Contributions of Women in Recent Research on Biopolymer Science



Ci a ion: Vee il, U.T.; Olza, S.;
B uge olle de F aissine e, N.;
Bascans, E.; Cas ejón, N.; Ad ien, A.;
Fe nández-Ma ín, R.; Na din, C.;
Fe nandes, S.C.M. Con ibu ions o
Women in Recen Resea ch on
Biopolyme Science. Polyme s 2022,
14, 1420. h ps://doi.o g/10.3390/
polym14071420
Academic Edi o : Co nelia Vasile
Recei ed: 31 Janua y 2022
Accep ed: 28 Ma ch 2022
Published: 30 Ma ch 2022
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c ea i ecommons.o g/licenses/by/
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polyme s
Re iew
Con ibu ions o Women in Recen Resea ch on
Biopolyme Science
Unnimaya Thalakkale Vee il 1,2 , Sheila Olza 1,2,3, Nelly B uge olle de F aissine e 1,2 , Elodie Bascans 1,2,4 ,
Na alia Cas ejón1,2,† , Amandine Ad ien 1,2, Ru Fe nández-Ma ín5, Co inne Na din 1
and Susana C. M. Fe nandes 1,2,*
1E2S UPPA, CNRS, IPREM, Uni e si e de Pau e des Pays de l’Adou , 64000 Pau, F ance;
[email p o ec ed] (U.T.V.); [email p o ec ed] (S.O.);
nelly.b [email p o ec ed] (N.B.d.F.); [email p o ec ed] (E.B.);
[email p o ec ed] (N.C.); [email p o ec ed] (A.A.); co inne.na [email p o ec ed] (C.N.)
2
E2S UPPA, Ma ine Ma e ials Resea ch G oup, Uni e si e de Pau e des Pays de l’Adou , 64600 Angle , F ance
3Depa men o Cellula Biology and His ology, Facul y o Medicine Nu se y, Uni e si y o he Basque
Coun y, B Sa iena, s/n, 48940 Leioa, Spain
4
CNRS, INRAE, INSA, Toulouse Bio echnology Ins i u e (TBI), Uni e si éde Toulouse, 31400 Toulouse, F ance
5En i onmen al and Chemical Enginee ing Depa men , Uni e si y o he Basque Coun y UPV/EHU,
Plaza Eu opa 1, 20018 Donos ia-San Sebas ián, Spain; [email p o ec ed]
*Co espondence: [email p o ec ed]
†
P esen add ess: Depa men o Food Chemis y and Toxicology, Uni e si y o Vienna, 1090 Vienna, Aus ia.
Abs ac :
Nowadays, biopolyme s a e playing a undamen al ole in ou socie y because o he en-
i onmen al issues and conce ns associa ed wi h syn he ic polyme s. The aim o his Special Issue
en i led ‘Women in Polyme Science and Technology: Biopolyme s’ is highligh ing he wo k designed
and de eloped by women on biopolyme science and echnology. In his con ex , his sho e iew
aims o p o ide an in oduc ion o his Special Issue by highligh ing some ecen con ibu ions o
women a ound he wo ld on he pa icula opic o biopolyme science and echnology du ing he las
20 yea s. In he i s place, i highligh s a selec ion o impo an wo ks pe o med on a numbe o
well-s udied na u al polyme s, namely, aga , chi in, chi osan, cellulose, and collagen. Secondly,
i gi es an insigh in o he disco e y o new polysaccha ides and enzymes ha ha e a ole in hei
syn hesis and in hei deg ada ion. These con ibu ions will be pa ing he way o he nex gene a ion
o emale and male scien is s on his opic.
