21606_01d

Ch01-N52160.fm Page 40 Wednesday, December 27, 2006 12:36 PMCh01-N52160.fm Page 40 Wednesday, December 27,2006 12:36 PM

40 G. Pistoia

electrolyte onto a current collector or loading the material into a honeycombmatrix [48]. Graphite may be included and, sometimes, CoS2 and NiS2 are alsoadded.

The bipolar cell configuration is preferable over the monopolar one. Anexploded view is shown in Figure 1.31(a). The electrodes are of high surfacearea and the cell design is compact, also thanks to the use of starved electrolyteand MgO separator, this resulting in a higher power output. The presence of thetwo-phase alloy at the negative electrode ensures tolerance to overcharge, sothat the state of charge of all cells can be equalized. Indeed, the alloy (LiAl+Li5Al5Fe2) has a sufficiently high Li activity towards the end of charge to causesolubilization of Li metal in the molten-salt electrolyte; Li can be reoxidized atthe positive, thus giving rise to a shuttle mechanism [48].

The design criteria to be met for an efficient bipolar stack are [48]:1. Provision for an equalized state of charge of the cells in series, as mentioned

above.2. The use of a starved-electrolyte regime and a MgO separator. This is made

possible by using the Li-rich LiCl-LiBr-KBr electrolyte that has aconductivity, in the starved configuration, equivalent to that of the LiCl-LiBr eutectic in the flooded configuration. Furthermore, in these conditionsthe corrosion is limited.

3. The use of effective seals. Bipolar cells are more difficult to seal thanmonopolar cells. This problem was solved by introducing the chalcogenideseal mentioned above. For cells with FeS2 cathodes, a steel-ceramic-molibdenum seal was found adequate.

Several prototypes of bipolar Li-Al/FeS* batteries were manufactured inthe early 1990s. Such cells (diameter: 130 mm, weight: 250 g) could deliver 25Ah at the C/5 rate, as shown in Figure 1.31(b). The specific energy and powervalues of cells (not batteries) are presented in Table 1.7 [49]. In terms of energy,both cells meet the mid-term USABC's target (80-100 Wh/kg) and the Li/FeS2

cell approaches the long-term target (200 Wh/kg). However, it has to be notedthat the above targets refer to fully engineered batteries. The specific power ofthe Li/FeS2 cell is very interesting. Indeed, the mid- and long-term values set bythe USABC are 150-200 W/kg and 400 W/kg, respectively. Other positive

Table 1.7. Performance characteristics of bipolar Li-Al/FeS* cells. The data do not includethermal enclosure. {From Ref. 49)

Cell Type

Li-Al/FeS2

Li-Al/FeS

Specific Energy(Wh/kg)

180 at 30 W/kg130 at 25 W/kg

Specific Power at 80%DOD (W/kg)

400240

Previous Page


Nonaqueous Batteries Used in Industrial Applications 41

features of this system are: good cyclability (in excess of 1000 cycles),tolerance to overcharge and overdischarge and to freeze-thaw cycles.

Sealed modules with a nominal voltage of 25 V and a capacity of 60 Ahhave been fabricated from prismatic bipolar cells [49]. They have a specificenergy of 75 Wh/kg and an energy density of over 200 Wh/L, and can be cycledfor many hundreds of deep discharge cycles. It is noteworthy that failure ofthese modules occurs via short circuits when they reach the end of life.However, series stacks remain operational after the loss of one or more cells:the loss of energy, in this case, is limited to the energy content of the failedcell(s) [50].

The advantages of the Li-Al/FeS* system can be summarized as:• Simple modular design and construction• High energy - at least twice that of lead-acid batteries• High power• Long cycle life• Heat management not requiring auxiliary heating or cooling during use• Safe, even under severe abuses

The Li-Al/FeS* system shows an improved safety over sodium/sulfur(see Sub-section 1.3.3.1), while with respect to sodium/nickel chloride (seeSub-section 1.3.3.2) it has a higher specific power (but less safety). On the otherhand, a couple of disadvantages are evident: a) as any other thermal battery,stored energy is consumed to keep the cell warm during standby periods, and b)the bipolar design is likely to have manufacturing problems and high costs.

