materials processing for li-ion batteries_pdf

8/19/2019 Materials Processing for Li-Ion Batteries_pdf

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Review Materials processing for lithium-ion batteries

Jianlin Lia, , Claus Daniela,b, David Wooda∗

a Materials Science and echnolog! Division, "a# Ridge $ational Laborator!, "a# Ridge, $ %&'%(-)*'%, +nited States b

Department of Materials Science and ngineering, +niversit! of ennessee, no.ville, $ %&//), +nited States

a r t i c l e i n f o0rticle histor!1 Received 2/ September 2*(* Received in revised form 2' "ctober 2*(* 0ccepted ( $ovember 2*(* 0vailable

online / $ovember 2*(*

e!words1 Lithium-ion batter! Materials processing Cathode 0node Separator

a b s t r a c t

.tensive efforts have been underta#en to develop and optimi3e new materials for lithium-ion batteries to address power and

energ! demands of mobile electronics and electric vehicles4 5owever, the intro- duction of large-format lithium-ion batteries is

hampered b! high cost, safet! concerns, and deficiencies in energ! densit! and calendar life4 0dvanced materials-processing

techni6ues can contribute solutions to such issues4 7rom that perspective, this wor# summari3es the materials-processing

techni6ues used to fabricate the cathodes, anodes, and separators used in lithium-ion batteries4

8 2*(* lsevier 94:4 0ll rights reserved4

Contents

(4 ;ntroduction 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4

4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 2rocessing for electrol!tes 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4

4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 2rocessing for electrode

fabrication 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4

4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 2


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-mail address1 lirocessing research and

development intended to improve performance can also affect the cost of fabrication4 ;n 2***, the cost Elabor and overheadF for a(',)=* cell was estimated to be G*4


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J4 Li et al4 I Journal of >ower Sources (/) E2*((F 2


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2. Processing for electrolytes

0n electrol!te for lithium-ion batteries should be able to dis- solve and dissociate into the solvent s!stem, and the Li ions

should be able to diffuse in the s!stem with high mobilit!4 Conventional electrol!tes consist of lithium salts dissolved in organicsolvents ?=@4 >rop!lene carbonate E>CF has attracted attention ?),&@ due to its high dielectric constant, the wide temperature range

of its li6uid phase, and its compatibilit! with lithium ?)@4 5owever, a solid electrol!te interface ES;F film cannot be formed on>C- based electrol!tes because the >C tends to intercalate with lithium ions into the graphite anode, resulting in continuous

decomposition and severe e.foliation of graphite la!ers ?(,'@ and a large irreversible capacit! loss during the initial c!cling?/,(*@4 Man! attempts have been made to improve the compatibilit! of >C with graphite b! introducing additives, such as

vin!lene carbonate ?((@, but!l meth!l carbonate ?(2@, or trieth!l orthoformate to the electrol!tes ?(%@4 he additives form an S;

la!er at poten- tials higher than (: vs4 ELiILiAF before >C begins to decompose ?(C ?/,(*@, dietho.!ethane ?(*,()@, tertah!drofuran E57F,

2-Me-57 ?(&,('@, and dimetho.!ethane ?(/,2*@ have been made to optimi3e electrol!te composition4 5owever, because these

ethers can be o.idi3ed b! the charged cathode ?(*,()@, the! are not good C cosolvents and do not meet electrol!te safet!

re6uirements4 Linear carbon- ates, such as dimeth!l carbonate EDMCF ?2(H2=@ or eth!l meth!l carbonate EMCF ?2)@, commonl!

#nown as thinning solvents, are also used with C to reduce its viscosit!4 his mi.ture has wide electrochemical stabilit! and

remains stable on a cathode surface up to =4*: ?)@4 ach component in a mi.ture of C, DMC, and MC has merits that are

integrated into the mi.ture Ee4g4, the high anodic stabilit! of C on cathode surfaces, the high solva- tion of C toward lithiumsalts, and the low viscosit! of DMCIMC to promote ion transportF4 his formulation represents the state of the art in lithium-ionelectrol!tes and has been adopted b! researchers and manufacturers ?),(/,2&H%*@4 "ther linear carbon- ates, such as dieth!lene

carbonate EDCF ?%(H%


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!pical electrodes for lithium-ion batteries are composites consisting of agglomerated primar! particles of active inter-calation compounds Ecalled secondar! particlesF, binders, and conductive additives coated and calendared on current collectors4

Currentl!, the most desirable compounds for cathode materials are Li$i

.