Keywo ds:
na u al polyme s; aga ; chi in; chi osan; cellulose; collagen; ma ine polysaccha ides;
ma ine CAZymes
1. In oduc ion
Na u al polyme s, also known as biopolyme s, a e na u ally occu ing ma e ials,
o med du ing he li e cycles o li ing o ganisms. They can be de i ed om plan s (e.g., cel-
lulose), algae (e.g., aga ), animals (e.g., chi in and collagen), bac e ia (e.g., bac e ial cel-
lulose), and ungi (e.g., chi osan) (Figu e 1). Biopolyme s p esen unique p ope ies and
ad an ages, namely, high biocompa ibili y, lack o oxici y, biodeg adabili y, s abili y, a ail-
able unc ional g oups, and o en a e low cos . These p ope ies make na u al polyme s
in e es ing sus ainable al e na i es o eplace syn he ic polyme s in ma e ials de elop-
men . Thus, in he las decades, he e has been a p omp de elopmen and b eak h ough
in biopolyme science and echnology o be e unde s and hei undamen al and applied
biological, physicochemical, mo phological, and mechanical p ope ies [
1
–
7
]. Mo eo e ,
he challenging p ospec ion o no el na u al polyme s has led o undamen al disco e ies;
in pa icula , wi hin he ich oun o ma ine polysaccha ides, and hei ela ed enzymes
(ca bohyd a e-ac i e enzymes o CAZymes) ha ep esen ma ine mic oscopic li e [
8
–
10
].
Polyme s 2022,14, 1420. h ps://doi.o g/10.3390/polym14071420 h ps://www.mdpi.com/jou nal/polyme s
Polyme s 2022,14, 1420 2 o 20
Figu e 1. Chemical s uc u e o (A) aga ose, (B) cellulose, (C) chi in, (D) chi osan, and (E) collagen.
Hen i B aconno o Anselme Payen a e names ha a e e y well known in he biopoly-
me ield o hei ou s anding disco e y o chi in and cellulose. Maybe he names An-
gelina Fanny Hesse and Wanda Ki kb ide Fa a e no as widely ecognized as o he s
a e in he ield, howe e , he ou s anding idea o Hesse o use aga as cul u e media o
g owing mic oo ganisms in 1882 e olu ionized mic obiology [
11
]. In 1940, Fa disco e ed
he mechanism o cellulose o ma ion in he plan cell walls, answe ing a ques ion ha had
puzzled scien is s o a long ime [
12
]. Since he disco e y o hese polyme s, a numbe
o g ea wo ks ha e highligh ed hei impo ance and g ea ly implemen ed he wo k o
he pionee s o biopolyme science. Du ing he las 20 yea s, many esea ch eams ha e
dedica ed hei ime o biopolyme sciences and ha e led o se e al ad ances, disco e ies,
and inno a ions (Figu e 2), building upon he gene al knowledge o na u al polyme s [
13
].
In his pape , we wan ed o showcase some o hese ecen de o ed e o s by highligh ing
he wo k o women in es iga o s wo ldwide (bo h well- ecognized leade s and ising
s a s) in he biopolyme communi y. The aim o his pape is no o lis all he nume ous
accomplishmen s o women in he biopolyme science as i would be an impossible ask.
He ein, we a he wan o highligh some examples o scien i ic ad ances o some well-
known na u al polyme s ha ha e been made possible by he dedica ion o esea che s
in women-led eams.
Polyme s 2022,14, 1420 3 o 20
Figu e 2. Applica ions o biopolyme s. Rep in ed om e . [14].
2. Ad ances in Biopolyme Resea ch: Examples om Well-Known Biopolyme s
2.1. Aga
The use o aga as a gelling agen is e y ancien , and in pa icula , in se e al Sou heas
Asian cuisines. I is said ha i was disco e ed in he 17 h cen u y in Japan by an innkeepe
named Mino Ta
¯
ozaemon who no iced he jelli ica ion o a seaweed soup a e a nigh
a cold empe a u es. I was only in 1859 ha he chemis Anselme Payen subjec ed
aga , ex ac ed om he ed seaweed Gelidium co neum, o chemical analysis [
15
]. One o
he majo b eak h oughs conce ning he use o aga was i s u iliza ion as a solid medium o
he cul u e o mic oo ganisms. Al hough aga was i s desc ibed o use in mic obiology
in 1882 by he Ge man mic obiologis Wal he Hesse, an assis an wo king in Robe
Koch’s labo a o y [
16
], i was Fanny Hesse’s idea, Wal he Hesse’s wi e, o use aga as
an al e na i e o gela in. Since hen, he knowledge on aga , i s ex ac ion p ocesses, and i s
p ope ies ha e widely ex ended.