The remarkable advancements made with this systems suggested to theUSABC to select it as the long-term battery to be developed for electric vehicles.However, in the mid-1990s the R&D efforts were discontinued also in view ofthe new technologies based on Li-ion and Li-polymer batteries. Indeed, thesetechnologies have power and energy outputs similar to that the Li-Al/FeS2battery, but can operate at much lower temperatures. This system remains aviable candidate for stationary energy storage [50].

Development of the Li/iron sulfide system is continuing, but moltensalts electrolytes have been replaced by polymeric electrolytes. An example,with a composite electrolyte based on PEO, has already been mentioned (seeRfifs. [37,38]).

1.3.3. Batteries with a Sodium Electrode

High-temperature batteries based on sodium as a negative electrode,sulfur or NiCl2 as a positive, and /?"-Al2O3 as a Na+-conducting solidelectrolyte are now used for energy storage applications and are receiving


42 G. Pistoia

attention for EV and space applications. The theoretical specific energies of theNa/S system (760 Wh/kg) and Na/NiCl2 system (796 Wh/kg) are much higherthan those of the aqueous systems (Pb/Acid and Ni/Cd) thus far used forenergy storage.

1.3.3.1. Sodium/Sulfur Batteries

Investigations on this battery date back to the early 1970s and wereoriented for several years to motive applications. However, technical andeconomic issues have suggested switching to large battery packs for stationaryapplications. Indeed, the Na/S battery has distinct advantages over othertechnologies, such as high energy and good power density, high cycle life, highenergy efficiency, independence from external temperature, and moderate cost.

The operating temperature of this system is between 310 and 35O°C. Inthis temperature range, both Na and S are liquid, while the solid electrolyte hasa high Na+ conductivity, thus ensuring good kinetics.

During discharge, Na+ migrates from Na to S and forms polysulfides, asindicated in Figure 1.32. The first plateau corresponds to the coexistence oftwo immiscible liquids, S and Na2S5; in the single-phase sloping section, thesulfur content of the polysulfide decreases down to Na2S2.7; the secondplateau corresponds to the formation of Na2S2 [51], but is never reached inpractical cells. Indeed, formation of Na2S3, at 1.78 V, is taken as the dischargelimit. Complete discharge would cause corrosion and local overdischarge due tonon-uniformities in temperature and DOD. At the C/3 rate, the average voltageis 1.9 V.

o 1,8

1,6

1,4

2 ,076 V

1,74 V

Na2S5

20 40 60 80 100 120

State of discharge ( % w.r.t. Na2 S3

140

Figure 1.32. OCV of aNa/S cell at 350°C. (From Ref. 51)

Electrons

SealsLoad

+ –

Celldischarging

Insulator

Sodiumelectrode

Current-collector

Safety can

Beta-aluminaelectrolyte

Metering hole

Sodium ions

Sulfur electrode

Outer case



During charge, the reactions described above are reversed and in thefinal stages there is a marked resistance increase due to the insulating characterof sulfur. Therefore, the charge has to be stopped before complete Na recovery,and subsequent discharges provide 85-90% of the theoretical capacity [52].

As already mentioned, this system has a high cyclability (up to 5000-6000 cycles). This is mainly due to the liquid state of reactants and products: theaging mechanism based on morphological changes of the electrodes is notoperating here.

A scheme of a Na/S cell is shown in Figure 1.33 for the commonconfiguration with the central sodium electrode. An essential pre-requisite forthis electrode is high purity, i.e. other metals and Na compounds are notallowed. Contaminants tend to concentrate at the interface with the electrolyte,reducing the electrode active area or even causing its failure [48].

In order to minimize cell resistance, molten sodium has to properly wetthe electrolyte surface. This requires a smooth surface, a proper temperaturerange (300-350°C) and the absence of impurities. The sodium electrode iscontained in a metal (safety) can that restricts, through the metering hole, theflow of sodium to the electrolyte, thus reducing the amount of Na that maycome into direct contact with S in case of tube failure.

