Elec ochemis y Communica ions 135 (2022) 107210
A ailable online 10 Janua y 2022
1388-2481/© 2022 The Au ho (s). Published by Else ie B.V. This is an open access a icle unde he CC BY license (h p://c ea i ecommons.o g/licenses/by/4.0/).
Elec ode ab ica ion p ocess and i s in luence in li hium-ion ba e y
pe o mance: S a e o he a and u u e ends
R. Gonçal es
a
, S. Lance os-M´
endez
b
,
c
, C.M. Cos a
d
,
e
,
*
a
Cen e o Chemis y, Uni e si y o Minho, 4710-057 B aga, Po ugal
b
BCMa e ials, Basque Cen e o Ma e ials, Applica ions and Nanos uc u es, UPV/EHU Science Pa k, 48940 Leioa, Spain
c
Ike basque, Basque Founda ion o Science, 48009 Bilbao, Spain
d
Cen e o Physics, Uni e si y o Minho, 4710-057 B aga, Po ugal
e
Ins i u e o Science and Inno a ion o Bio-Sus ainabili y (IB-S), Uni e si y o Minho, 4710-057 B aga, Po ugal
ARTICLE INFO
Keywo ds:
Elec ode ab ica ion
Li hium-ion ba e ies
Anode, ca hode
ABSTRACT
Li hium-ion ba e ies (LIBs) a e he main ene gy s o age sys em used in po able de ices. Thei ou s anding
cha ac e is ics allied o he g owing ma ke o po able de ices and elec ic ehicles p o ides ba e ies an
inc easing end o e he nex yea s. Du ing he pas decade, imp o ed ma e ials o LIBs ha e been de eloped,
wi h less a en ion being ocused on he manu ac u ing p ocess, despi e i s c i ical in luence in ba e y pe o -
mance. In he p esen wo k, he main elec ode manu ac u ing s eps a e discussed oge he wi h hei in luence
on elec ode mo phology and in e ace p ope ies, in luencing in u n pa ame e s such as po osi y, o uosi y o
e ec i e anspo coe icien and, he e o e, ba e y pe o mance. A s a e o a on he main s eps o he elec-
ode manu ac u ing p ocess is p esen ed, oge he wi h u u e di ec ions wi h espec o LIBs ab ica ion.
1. In oduc ion
Recha geable li hium-ion ba e ies (LIBs) a e nowadays he mos
used ene gy s o age sys em in he ma ke , being applied in a la ge a-
ie y o applica ions including po able elec onic de ices (such as sen-
so s, no ebooks, music playe s and sma phones) wi h small and
medium sized ba e ies, and elec ic ehicles, wi h la ge size ba e ies
[1]. The ma ke o LIB is es ima ed a $41.1 billion in 2021, wi h a
o ecas compound annual g ow h a e (CAGR) o 12.3% up o 2030
[2,3].
Compa ed o o he ba e y echnologies, he main ad an ages o LIBs
a e being ligh weigh , low-cos , p esen ing high ene gy and powe
densi y, no memo y e ec , p olonged se ice-li e, low cha ge los (sel -
discha ge), highe numbe o cha ge/discha ge cycles and being ela-
i ely sa e [4,5]. Despi e hose ad an ages, p ope ies including speci ic
ene gy, powe , sa e y and eliabili y a e key issues o u he imp o e in
LIBs. The main componen s o LIBs a e he elec odes (anode and
ca hode) and he sepa a o o solid polyme elec oly e [4,6].
2. Elec ode componen s
Independen ly o he elec ode ype, hey a e composed o a polyme
binde (PB), a conduc i e addi i e (CA) and an ac i e ma e ial (AM).
The main unc ion o he polyme binde is o hold oge he he ac i e
ma e ial and conduc i e addi i e, imp o ing he mechanical s abili y,
pa icles cohesion and lexibili y o he elec odes. The conduc i e ad-
di i e allows o imp o e he elec ical conduc i i y o he elec ode and
he ac i e ma e ial is esponsible o he cell capaci y and po en ial.
Fig. 1 shows a schema ic ep esen a ion o an elec ode and i s main
componen s [7].