Mn

!Co

(N.N!

"

2

, LiMn

2

"

<

and Li7e>"<

based s!stems4 Most of these materials are s!nthesi3ed in-house through solid-

state reactions ?=/,)*@, h!drothermal s!nthesis ?)(@, solHgel preparation ?)2@, etc4 Such active materials are also available from a

few compa-

remains stable up to =4( : and has high conductivit! in CIDMC E/4* mS cmN(

at 2* KCF ?22@4 here is less concern about metal dissolution from cathode materials because of the absence of fluorine species4Lower impedance has been reported for S; films formed on anode surfaces in LiCl"

<

electrol!te than for films formed in Li>7

)or lithium tetrafluoroborate ELi97

<

F ?%)@4 5owever, LiCl"

<

is a strong o.idant and reacts easil! with other organics because of the high

o.idation state of chlorine, and thus raises safet! concerns ?%&@4 Li97

<

remains stable up to about = : vs4 ELiILiAF ?%'@, but its applicationis limited b! the low conductivit! in CIDMC E


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because of its rapid dissolution in carbonate solvents and its low cost4 he t!pical concentrationof Li>7

)

%4(4 0ctive particle properties salt is ( M in an

electrol!te s!stem4 Most li6uid electrol!tes com- posed of C, DMC or MC, and Li>7

)are suitable for use in practical

>roperties, such as particle si3e, shape,

morpholog!, distribution cells because the! e.hibit a conductivit! higher than (*N% S cmN(

and cr!stallite si3e, affect batter! performance ?&2@4 0

wide range of at room temperature ?22@4 5owever, the flammabilit! of these sol-

particle si3es can be found in the literature, from tens

of nanome- vents and their vapors can cause a maor safet! issue in lithium-ion

ters in primar! particles to tens of micrometers in

agglomerates4 batteries4

Man! efforts have been made to tailor the particle si3e of cathode


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2ower Sources (/) E2*((F 2


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able ( 7lame retardants and their performance capabilities4

7lame retardant lectrol!te medium >erformance

rimeth! phosphite EM>EiFF ?7

)

in (I( CIDC EwtQF M> EiF reduces the flammabilit! of the electrol!te4 ;t enhances both the

thermal stabilit! of the electrol!te and impedance

stabilit! of the lithium cells rimeth!l phosphate EM>EaFF ?7

)

in (I( CIDC EwtQF M> EaF reduces the flammabilit! of the electrol!te4 ;t improves the thermal stabilit! of the electrol!te but

increases the chare transfer resistance on the cathode side risE2,2,2-trifluoroeth!lF phosphate E7>F ?CICIMC E%I%I< and (I(I% wtQF lectrol!te becomes nonflammable with (= wtQ 7> at the e.pense of 2*Q loss

in ionic conductivit!4 7> can increase c!cling efficienc! of the graphite electrode in >C-based electrol!tes b! suppressing >C

decomposition and graphite e.foliation 7> ?=2@ ( M Li>7

)

in CIMC E(I( wtQF 7> Eless than 2* volQF improves capacit! retention andcapacit! utili3ation 2,>> concentration of *Q, =Q, (*Q, (=Q, and 2*Q, respectivel!4 =Q ;>>> additive dela!s the onset temperature of S;

decomposition b! (& KC, and the heat generation is reduced from N> content below (=Q in electrol!tehas little effect on c!cle efficienc! of the batter! rieth!l phosphate E>F, M> EaF,

he.ametho.!c!- clotriphospha3ene E5M>$F ?7

)


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( M Li>7

)

in CIMC E(I( wtQF 5igh content E(* wtQF is re6uired to effectivel! suppress the flammabilit! of

the electrol!te and results in severe degradation in performance4 he capacit! retention in full cell after (** c!cles follows1

5M>$ > M> EaF

Meth!l difluoroacetate EM70F,

eth!l difluoroacetate E70F ?7

)

in CIDMC E(I(F Li>7

)

IM70 shows the best thermal stabilit! toward lithium metal or Li

*4=

Co"

2

, shifting the e.othermic pea# with lithium metal or Li

*4=

to %** KC4 M70 had a better capacit! than other fluoroesters4 he c!cling efficienc! is about '*Q after (** c!cle times b! the

method Li on stainless steelT Meth!l nonafluorobut!l ether

EM7F ?