The sulfur electrode is impregnated into a layer of carbon or graphitefelt. The carbon fibers ensure a good electronic conductivity, as sulfur is an

©Celldischarging

rzt-e©Insulator

Sodiumelectrode

Current-collector

- Safety can

Beta-aluminaelectrolyte

Outer case Metering hole

Figure 1.33. Schematic of cross-section of the Na/S cell. (From Ref. 48)


44 G. Pistoia

insulator for both electrons and ions. Fortunately, Na polysulfides are goodionic conductors.

The electrolyte is /?"-Al2O3, which has a negligible electronicconductivity and is impermeable to molten Na and S. Its basic structural unity isa spinel-like slab formed by 4 layers of close-packed oxygen ions in a cubicstacking. The slabs are separated from each other by oxygen bridges. Thesodium ions move in the space between these slabs. The idealized compositionof yfl"-Al2O3is Na2O5.33Al203 or Na6Al32[Vac]A1

3+05i, with a vacancy of Al3+

in the spinel block that is balanced by 3 Na+ in the conduction plane. Thisresults in high conductivity. Pure /?"-Al2O3 is not easy to prepare, so it has to bestabilized with Mg or Li ions that substitute for Al ions. Typical compositionscontain 4.0 wt% MgO or 0.7 wt% Li2O.

The conductivity of this electrolyte is -0.5 ohnf'cm"1 at 350°C for thepolycrystalline form. However, /?"-Al2O3 is rather sensitive to moisture, thisfavoring deterioration of its mechanical properties. Therefore, some /?-Al2O3

(idealized formula, Na2OllAl203) is enclosed in the mixture, in spite of itslower conductivity, as it is less hygroscopic. A conductivity of ~0.2 ohm~'cm"1

is regarded as acceptable for practical electrolytes [48].Production of Na/S batteries for stationary applications is particularly

active in Japan. Table 1.8 presents the basic characteristics of some cells.In Figure 1.34, three single cells and the module constructed with the

largest one are shown [53]. Different modules are presented in Table 1.9, forapplications connected with energy networks (see footnote). Very large energy-storage systems can be built with these modules: their storage capacity may beas high as 57.6 MWh (see Figure 1.35) [54]. A comparison of different energystorage systems, including various batteries, pumped hydro storage, compressed

Table 1.8. Characteristics of stationary Na/S cells {From Ref. 52)

Manufacturer

CellDesignationCapacity, AhDiameter, mmLenght, mmWeight, kgEnergyDensity, Wh/LSpecificEnergy, Wh/kgPower Density,W/L

NGK

T4.1

160623752

285

160

36

NGK

T4.2

248683902.4

340

202

43

NGK

T5

632915155.4

370

226

46

Yuasa

17664

4302.7

240

120

60

Hitachi

28075

4004

300

133

Electric HeaterDry Sand

Fuse

Heat Insulated Container(Lower)Cell

Main Pole

Heat Insulated Container (Upper)

T4.2T4.1

T5

518

390

375

6891

62



Dry Sand Heat InsulatedElectric Heater Fuse Container (Upper)

Main PoleHeat Insulated Container

C e l l (Lower)

Figure 1.34. Na/S cells (left) and module (right). The module is built with 384 T5 cells and has anenergy of 421 kWh (energy density, 170 Wh/L) and a power of 52.6 kW. (From Ref. 53)

Table 1.9. Na/S modules for stationary applications. (From Ref. 52)

Manufacturer

BatteryDesignationPrimeApplication*Number ofCellsCapacity, AhEnergy, kWhVoltage, VVolume, LWeight, kgSpecificEnergy, Wh/kgEnergyDensity, Wh/L

NGK

12.5 kW

LL;PS;PQ

336

2280105489411400

75

112

NGK

25 kW

LL;PS;PQ

480

227221196

14482000

105

145

NGK

52 kW

LL;PS;PQ

384

3624421128

24813620

116

170

Yuasa

25 kW

LL

320

140810080

10861700

59

92

Hitachi

12.5 kW

Renew

216

290100144

25921900

53

40

' LL: utility-based load leveling; PS: peak shaving; PQ: power quality; Renew: renewable energy hybrid

air storage, and superconducting magnetic storage, has shown that the Na/Sbatteries have the highest energy densities [55]. They can live in this applicationfor up to 15 years providing thousands of cycles. (See also Chapter 8).