The main di e ence be ween he anode and he ca hode is he ac i e
ma e ial. Anodes a e ypically based on silicon and/o ca bonaceous
ma e ials such as g aphi e, g aphene, o ca bon nano ubes [8]. Fo he
ca hode, li hium compounds a e used, such as li hium cobal oxide
(LiCoO
2
, LCO), li hium nickel oxide (LiNiO
2
, LNO), li hium manganese
dioxide (LiMnO
2
, LMO), li hium i on phospha es (LiFePO
4
, LFP), o
li hium nickel cobal aluminum oxide (LiNi
x
Co
y
Al
z
O
2
, x +y +z =1,
NCA), among o he s [9–11].
The elec ode ab ica ion p ocess is c i ical in de e mining inal
ba e y pe o mance as i a ec s mo phology and in e ace p ope ies,
in luencing in u n pa ame e s such as po osi y, po e size, o uosi y,
and e ec i e anspo coe icien [12,13]. Elec ode manu ac u e in-
ol es se e al s eps including he mixing o he di e en componen s,
cas ing in a cu en collec o and sol en e apo a ion [14]. A e he
sol en e apo a ion s ep, a calende ing p ocess is used o educe
po osi y and o imp o e pa icles cohesion, consequen ly imp o ing
* Co esponding au ho .
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Elec ochemis y Communica ions 135 (2022) 107210
2
ba e y pe o mance [15]. The mixing, cas ing and sol en e apo a ion
s eps depend on pa ame e s such as sol en ype, polyme ma ix,
conduc i e addi i e, ac i e ma e ial, sp eading me hod, hea ing and
sol en e apo a ion condi ions [16].
In he ollowing, elec ode main p epa a ion pa ame e s and hei
in luence on elec ode mo phology and consequen ly on ba e y pe -
o mance a e p esen ed.
3. Elec ode p ocessing and ab ica ion
The elec ode manu ac u ing is di ided in o wo main p epa a ion
phases: slu y and ilm p ocessing. Each one o hese phases and hei
co esponding mos in luen ial pa ame e s a e illus a ed in Fig. 2a).
The i s phase is he elec ode slu y ab ica ion which in ol es
mixing he di e en elec odes componen s: polyme binde and sol-
en , conduc i e addi i e and ac i e ma e ial. Mixing is an essen ial s ep
o con olling he heological p ope ies o he sys em and o p ope ly
dispe se he componen s wi hin he slu y. To achie e a p ope mixing
homogenei y, magne ic s i e s, ul asonic ba hs and ball mills a e he
mos used s a egies a a labo a o y scale, allowing o op imize he
iscosi y o he slu y [17]. A an indus ial scale, he mixing o hese
componen s is achie ed h ough la ge-scale mixe s including uni e sal
and high-speed mixe s, plane a y mixe s, and homogenize s, among
o he s [17].
I has been demons a ed ha he slu y p epa a ion me hod,
including he o de in which he componen s a e added, in luences he
heological beha io and consequen ly elec ode ba e y pe o mance
[18]. Addi ionally, di e en sp eading me hods including slo -die
coa ing [19], sc een-p in ing [20] and elec opho e ic deposi ion
Fig. 1. Schema ic ep esen a ion o he di e en componen s o
LIBs elec odes.
Fig. 2. a) Schema ic ep esen a ion o he main elec ode ab ica ion phases and s eps wi h indica ion o he mos in luen ial pa ame e s and b) ep esen a i e alues
o each pa ame e s o ob aining high cell ene gy densi y.
R. Gonçal es e al.
Elec ochemis y Communica ions 135 (2022) 107210
3
(EPD) [21] a e used o ensu e uni o m elec ode hickness and
geome y.
Wi h espec o ilm p epa a ion, he main s eps a e sol en e apo-
a ion and calende ing. The sol en e apo a ion s ep consis s o sol en
ex ac ion h ough he combina ion o empe a u e and ime o ob ain a
ilm wi h good adhesion o he cu en collec o , lexibili y and wi hou
he o ma ion o c acks on he elec ode su ace [22]. Finally, a e
sol en e apo a ion, he ilms unde go ypically a calenda ing p ocess.
Calende ing is used o educe elec ode’s po osi y h ough he compo-
nen s compac ion, educing i s hickness and inc easing i s densi y [23].