Aga is a collec i e e m used o desc ibe a mix u e o gelling polysaccha ides made
up o D- and L-galac ose. I has a linea suga skele on consis ing o al e na ing uni s o
1-4 linked 3-6-anhyd o-
α
-L-galac ose and 1-3-linked
β
-D-galac opy anose [
17
]. Aga can
be ac iona ed p incipally in o wo componen s, aga ose and aga opec in. Aga ose is
he gelling ac ion, and i is a neu al linea molecule wi h low le els o sulpha ion, while
aga opec in is he non-gelling ac ion cha ac e ized as a he e ogeneous mix u e o smalle
molecules including subs i u ed galac ose esidues and me hyla ed o sulpha ed suga
uni s. The ela i e p opo ions o aga ose and aga opec in a e known o a y be ween
species, locali y, and en i onmen al condi ions. Thus, he selec ion o aw ma e ial can be
used o sou ce speci ic aga unc ionali y [
18
]. Aga is mainly ound in he cell-ma ix o ed
seaweeds o he o de Gelidiales (Gelidium and P e ocladia) and G acila iales (G acila ia
and Hyd opun ia), which ha e become he majo wo ldwide sou ces [
19
]. The p op-
e ies o aga make i sui able o applica ions in di e se ields wi h high-added alue.
Fo ins ance, he mos common applica ions include ood, eed, cosme ics, pha maceu ical,
and bio echnology (mainly mic obiology as g ow h media o cul u ing bac e ia), bu po-
en ially eme ging applica ions may also include biomedical, ag icul u e, bioma e ials,
and bioplas ics.
The indus ial p oduc ion o aga is pe o med by adi ional ho wa e ex ac ion
du ing se e al hou s unde con en ional hea ing [
20
]. Howe e , his con en ional me hod
in ol es a la ge olume o wa e and high-ene gy equi emen s; hus, no el s a egies
Polyme s 2022,14, 1420 4 o 20
using eco- iendly echniques a e needed. In his sense, Ampa o López-Rubio and he
g oup ha e made an impo an con ibu ion, no only o he success ul ex ac ion o
aga om he ed algae Gelidium sesquipedale bu also o he use o eco- iendly me hods
ollowing he p inciples o ‘G een Chemis y’. Fo ins ance, Ma inez-Sanz e al. epo ed
he p oduc ion o aga -based ex ac s by applying ul asound- and mic owa e-assis ed
me hods, highligh ing he po en ial o hese al e na i e me hods o p oduce mo e sus ain-
able aga -based ex ac s o ood- ela ed applica ions [
21
,
22
]. Addi ionally, a u he s ep
in he sus ainable use o na u al sou ces by eco- iendly app oaches was pe o med by
Sag a io Bel án’s and Rod igo Melgosa’s g oup om he Uni e si y o Bu gos, Spain. They
ha e been wo king on he alo iza ion o he solid esidue gene a ed a e aga ex ac ion
om he ed algae G. sesquipedale [23].
In ecen yea s, he use o aga -based bioma e ials in eme ging a eas, such as issue
enginee ing o ‘sma ma e ials’, has gained g ea in e es . In his sense, he g oup o
Gonçal es and colleagues has made a signi ican con ibu ion. Fo ins ance, Sousa e al.
s udied he s uc u al and physicochemical p ope ies o aga ex ac ed om G acila ia
e miculophylla unde mic owa e hea ing [
24
–
26
]. In a u he s udy, he same esea ch
g oup in es iga ed he o ma ion o aga gels in aqueous media ocusing on he di e en
molecula assemblies o unde s and how hese associa ions can be modi ied o mee he spe-
ci ic needs o a gi en applica ion [
27
]. A e a deep cha ac e iza ion o aga and aga gels,
hey success ully epo ed he i s s udy o he p oduc ion o aga -based nano ibe s by
elec ospinning, opening new oppo uni ies o he ab ica ion o aga -based bioma e ials
in he o m o nano ibe s [28].
Ano he impo an applica ion o aga -based ma e ials is he p oduc ion o ilms o
ood packaging. Ko o De la Caba and he eam (Uni e si y o Basque Coun y, Spain)
ha e been ac i ely wo king on he p oduc ion o ood packaging om ma ine by-p oduc s.