All development of Na/S batteries for EV applications was stopped by


46 G. Pistoia

Figure 1.35. 57.6 MWh (8 MW) battery installed in Japan for load levelling by NGK. (From Ref.54)

mid-1990s. Two companies (Asea Brown Bovery in Germany and Silent Powerin the U.S.A.) were especially involved in this field. The properties of the cellsdeveloped by these companies are compared in Table 1.10 with those of an

cell developed by the Swiss company MES-DEA.

1.3.3.2. Sodium/Nickel Chloride (Zebra) Batteries

This battery bears some analogies with the Na/S battery. The negativeelectrode and the electrolyte are the same, but a metal chloride is used instead of

Table 1.10. Comparison of cells with Na as a negative electrode for EV applications. (From Ref.52)

Manufacturer

Cell DesignationChemistryCapacity, AhElectrolyte ShapeDiameter, mmLenght, mmWeight, gResistance, ohmSpecific Energy,Wh/kgSpecific Peak Power,W/kg*

Asea Brown Boveri

A04Na/S

38cylindrical

35220410

6

176

390

Silent Power Ltd

PBNa/S10.5

cylindrical444512032

178

250

MES-DEA

ML3Na/NiCl2

32cruciform

36.52327156-20

116

260

• At 2/3 OCV and 80% DOD



sulfur as a positive electrode. As the initial research was carried out in SouthAfrica for EV applications, the acronym Zebra (Zero Emission BatteryResearch Activity) is often used [52].

Preferred material for the positive electrode is NiCU, but FeCl2 has alsobeen studied. During normal discharge, Ni and NaCl are formed, as shown bythe scheme of Figure 1.36. The voltage, 2.58 V, is higher than that of Na/S,2.06-1.78 V (see Figure 1.32). Other differences will be remarked in thefollowing description.

A schematic of this cell (Figure 1.37) shows that liquid Na is placed inthe outer part, while in practical Na/S cells it is in the central part. Furthermore,Na is not initially included in the cell assembly, but produced in situ duringcharge, as the cell is assembled in the discharged state. The positive electrode issolid and this would pose problems, as the solid-solid interface with theelectrolyte would not allow high currents. Therefore, a second electrolyte,NaAlCl4, which is liquid at the operating temperatures, is added. Inside the /?"-A12O3 tube, a compact mix of Ni metal and NaCl is inserted, and moltenNaAlCU is then poured to form a narrow annulus between the positive electrodeand the electrolyte. The presence of the second electrolyte lowers the specificenergy of the ZEBRA battery by -10% [56].

The tolerance to over-charge and over-discharge is outstanding byvirtue of the reversible reactions occurring in these segments (see Figure 1.36).On over-charge, NaAlCLt further chlorinates the Ni matrix, while on over-discharge excess Na reacts with the liquid electrolyte. This feature has apractical implication: it is possible to connect in series several cells, withoutparallel connections, as cell imbalances are leveled out by the above reactions.

3.05

w 2 .58-o>B"5

1.58-

2Na + 2AICI3 + NiCI2<=* N» + 2NaAlCI4

Overcharge| 2Na + NiClj <=> Ni • 2NaC!