To imp o e elec ode homogenei y, machine lea ning-based e alu-
a ion a e being used o assess he impac o he elec ode’s o mula ion
on he manu ac u ing p ocess, he mos ele an pa ame e s being mass
loading and hickness [24].
Typically, he elec ode manu ac u ing cos ep esen s ~33% o he
ba e y o al cos , Fig. 2b) showing he main pa ame e alues o
achie ing high cell ene gy densi ies >400 Wh/kg, depending on he
ac i e ma e ials used o he elec odes and he sepa a o /elec oly e
[25,26].
In o de o imp o e ba e y pe o mance, he elec ode mus p esen
high adhesion o he cu en collec o , low po osi y <35%, o uosi y o
1 and low impedance alue.
In addi ion, conside ing he g owing demand o li hium and o he
ma e ials needed o ba e y manu ac u ing, such as [3], [27] and [28],
i is necessa y o ocus on mo e sus ainable ma e ials and/o p ocesses
and de elop e icien , cos -e ec i e and en i onmen al iendly
me hods o ecycle and euse ba e ies, p omo ing a ci cula economy
app oach and educing bo h he need o ex ac mo e esou ces and he
land ill disposal o used de ices. I his scope, he elec ode ab ica ion
plays an impo an ole due o i s alue and complexi y in e ms o
ma e ials and ma e ials combina ions. The ma e ial eco e ed om he
ecycling p ocess o elec odes, which include di ec ecycling, py o-
me allu gical and hyd ome allu gical app oaches, can be eused in he
elec ode manu ac u ing phase o ob ain a new ba e y wi h dec eased
en i onmen al impac [28].
3.1. E ec o he mixing s a egy and sp eading me hod
Being he i s s ep, mixing is a c i ical issue as i will a ec all
subsequen s eps o elec ode ab ica ion and con ibu es o app oxi-
ma ely 7 o 8% o he o al manu ac u ing cos [29]. The objec i e o his
s ep is he uni o m pa icle dis ibu ion and he ailo ing o he heo-
logical p ope ies o he sp eading p ocess. Di e en me hods a e used
a a labo a o y scale such as magne ic s i ing, ball milling, o ul asonic
mixing, among o he s, in o de o p ope ly dispe se and mix he
di e en amoun o pa icles (conduc i e addi i e and ac i e ma e ial)
in he polyme binde solu ion [29]. A an indus ial le el, he me hods
o mixing a e hyd odynamic shea mixing (HSM), ball milling, ho-
mogenize s, plane a y mixe s, uni e sal and high-speed mixe s, among
o he s [29].
The componen s mixing sequence a ec s elec ode p ope ies and
heological beha io and consequen ly ba e y pe o mance [18]. I has
been shown ha he mixing o ca bon black (CB) wi h poly( inylidene
luo ide) (PVDF) solu ion a he i s s ep can acili a e he o ma ion o a
gel like slu y, main aining his beha io a e adding he ac i e ma e ial
pa icles [30].
CB is widely used as conduc i e addi i e and i has been obse ed
ha inc easing mixing ime and mixing in ensi y inc eases he deg ee o
deagglome a ion o he CB wi hin he slu y. In addi ion, he CB bonds
o he ac i e ma e ial su aces, p o iding sho - ange elec ical con ac s
[31]. Fu he mo e, high in ensi y d y mixing e eals o inhibi elec ical
conduc i e ne wo k o ma ion [32].
Wi h he objec i e o imp o ing e ec i eness and o simpli y elec-
ode ab ica ion, a me hod based on ex usion mixing and subsequen
sp eading using slo -die echnique has been de eloped. The ex usion-
based ab ica ion ou e allows highe solid con en s (~85 w %) and
excellen pa icle dispe sion and homogenei y wi h no endency o
binde mig a ion [33]. Fo his mixing echnique, solid con en s anging
om 70 o 75 w % wi hin he elec ode slu y esul s in an imp o ed
deg ee o dispe sion o he CB [34].
Fu he mo e, i has been obse ed ha he CB pa icle size has an
impo an impac on he elec ode s uc u e, smalle pa icle sizes
leading o smalle deg ee o po osi y, p omo ing a highe elec ode laye
igidi y [35].