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generate solid products, which ma! form a passivating la!er on the cathode, resulting in larger polari3ation of the cell ?22@ and,conse6uentl!, c!cle-life degrada- tion4

he effect of particle si3e on cathode performance is summa- ri3ed in able 24 ;t has been reported that capacit! retention is better for an LiMn

(4=

the discharge capacit! decreases when the average particle si3e is increased from (4( to % m4 he capacit! of an LiCr *42

Mn

(4'

"

< cathode increases with increasing particle si3e up to =*nm

but decreases with increasing particle si3e for particles larger than =* nm ?&


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specific surface area and larger grain si3e produced better c!cle si3ed particles at N(* KC, but it is inferior at 2= KC ?'*@4 ;t has

performance4 he! also reported that the c!cle performance for been reported that both capacit! and coulombic efficienc! increase

dense LiMn

2 as LiMn2

"

<

particles and hollow particles with thic#er

shells "

<

particle si3e is decreased from =< to 2* m ?&)@4 0n

were similar to or better than that for hollow particles

with thin- LiCr

*42

$i

*4<

Mn

(4<

"

<

cathode with a particle si3e larger than =** nm

ner shells4 he structure of dense particles and hollow

particles with shows higher discharge capacit! and better c!cling stabilit! than

thic#er shells remained after (** c!clesB hollow

particles with thin- a cathode with a particle si3e smaller than =** nm ?%*@4 5owever,

ner shells developed crac#s in the shell structure ?&2@4 he crac#s


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able 2 >article si3e effect on cathode performance4

Cathode material >article si3e Lattice parameter EUF 9 Em2 gN(F Comments

LiMn

2N.

?2(@ &* nma '4()'< &H' 9etter capacit! retention achieved with fine particle, especiall! at

high C rate ( ma '4()') *4< LiCr

*42

$i

.

"

<

?%*@ ==H%2(= nma '4(')H'4(/& ' to V( 5ighest discharge capacit! and best c!cling stabilit! was achieved

with particle si3e of ((** nm LiMn

2

$i

*4<

Mn

(4<

"

<

?'2@ '=


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si3e distribution would be improved as compared with nanoparticle of narrower si3e distribution LiCo"

2

?/=@ '4* mb :OC7s became h!drophilic after being treated with 5

2

"

2

, which help it disperse in the suspension and improved the discharge performance Li$i

*4=

Mn

(4=

"

<

?'*@ $ano si3e and < ma he electrodes with micro-si3ed particle have better discharge

capacit! at 2* KC, whereas the electrodes with nano-si3ed particle e.hibit better discharge capacit! at N(* KC

a 0verage particle si3e4 b Median diameter4

li#el! caused a portion of the capacit! fading4 5uang and cowor#- ers ?&2@ reported that LiMn

2

diffusion path and higher surface area of smaller graphite parti- "

<

with uniform spherical particles and

cles facilitate thermall! induced delithiation andgenerate more spherical cr!stallites showed better c!clabilit!, while an irregular

heat ?''@4 Conse6uentl!, the thermal stabilit! of

graphite electrodes particle morpholog! and the presence of faceted cr!stals led to lessdecreases with decreasing particle si3e4 optimal

electrochemical c!cling4

he influence of the particle si3e distribution in a composite

%424 0ctive electrode materials processing electrode

has been modeled for constant current discharge assum- ing that the intercalation ratio is the same for each particle ?'%@4

0ccording to the t!pe of solvent used, the

processing of elec- he first discharge depth can be estimated using an average grain

trodes can be classified into two categories1 water-

based Ea6ueousF si3e corresponding to the ma.imum of the volume distribution for

and organic solvent-based Enona6ueousF s!stems ?/(@49ecause the constant standard deviation Oaussian, Oamma, and 7ermi distribu-

voltage of lithium-ion batteries is much higher than the

voltage at tions, and Oaussian distribution with various standard deviations4

which water electrol!3es, an! water must be removed

from the he presence of a small fraction of large particles in a composite

electrode material4 his results in stringent

re6uirements of below electrode with a maorit! of monodispersed small particles low-


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(*H2*ppm of water, which led industr! to focus onnona6ueous ers the overall capacit!4 0 noticeable increase in the first discharge

s!stems processed in controlled dr!-roomatmospheres4 depth is observed when the largest particles are eliminated from

;n a t!pical nona6ueous s!stem, flammable organicsolvents are the upper part of the Oaussian distribution4

used to obtain a stable suspension with pol!vin!lidenefluoride he effect of particle si3e and particle si3e distribution ?'%@ on

E>:D7F as the binder and $-meth!l-2-p!rrolidone

E$M>F as the performance ?'