Fo ins ance, hey epo ed he p epa a ion o aga -based ilms om G. sesquipedale using
a he mo-molding me hod o p oduce enewable and biodeg adable ilms [
29
–
31
]. Fol-
lowing a simila app oach, he g oup o Gonçal es and colleagues de eloped di e en
s a egies o imp o e he mechanical s eng h and wa e esis ance o aga ilms [
32
,
33
] and
p oposed al e na i e plas icize s o he p oduc ion o he mo-comp essed aga ilms [
34
].
Mo eo e , he g oup o Ampa o López-Rubio om he Spanish Na ional Resea ch Coun-
cil p esen ly wo ks on he p oduc ion o aga -based hyd ogels and bioac i e ae ogels as
ma ices o he con olled elease o bioac i e compounds in ood sys ems [
35
,
36
]. An o ig-
inal idea om he same g oup was o use aga ose o encapsula e p obio ic bac e ia and
imp o e hei iabili y du ing s o age, which is a p omising app oach o he p epa a ion
o p obio ic unc ional oods [37].
2.2. Chi in and Chi osan
Chi in has a scien i ic esea ch s o y o o e 200 yea s. I began in 1811 wi h he F ench
chemis Hen i B aconno , wi h chi in isola ion and cha ac e iza ion om some ungal
species. I was no un il 1859 ha Rougeu disco e ed ha chi in could be manipula ed
h ough chemical and empe a u e ea men s, wi h hea ed po assium hyd oxide, esul ing
in a soluble subs ance. This compound was named “chi osan” in he la e 19 h cen u y
by he Ge man scien is and physiologis Felix Hoppe-Seyle [
38
]. Since hen, esea che s
e o s ha e led o he disco e y o a ious sou ces o chi in, i s s uc u al cha ac e iza-
ion [
38
,
39
], and mo e ecen ly he isola ion o nanochi in [
40
]. In he las wo decades,
esea ch has ocused on imp o ing he p ope ies o chi in- and chi osan-based ma e ials,
ei he h ough hei combina ion o wi h o he ma e ials o ob aining de i a i es by unc-
ionaliza ion [
41
]. Ex ac ion echniques ha e also been imp o ed, which ha e e ol ed
om classical chemical ex ac ion o chi in o g een chemis y s a egies.
Chi in is a semi-c ys alline, high-molecula -weigh linea polysaccha ide made up o
β
-(1,4)-linked N-ace yl-2-amido-2-deoxy-D-glucose uni s [
42
]. The e a e wo p incipal ypes
o c ys alline iso o ms,
α
- and
β
-chi in. Those wo iso o ms di e on hei chain alignmen ,
which de e mines he inal physicochemical p ope ies o he chi in.
α
-chi in has a compac
Polyme s 2022,14, 1420 5 o 20
and highly c ys alline s uc u e ha esul s om an ipa allel chain a angemen ha
a o s s ong hyd ogen bonds, whe eas he less abundan
β
-iso o m is mo e eac i e and
has a high a ini y o sol en s due o i s pa allel chain a angemen ha p o ides weake
hyd ogen bonds [
43
]. This biopolyme is p esen in he cell wall o ungi and is he main
compound in he exoskele on o c us aceans and a h opods and is also p esen in mollusks,
hus making i he second mos abundan polysaccha ide on ea h a e cellulose. The majo
sou ce o chi in is he ma ine c us acean shells was e om he ishe ies indus y, such as
sh imp, lobs e , and c ab shells [44].
Rinaudo and colleagues made signi ican ad ances on he ex ac ion and cha ac e iza-
ion o chi in om di e en ma ine sou ces such as
α
-chi in om sh imp was e and c ab
shells and
β
-chi in om cu le ish bones [
43
,
45
–
47
]. They made also a g ea con ibu ion
o he op imiza ion o he dep o eina ion and demine aliza ion p ocesses om sh imp
shells. They ound ha an enzyma ic dep o eina ion by c ude mic obial p o eases led
o an
88 ±5%
dec ease o he p o ein con en , which is simila o he alkali dep o eina-
ion [48–50].