In addi ion, 3D p in ing echniques such as ex usion ee o m
ab ica ion (EFF) ha e ecen ly been used o achie e high mass loadings
and complex geome y designs, compa ed o con en ional lamina ed
s uc u es [36]. 3D p in ing echniques also allow o une he elec ode
pe o mance by a ying speci ic pa ame e s such as he dis ance be-
ween he p in ed lines [37].
The selec ion o sol en has as impac on he elec ode slu y pa icle
dispe sion, as well as on p ocess sus ainabili y, due o he en i onmen al
impac o se e al o he mos commonly used sol en s [38]. In his
scope, a sol en - ee di ec coa ing p ocess has been de eloped o
elec ode ab ica ion ha only in ol es he d y-sp aying o he sol en -
ee elec ode componen mix u e and a subsequen iso he mal ho -
p essing. I has been obse ed ha he elec odes p oduced by his
me hod p esen homogeneous pa icle dis ibu ion and sui able ba e y
pe o mance [38]. Ano he echnique o manu ac u e sol en - ee
elec odes is elec os a ic coa ing [39].
In addi ion, elec ode hickness is co ela ed wi h he sp eading
p ocess and ba e y a e pe o mance dec eases wi h inc easing elec-
ode hickness and discha ge a e due o anspo limi a ion and ohmic
pola iza ion o he elec oly e [40]. Also, hicke elec odes a e di icul
o d y and end o c ack o lake du ing hei p oduc ion [41]. I has been
obse ed ha he elec ode hickness and he elec ode’s densi y (i.e.
po osi y), ha e simila con ibu ion and signi ican impo ance o
maximize ba e y capaci y [42].
3.2. E ec o polyme binde /sol en
The polyme binde is essen ial o main ain he cohesion o he
pa icles wi hin he elec ode. The mos used polyme binde o LIBs is
PVDF ha dissol e in oxic and lammable sol en s such as n-me hyl
py olidone (NMP) and n,n-dime hyl o mamide (DMF) [16].
Thus, sol en eco e y is impo an o ba e y cos educ ion and o
imp o ing sus ainabili y o elec ode p ocessing, and a p ocess model
was de eloped o s udy he ene gy and cos implica ions o ca hode
d ying and NMP sol en eco e y, he eco e y p ocess leading o an
ene gy demand o ~10 kWh pe kg o NMP sol en [43]. To de elop
sus ainable app oaches o LIBs manu ac u ing, g een, less oxic and
sa e sol en s a e being p oposed [44]. In o de o educe en i onmen al
impac , li e cycle assessmen (LCA) s udies on wa e -based
manu ac u ing o NMC-g aphi e ba e y packs ha e been epo ed. I
has been obse ed ha wa e -based manu ac u ing can educe he
manu ac u ing ene gy by mo e han 40% [45]. I has been also shown
ha elec odes p ocessed wi h wa e show compa able ba e y pe o -
mance o elec odes p ocessed wi h NMP sol en [46].
The adhesion o he elec ode o he cu en collec o depends on he
binde ype and i has been epo ed ha he molecula chain leng h o
he binde in luences i s adhesion s eng h and ha binde s wi h highe
molecula weigh show less mig a ion e ec s due o he inc ease o
slu y iscosi y [47]. Polyme binde con en up o 20% a ec s he
pa icle/pa icle cohesi e s eng h and he elec ode- ilm/cu en -
collec o adhesion s eng h and, consequen ly, elec oly e soaking [48].
Mo eo e , d y powde mixing wi h sol en - ee polyme has been
de eloped, he unc ional elec odes being manu ac u ed using binde
and conduc i e addi i e ma e ials as low as 1 w , leading o well
dis ibu ed pa icles [49].
R. Gonçal es e al.
Elec ochemis y Communica ions 135 (2022) 107210
4
3.3. E ec o sol en e apo a ion p ocess
Typically, he sol en e apo a ion p ocess in he p epa a ion o LIB
elec odes consis s o sol en ex ac ion om he elec ode slu y, which
depends on sol en ype and polyme binde . Fo he NMP sol en , he e
a e di e en combina ions o empe a u e and ime o ensu e he elec-
ode sol en e apo a ion [16] whe e a apid sol en e apo a ion has
been shown o a ec nega i ely elec ode adhesion and cohesion
s eng h [22].