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of an environmental ha3ard and are lower in cost, butthe! chal- E2H:D7 E(=H(' +R

#gN(F binder com- >article si3es of (2 and 2* m are considered to provide the opti-

monl! used with the $M> solvent ?)&@4 he s!stems

suffer from mum combination of reversible capacit! and ;CL in the electrol!te

powder agglomeration caused b! strong h!drogen

bonding and for fla#e ?'=@ and artificial ?')@ graphite, respectivel!4 he reduced

electrostatic force introduced b! the use of water as a solvent ?/&@4


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able % 7ormulations of various cathode dispersions4

Oroups lectrode composition

Ouo et al4 ?%2@ Cr-doped Li?$i

(I%

Co

(I%

Mn

(I%

@"

2

A acet!lene blac# A >7 E'=I(*I= wtQF 0#lalouch etal4 ?%*@ 2* mg LiCr

*42

$i

*4<

Mn

(4<

"

<

A MMM super p carbon blac# A >:D7-57> E&2I(&I(( wt

QF unduraci and 0matucci ?2(@ LiMn

2N.

$i

."

<

A super p carbon blac# A >:D7-57> A D9> E%)4=I/4(I2


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2

"

<

A >:0 EMW (*****F A graphite E'&I%I(* wtQF Lee et al4 ?/=@ LiCo"

2

A graphite ES-)F and :OC7s A S9R and SCMC EMW 2=* ***, DS of

(42F E/24=I)I(4= wtQF am et al4 ?(/%@ Li?$i

(I%

Co

(I%

Mn

(I%

@"

2

A super > blac# A >:D7 E')I'I) wtQF ao et al4 ?"

<

A etchen blac# A CMC A >7 E/*I=I


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Mn

(4'=

@"

<

A Super > carbon blac# A >:D7 E'=I&4=I&4= wtQF >orcher et

al4 ?(/=@ Li7e>"

<

Isuper p carbonI>:D7 E'*I(*I(* wtQF Ligneel et al4 ?(/)@ Li

(4(

:

%

"

'

IC9I>MM0 E&%I'I(/ wtQF Li et al4 ?(/&@ Li7e>"

<

IS)ISuper >I>90ISCMCI>SS0 E:0, pol!vin!l alcoholB :OC7s, vapor-grown carbon fibersB S9R, st!rene butadieneB SCMC,

sodium carbo.!meth!l celluloseB >MM0, pol!- meth!lmethacr!lateB >90, pol!but!l acr!lateB >SS0, pol!E00F have been tested in an

a6ueous-based Li7e>"

<

?(*)H(*/@, electrostatic spra! deposition ?((*H((=@, pulsed laser deposition ?(()H(2*@, radio fre6uenc! sputtering ?(2(H(2%@,

spin coating ?(2


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addressed in future publications4 best dischargecapacit! were obtained at p5X& ?//@4 mulsion-

Recentl!, three-dimensional E%DF batteries have been proposed pol!meri3ed st!reneHbutadiene copol!mer late. was chosen as a

to miniaturi3e batter! si3e ?(%%H(%=@4 ;n contrast tothe in-plane binder to enhance the strength of the green graphite electrode sheet

surface in traditional electrodes, the out-of-planedimension in a ?/'@4 .tra pretreatments, including ph!sical and chemical meth-

%D configuration ma! enable the batter! to have a

small areal ods, are needed to disperse carbon material as conducting additive

footprint4 he %D configuration ma! also provide a

shorter diffu- in a6ueous s!stems4 >h!sical methods include ultrasonication, ball

sion path length for lithium ions between anode and

cathode and milling, grinding, and high-speed shear mi.ing ?(**,(*(@4 Chemical

a higher electrode surface area ?(%%@4 Some %D

architectures are methods include using chemical functionali3ation ?(*2@ or surfac-

achieved b! depositing thin films in a %D arrangementusing a tants ?(*%@, reflu.ing carbon materials in concentrated acids ?(*


