A”. The “top battery disks” (Fig. 1) consist
of 2 non-electro-active disks of zero internal radius (non-annular disks), and an external
radius of 17.5 mm; both disks are of an axial thickness of 2.0 mm each, and utilize
Material Property Data of “Insulation Layer A” also. The “bottom battery disks” (see
Fig. 1) consist of 3 non-electro-active disks of zero internal radius (non-annular disks),
and an external radius of 17.5 mm; all 3 disks are of an axial thickness of 1.0 mm each, and
utilize Material Property Data of “Insulation Layer A”, too. The “internal”, “external”,
and “top external radial insulation” layers geometrical measures could be derived from
the other bodies’ measures given above; all 3 layers utilize Material Property Data of
“Insulation Layer C” (summed in Table AI, too). The “igniter”, and “pyrotechnic cylinder”
(Fig. 1) layers geometrical measures could also be derived from the other bodies’ measures
given above; Material Property Data used in the simulations for these 2 bodies are the
same as those used for them in, Ref. 8 respectively. A 1.5 mm thick external (battery)
“case” (see Fig. 1) seals this internal battery configuration; Material Property Data used
in the simulations for the case is the same as was utilized in, Ref. 8 including external
convection and radiation coefficients.
The 24-cell battery model of external cell diameter of φ = 30 mm presented in
Fig. 2b (and discussed in the Results and Discussions section) follows the same description
as the 12-cell “base-case” battery of external cell diameter of φ = 30 mm, except for
2. Pyrotechnic Disk– 0.75 mm.
3. Salt Buffer – 1.1 mm.
4. Pyrotechnic Disk– 0.75 mm.
5. Salt Buffer – 1.1 mm.
6. Pyrotechnic Disk– 0.75 mm.
7. Insulation Layer A – 1.0 mm.
Material Property Data used for “Insulation layer A” and “Pyrotechnic Disk(s)” is
the same as in their original groups. Material Property Data temperature/concentration
dependent correlations used for the salt buffer disks (which are non electro-active) are the
same as those used in the separator disks within the electro-active cells, with the exception
of Teu = 450◦ C = 723 K (but with the same T = 5◦ C). In addition, the “top stack disks”
group (as in Fig. 1) is replaced with 2 non-electro-active disks of the same internal and
external diameter as the rest of the stack (φ = 30 mm), and with disks’ axial thicknesses
from bottom to top:
1. Salt Buffer – 1.1 mm.
2. Pyrotechnic Disk– 0.75 mm.
Material Property Data used in model calculations for these disks is the same as that
used for the (replaced) “bottom stack disks” group, respectively. Finally, 1 of the 3 disks
in the “top annular disks” group (as in Fig. 1) is removed in order to maintain the same
battery external measures in the axial direction (up to 0.05 mm) as would have been
specified within the original design constraints.
The thermal battery geometrical models for the 12-cell “base-case” battery special
variation: “exterior case object (flange) addition” involve the same geometrical and ma-
terial property data details as in the 12-cell “base-case” battery model (shown in Fig. 1),
except for an external addition to the case geometry (of the same material property data) in
two separate cases: small and large flange - at the (battery) case’s lower and radially exter-
nal corner. The geometrical details for each flange configuration are presented in Fig. A1.
The thermal battery geometrical model for 12-cell “base-case” battery special varia-
tion of “inhomogeneous stack initial conditions” also involves the same geometrical and
material property data details as the 12-cell “base-case” battery model (shown in Fig. 1),
except for the use of the “Insulation Layer A” Material Property Data in the pyrotechnic

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 A362 Journal of The Electrochemical Society, 162 (3) A350-A362 (2015)

r radial coordinate; [m] or [mm]

T temperature; [K] or [◦ C]
Teu temperature at the eutectic point; Teu = 355◦ C (for LiCl-KCl)
t time; [s], or [min]
U potential of an electrode reaction at equilibrium; [V]
V volume; [mm3 ], [cm3 ], or [m3 ]
w mass fraction of the liquid phase within the electrolyte (salt); [ ]
X mole fraction of the binary salt first species (e.g., LiCl) in the liquid phase; [ ]
Xeu mole fraction of the binary salt’s first species at the eutectic point; Xeu = 0.585
(for LiCl-KCl)
Z mole fraction of the binary salt’s first species (e.g. of LiCl); [ ]
z axial coordinate; [m] or [mm]

Greek
χ mass fraction of electrolyte within the combined electrolyte, matrix and binder
phase; [ ]
ε emissivity; [ ]
φ electro-active cell(s) external diameter; [mm]
ρ mass density; [kg/m3 ]
ρsalt mass density of molten salt; [kg/m3 ]
ω mass transfer resistance coefficient for an electrochemical cell component (e.g.,
cathode); [ ]
ξ fraction of cross-section area available for charge transfer in cell component
(e.g., cathode); [ ]
Hfus binary salt’s heat of fusion per unit mass; [J/kg]
T artificial temperature difference below eutectic line, representing the mushy
region there, as defined in Ref. 8, [K] or [◦ C]
t infitisimal time-step; [s]

Subscripts
0 initial (at time zero)
1 binary salt first species (e.g., LiCl)
2 binary salt second species (e.g., KCl)
A density per unit area
eu eutectic
fus fusion
J-h joule heating
Figure A1. Geometrical model of the twelve-cell “base-case” thermal-battery rxn reaction
with an external cell diameter of φ = 30 mm with (and zoomed to) an exterior V density per unit volume
case object (flange) addition: (a) (small) flange (b) larger flange.
References
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#F Faraday number; F = 96,487 C/mol (2008).
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transfer (positive value); [A/m2 ] or [A/cm2 ] 110, 267 (2002).
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charge transfer multiplied by either 0 in the separator, +1 in the anode or −1 (2009).
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in the cathode; [A/m3 ] or [A/cm3 ]
875 (1990).
k thermal conductivity; [W/mK] 10. M. Bhattacharya, T. Basak, and K. G. Ayappa, Int. J. of Heat and Mass Transfer, 45,
Mj molecular weight of species j; [kg/k-mol] 4881 (2002).
-Qrxn heat of reactions (per unit time per unit volume); [W/m3 ] 11. A. J. Bard and L. R. Faulkner, Electrochemical Methods, 2nd ed., Wiley (2001).
R electrical resistivity; [m] 12. O. Shalev and D. R. Dekel, in 43rd Power Sources Conf. Proc., 20.1, p. 417 (2008).

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