The sol en e apo a ion p ocess in ol es di e en physical p ocesses
including hea and mass ans e wi h phase change. Fo 150
μ
m hick
elec odes, he la ges amoun o sol en e apo a es in he i s 30 s and
hen slows down because o mass ans e limi a ions. Fu he mo e, 90%
o he sol en is emo ed in less han hal o he o al d ying ime o 100 s
[50].
An impo an pa ame e du ing sol en e apo a ion is binde
mig a ion, which may lead o capaci y ade and mechanical ailu e,
esul ing in elec ode delamina ion om he cu en collec o . I has
been obse ed ha highe e apo a ion a es end o induce supe io
binde concen a ion g adien s as a sho e e apo a ion ime allows less
oppo uni y o edis ibu e he binde mo e e enly h oughou he ilm
[51].
3.4. E ec o he calende ing p ocess
Calende ing is applied a e he sol en e apo a ion s ep o educe
po osi y and po e mic os uc u e, using a wo oll compac o o dec ease
elec ode hickness [15]. The calende ing speed was ound o ha e
negligible impac on ba e y pe o mance up o speeds o 5 m.min
−1
[15]. In addi ion, an impe ec calende ing p ocess can lead o de ec s in
he elec ode s uc u e, such as c acks, and o poo bending cha ac e -
is ics [52].
Calende ing di ec ly a ec s he elec ode po osi y and he po osi y
a ec s elec ode we abili y by he elec oly e, ha consequen ly a ec s
ba e y pe o mance. Lowe ca hode we abili y leads o lowe cell ca-
paci y and lowe anode we abili y can cause li hium deposi ion, which
a ec s sa e y and cycle li e [53]. I is de e mined ha he we abili y
depends mainly on he po e s uc u e and pa ame e s such as po osi y,
po e size dis ibu ion, po e geome y and opology [54].
The ionic conduc i i y o he elec ode depends on i s mo phology,
smalle ac i e ma e ial size o high olume ac ions inducing po es
wi hin he elec odes, hinde ing he Li-ion anspo and inc easing
o uosi y [55]. A e calende ing, he elec ode should ideally p esen a
o uosi y o 1 and a po osi y abou 30–50% in o de o op imize ba e y
pe o mance [56,57].
3.5. Indus ial scale
Indus ial manu ac u ing o LIBs uses simila p ocedu es as o lab-
o a o y scale, he main di e ence being he scale o he used o indus-
ial machines such as indus ial mixe s. The main gap be ween
labo a o y and indus ial scale is he highe quan i ies o he di e en
componen s a he indus ial scale. Typically, he ocus o indus ial
p ocedu es is o lowe he binde and ca bon componen s in he elec-
ode o mula ion down o 2% each. A he labo a o y scale, he ypical
elec ode o mula ion is 80–10-10 w % (ac i e ma e ial-polyme binde -
conduc i e addi i e). Some epo s al eady poin o indus ial scale
elec ode o mula ions o 96% ac i e ma e ial, 2% binde and 2%
conduc i e addi i e in o de o inc ease elec ode densi y [58]. LIB’s
manu ac u ing a indus ial scale allows a be e ope a ion and con ol
wi h he use o inline con igu a ions [14].
4. Conclusion and ou look
Li hium-ion ba e y manu ac u ing p ocesses ha e di ec impac on
ba e y pe o mance. This is pa icula ly ele an in he ab ica ion o
he elec odes, due o hei di e en componen s. The manu ac u ing o
he elec odes can be di ided in o wo phases: slu y and ilm ab ica-
ion. Each one o hese phases is cha ac e ized by speci ic pa ame e s
and condi ions ha in luence he s uc u al, mo phological and chemi-
cal p ope ies o he elec odes. Di e en s udies on mixing p ocess,
slu y sp eading, polyme binde , sol en e apo a ion and calende ing
s eps ha e been ca ied ou no only o assess how hese pa ame e s
in luence elec ode p ope ies bu also o op imize he condi ions o
maximize ba e y pe o mance. To de elop hese high-pe o mance
elec odes some aspec s such as he o de ing o componen s addi ion
du ing mixing, p in ing o coa ing pa ame e s, elec ode hickness,
c acking and po osi y o ma ion, sol en e apo a ion empe a u e and
ime, among o he s, ha e been s udied showing no only he op imal
p ocessing condi ions bu also new app oaches o imp o e elec ode
p ope ies.