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%42424 lectrode modification and optimi3ation onsma! be an issue since this causes poor wettabilit! on current

he rate capabilit! of batteries is determined b! the#inetics of collectors and delamination4 his issue can be solved b! either

the chargeHdischarge reactions and the mobilit! oflithium ions to decreasing the surface tension of dispersions or increasing the sur-

and from their final intercalation sites4 he rate performance of the face energ! of current collectors4 he surface tension of dispersions

cathode material appears to be the bottlenec# in the

development can be increased b! using a co-solvent or multi-solvent s!stem,

of lithium ion batteries with high rate capabilit! ?(%/@4

Different such as ethanolHwater4 he surface energ! of current collectors

methods have been attempted to improve the rate

performance of can be enhanced b! some heat treatment, such as corona discharge

the cathode materials, including adding a conductive

coating such treatment ECDF or plasma treatment4 ;t has been demonstrated at

as carbon ?(


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tion of carbon anode materials ?(


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?()2@4 he surface coating ma! improve the

temperature, respectivel! ?()',(&


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are used as batter! separators ?(/*@4 the o.ides remainas a coating on the particles of active material

0 new direction in lithium ion batter! separatorresearch is the ?()2@4 he thermomechanical process is cost-effective4 he c!cla-

addition of ceramics and metal o.ides to the separator pol!mer bilit! of i"

2

-coated LiCo"

2

is better when the thermomechanical

solution to form highl! filled pol!mer composites4

his modifica- process is used than when the solHgel process is used ?()2@4

tion to the conventional pol!mer separator is thought to

improve Recentl!, Oao et al4 coated a la!er of silver onto a graphite elec-

the short resistance, as well as the thermal and

mechanical prop- trode ?(=2@ and found that the 0g-coated graphite electrode canerties during batter! operation4 o date, there is little

information significantl! suppress >C decomposition and graphite e.foliation4

available on the processing methods related to these

novel com- Charge-transfer resistance decreased, and the diffusion coefficient

posite separators4 of Li ions increased4 5owever, silver

is not e.pected to be introduced into large-scale energ! storage devices4

5. Cost assessments

4. Separator

Currentl!, the cost of lithium-ion batteries is still too high4 7or e.ample, the cost of (',)=* cells is appro.imatel! G(&** ?2,%@,

twice 0 separator is placed between the cathode and the anode to

of the target price on a #W basis for 5:s4 he cost of lithium-ion prevent contact4 0 good separator should have high ionic flow,

batteries is appro.imatel! %H= times of the target priceon a #Wh negligible electronic conductivit!, good wettabilit!, high chemi-

basis for >5:s ?(/(@4 he main components of batter! costs are cal stabilit! against electrol!tes, high mechanical and dimensional

materials, labor and overhead4 he cost of materials isthe most sig- stabilit!, and sufficient ph!sical strength to withstand the assem-

nificant part4 ;t ma#es up over '*Q and /*Q of the total costs of high


28/37

2


29/37

power and high energ! batteries, respectivel! ?2@4 herefore, the potential for reducing costs of lithium-ion batteries lies inachieving low cost materials and materials processing4 ;t is especiall! impor- tant to lower the cost of cathode materials since

the! ma#e up over &*Q of the total cost for high power batteries ?2@4 o this end, novel methods that can s!nthesi3e largeamounts of cathode materials with low cost raw materials need to be developed4 Development of novel cathode materials with

higher capacit! andIor a wider state of charge is an alternative solution which reduces the re6uired amount of cathode materials

and, thus, the batter! si3e4 ;n addition, improvement in processing of cathode slurries can also significantl! reduce the cost4 he

cost of Li$i.