Norma!operation

<=* 4NaCJ + Al

Overdischarge

100 0State-of-charge / %

Figure 1.36. Equilibrium voltage vs. state of charge of Na/NiCl2 cell at 250°C. (From Ref. •


48 G. Pistoia

NaAICI4

. fi-alumina tube

Porous M, MCI2 electrode

Liquid sodium

Cell case

Figure 1.37. Schematic of sodium/nickel chloride cell. (From Ref. 48)

Another advantage of this battery, with respect to the Na/S system, isrepresented by its enhanced safety. If the electrolyte tube cracks, molten Nareacts first with NaAlCU, according to the reaction of Figure 1.36. The resultingAl metal shorts the cell, while NaCl tends to plug the crack. Therefore, in abattery with a series of cells, the shorted cell does not cause failure of the all

Figure 1.38. Cross-section of a conventional ZEBRA cell (left) and a high-power cell (right).(From Ref. 48)



battery [56].As a further advantage, the Zebra cell can work in a wider temperature

range, i.e. 220-450°C, although the practical range has to be restricted to 270-350°C.

To improve the battery capacity and energy, cells with a square sectionmay be constructed, as this greatly reduces the dead space typical of batteriesassembled from cylindrical cells. Specific energies of 120-130 Wh/kg arepossible.

A limitation of the conventional design is the increasing resistance withDOD, this lowering the power capability. A convenient way to overcome thislimitation is designing the ceramic electrolyte with the cruciform shape ofFigure 1.38. The tube so obtained, termed a "monolith", allows the constructionof thinner and less resistive positive electrodes. To further decrease theresistance, Fe-doped NiCl2 is used. As a result, the cell's specific power mayreach 260 W/Kg at 80% DOD (Table 1.10), and batteries with a specific powerof 150 W/kg (the USABC's mid-term target for EV) have recently been built.

The Zebra system is specifically intended for EV applications. Asshown in Table 1.10, it has lower specific energies (but the gap is reduced on avolumetric basis) and powers than Na/S cells. However, it is preferred for EVapplications thanks to such factors as safety, easiness of construction,cyclability (more than 1000 cycles), low corrosion, etc.

Some specific applications have recently been proposed: in photovoltaicsystems, for instrumentation packs in oil exploration, and in hybrid cars alsocontaining a PEM fuel cells. In this latter application, two 40-kW Na/NiCl2batteries are coupled to a 6-kW fuel cell. Using this hybrid architecture allowsdoubling the EV range from 120 km to 240 km [57].

1.3.4. Basic Parameters of Secondary Nonaqueous Batteries

In Table 1.11, relevant data of the secondary batteries dealt with in thischapter are summarized. Due to the continuous evolution of these batteries,especially Li-ion and Li-polymer, the data have to be considered with somecaution. Caution is also necessary in view of differences in batterysize/configuration and test conditions.

Ch01-N

52160.fm Page 50 W

ednesday, Decem

ber 27, 2006 12:36 PM

Table 1.11. Characteristics of non-aqueous secondary batteries.

8I*

System

Li-ion

b, stationary(L

iNi07C

o03O

2)L

i-ion", EV

(LiN

i i .x_vC

oxM

nvO

2)L

i-ionb, stationary

(Li1+xM

n2O

4)L

i-ionb,E

V(L

iCrxM

n2.xO

4)

Li m

etal-polymer b

Li/FeS

c

Li/FeS

2 c

Na/S

c

Na/N

iCl2 c

Voltage

Range(V

)

4.0-2.8

4.0-2.8

4.0-3.0

4.0-3.0

3.0-2.0

1.7-1.02.0-1.5

2.0-1.8

2.1-1.7

Operating

Tem

perature(°C

)

-20-^60

-20-50

-20^60

-20-50

40-60"60-80

3

375-500375-450

300-350

250-300

Cycle

Life

(cycles)

9001

570

12001

580

80010001000

6000

2500

SpecificE

nergy(W

h/kg)

128

150

122

155

140'120

3

130180155'175

3

115

Energy

Density

(Wh/L

)

197

252

255

244

174'160

3

220350300'350

3

190

SpecificP

ower

(W/kg) a

490

440

260240400

2503

260

Ref.

23,58

23,58

23,58

23,58

39,4241,46

2,50,582,50,58

2,522,522,58

a. pulse discharge, b. battery; c. cell1. single cells; 2. stationary applications; 3. E

V

I



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