•Componen s mixing is he mos impo an p ocess du ing elec ode
manu ac u ing once i a ec s slu y quali y and in luences he es o
he manu ac u ing p ocesses. The addi ion o conduc i e addi i e
igh a e polyme dissolu ion shows o be he bes me hod o
imp o e he elec ode conduc i e ne wo k quali y. Also, inc easing
mixing ime and mixing in ensi y imp o es he deg ee o
deagglome a ion.
•Sp eading is cu en ly he main ocus o s udy no only by echniques
such as hyd odynamic shea mixing (HSM), ball milling and ul a-
sonic mixing bu also by he inc easing use o 3D p in ing echniques.
P in ing echniques and hei p ocessing pa ame e s including dis-
ance and empe a u e be ween pla o m and p in ing head, p in ing
speed, o ex usion speed, among o he s, a e becoming inc easingly
ele an o he new gene a ion o ba e ies wi h op imized sizes,
capaci ies and imp o ed in eg a ion in o po able de ices.
•Sol en e apo a ion is esponsible o he sol en ex ac ion om he
slu y, leading o he o ma ion o he elec ode ilm. In his s ep,
c acks a e o med i he slu y does no ha e he op imal p ope ies.
Fu he , sol en e apo a ion empe a u e and ime ha e g ea
impac on c acking o ma ion. This p ocessing s ep is also ele an
o he adhesion be ween he o med elec ode ilm and he cu en
collec o .
•Calende ing is one o he las s eps du ing elec ode manu ac u ing
and i is esponsible o he pa icle’s cohesion, hickness and
po osi y o he elec ode ilm. Fu he , his s ep is esponsible o he
elec ode we abili y and elec ode densi y, which a ec s elec ode
sa e y, li e cycle and pola iza ion.
•Indus ial scale uses he same me hods as he labo a o y scale. The
main di e ence being he manu ac u ing speed, componen s quan-
i ies and he use o la ge scale indus ial machines. Inline p o-
cessing allows o dec ease he polyme binde and conduc i e
ma e ials pe cen ages, leading o highe ac i e mass loading
elec odes.
The di e en LIBs manu ac u ing s eps mus be aken in o consid-
e a ion du ing ba e y de elopmen . The complexi y and in e play be-
ween p ocessing pa ame e s and ba e y pe o mance leads o la ge
possibili ies o elec ode imp o emen s udies. To be e unde s anding
he complexi y o his p ocess, new ools such as machine-lea ning
me hodologies should be used. Sus ainable app oaches in LIBs
manu ac u ing should also be os e ed o educe en i onmen al impac
wi h espec o ma e ials and p ocesses. In his scope, sol en eco e y
du ing he manu ac u ing p ocess and ee sol en elec ode ab ica ion
mus be add essed, dec easing cos p oduc ion and en i onmen al
impac .
CRediT au ho ship con ibu ion s a emen
R. Gonçal es: W i ing – o iginal d a , W i ing – e iew & edi ing. S.
Lance os-M´
endez: W i ing – o iginal d a , W i ing – e iew & edi ing,
R. Gonçal es e al.
Elec ochemis y Communica ions 135 (2022) 107210
5
Funding acquisi ion. C.M. Cos a: W i ing – o iginal d a , W i ing –
e iew & edi ing, Funding acquisi ion.
Decla a ion o Compe ing In e es
The au ho s decla e ha hey ha e no known compe ing inancial
in e es s o pe sonal ela ionships ha could ha e appea ed o in luence
he wo k epo ed in his pape .
Acknowledgemen s
The au ho s hank he Fundaç˜
ao pa a a Ciˆ
encia e Tecnologia (FCT)
and COMPETE 2020 o inancial suppo unde he amewo k o
S a egic Funding g an s UID/FIS/04650/2021, UID/EEA/04436/2021,
and UID/QUI/0686/2021 and unde p ojec s POCI-01-0145-FEDER-
028157 and PTDC/FIS-MAC/28157/2017. The au ho s also hank he
FCT o he in es iga o con ac s CEECIND/00833/2017 (RG) and
2020.04028.CEECIND (C.M.C.). Financial suppo om he Basque
Go e nmen Indus y Depa men unde he ELKARTEK p og am is
acknowledged.
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