?((@ 54 9u6a, 04 Wursig, J4 :etter, M44 Spahr, 74 rumeich, >4 $ova#, J4 >ower

Sources (=% E2**)F %'=H%/*4 ?(2@ J4 :etter, >4 $ova#, J4 >ower Sources ((/ E2**%F %%'H%


30/37

?%(@ J4-54 Lee, J4-S4 im, C4 im, D4S4 Yang, 4-M4 Choi, W4;4 >ar#, +4 >ai#, lectrochem4

Solid-State Lett4 (( E2**'F 0(&=H0(&'4 ?%2@ J4 Ouo, L474 Jiao, 54 uan, L4Z4 Wang, 54[4 Li, M4 Yhang, 4M4 Wang,

lectrochim4 here is little doubt that materials processing and material development are critical to improving lithium-ion batter! perfor-

0cta =( E2**)F )2&=H)2'*4 ?%%@ 4 >eled, D4 Oolodnis#!, C4 Menachem, D4 9ar-ow, J4 lectrochem4 Soc4 (ure 0ppl4 Chem4 '* E2**'F 2==%H2=)%4 ?4 Yhang, >4 Yhang, Y454 Li, M4

Sun, 4>4 Wu, 54Z4 Wu, lectrochem4 Commun4

/ E2**&F (&**H(&*%4 that end, a shift from a

nona6ueous s!stem to an a6ueous s!stem

?ower Sources for fabricating composite electrodes might significantl! reduce the batter! cost and

environmental effects4 Comparable results can be obtained from an a6ueous s!stem such as those in conventional

(


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0(*&/H0(*'24 ?=%@ M4S4 Ding, 4 [u, 4R4 Jow, J4 lectrochem4 Soc4 (


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33/37

?)


34/37

4;4 ;3gorodina, 0ccounts Chem4 Res4 4J4 9ouwman, 9404 9ou#amp, 54J4M4 9ouwmeester, 54J4 Wondergem, >454L4

$otten, J4 lectrochem4 Soc4 (4 Reade, 4J4 Cairns,J4 lectrochem4 Soc4

(


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E2***F (2ower Sources

(2' E2**ower Sources /% E2**(F (2%H(2/4 ?(=)@ L4 You, 74 ang, 4->4 Yheng,

W4 Shen, lectrochim4 0cta =< E2**/F %/%*H%/%ower Sources (*/ E2**2F %''H%/%4


36/37



37/37

?()/@ S4-J4 Owon, J4-54 Choi, J4-4 Sohn, 4-4 ;hm, 4-C4 $ho, $ucl4 ;nstrum4 Methods

>h!s4 Res4, Sect4 91 9eam ;nteract4 Mater4 0t4 2)& E2**/F %%*/H%%(%4 ?(&*@ J4-4 Sohn, J4S4 ;m, S4-J4 Owon, J4-54 Choi, J4 Shin,

4-C4 $ho, Radiat4 >h!s4 Chem4,

&' E2**/F, =*=H=*'4 ?(&(@ 04 Subramania, $444 Sundaram, 04R4S4 >ri!a, O4:4 umar, J4 Membr4 Sci4 2/<

E2**&F 'H(=4 ?(&2@ S4S4 im, D4R4 Llo!d, J4 Membr4 Sci4 )< E(//(F (%H2/4 ?(&%@ 5s4 9ierenba, R494 ;saacson, M4L4 Druin,

S4O4 >lovan, ;nd4 ng4 Chem >rod4 Res4Dev4 (% E(/&F, a#ashima, atsu!a ESaitama, J>F, "#amoto,

en#ichi ESaitama, J>F, onen Corporation Eo#!o, J>F, +nited States, (//(4 ?(&=@ 4 Sarada, L4C4 Saw!er, M4;4 "stler, J4

Membr4 Sci4 (= E(/'%F /&H((%4 ?(&)@ Japan ;ndia $ews, (//), p4 /(4 ?(&&@ M4L4W4"4 Druin E$JF, Loft, John 4 ESpringfield, $JF,

>lovan, Steven O4 ELiv-

ingston, $JF, Celanese Corporation E$ew or#, $F, +nited States, (/&atent, Japan E(//)F4 ?('(@ 04W4-c4

5ashimoto EJ>F, agi, a3uo EWa#i-cho, J>F, Manto#u, 5itoshi EWa#i-

cho, J>F, Mitsui Chemicals, ;nc4 Eo#!o, J>F, +nited States, 2***4 ?('2@ W4-54 Seol, 4M4 Lee, J4-4 >ar#, J4 >ower Sources

()% E2**)F 2ar#, lectrochim4 0cta =<

E2**/F h!s4 Chem4 Solids )&

E2**)F

(2&=H(2'*4 ?(/&@ C4C4 Li, [4W4 >eng, J44 Lee, 74M4 Wang, J4 lectrochem4 Soc4 (=& E2*(*F

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