Al hough chi in p esen s in e es ing p ope ies o applica ions in he biomedical ield,
such as good biocompa ibili y, biodeg adabili y, low immunogenici y, and an imic obial
and wound healing ac i i ies, i s na u al insolubili y limi s i s use [
51
]. The e o e, chi osan,
he mos impo an de i a i e o chi in esul ing om i s deace yla ion [
44
], has gained g ea
in e es [
52
] because o i s highe solubili y, he ac ha i is posi i ely cha ged in acidic con-
di ions, p esen s he unique biological p ope ies o chi in, and has excellen ilm- o ming
p ope ies [
42
,
53
,
54
]. Chi osan and i s de i a i es ha e g ea po en ial in cosme ics, pha -
maceu ical, and biomedical applica ions such as deli e y sys ems o bioac i e ma e ials
o issue enginee ing [
55
,
56
]. The g oup o Lina Zhang has de eloped a la ge a ie y o
chi in and chi osan-based bioma e ials wi h p omising biomedical applica ions [
57
,
58
],
pa icula ly hyd ogels. Hyd ogels ha could se e as 3D cell cul u e pla o ms [
59
], cell
encapsula ion and d ug deli e y sys ems [
60
], and issue enginee ing sca olds [
61
] we e
de eloped by combining he ad an ageous bioac i e p ope ies o chi in and chi osan wi h
o he ma e ials. The new echniques de eloped by his g oup led o he concep ion o
elec oneu al and on-demand dissol able sel -healing hyd ogel sys ems [
62
,
63
]. Ano he
impo an con ibu ion o Zhang e al. was he c ea ion o chi in mic osphe es based on
a chi in solu ion in a NaOH/u ea aqueous sys em and he use o chi osan mic osphe es
as a sac i icial empla e [
64
,
65
]. This echnology has been success ully used in he biomedi-
cal ield o blood pu i ica ion he apy [
66
] and in issue enginee ing [
67
]. Ano he example
o chi osan alo iza ion comes om Eleono a Ma sich and colleagues, specialized in ca bo-
hyd a e polyme s. The eam ocused on he use o lac ose-modi ied chi osan, comme cially
known as CTL, o mimic biological ma ices [68–71].
In ecen yea s, he use o nanochi in has also gained a en ion because o i s in e -
es ing p ope ies a he nano scale, such as high su ace a ea and aspec a io, mechanical
p ope ies, and high an ibac e ial and an i-in lamma o y ac i i ies, among o he s [
72
].
Fo ins ance, he eam o Yimin Fan om he Nanjing Fo es y Uni e si y, China, de eloped
new me hods o isola e indi idualized wa e -dispe sed chi in nano ibe s and nanoc ys als
om bo h
α
- and
β
-chi in [
73
,
74
]. One o he mos p omising me hodologies was based
on he 2,2,6,6- e ame hylpipe idine-1-oxyl adical-media ed oxida ion (TEMPO) o chi in
ollowed by mechanical disin eg a ion in wa e [
75
]. In a u he s udy, Fan e al. de eloped
a simple p e ea men s a egy ha imp o ed he oxida ion e iciency o TEMPO-media ed
isola ion and educed he consump ion o he oxidan s, esul ing in a no el g een me hod-
ology [
76
]. Nanochi in can also be employed as nano ille o ob ain ein o ced composi es
o supe io mechanical and biological p ope ies [
77
]. Fo his pu pose, Col elli and col-
leagues wo ked on he use o chi in nano ib ils om ishe y biomass o de elop bio- and
eco-compa ible nanocomposi es. The inco po a ion o chi in nano ib ils as a ein o cing
agen in ex uded composi es based on biodeg adable polylac ic acid (PLA) imp o ed
he mechanical p ope ies and p o ided indi ec an imic obial ac i i y, esul ing in po en ial
bioplas ics o ood packaging and o skin issue egene a ion [
78
]. Recen ly, he same

Polyme s 2022,14, 1420 6 o 20
e ec was pe o med wi h cellulose-based bioplas ics o ood packaging [
79
]. Ano he
biomedical applica ion o chi in nano ib ils in combina ion wi h elec onega i e nanolignin
in mic ocapsule-like complexes was used o en ap and la e deli e bo h hyd ophobic and
lipophilic molecules [72].
These a e jus a ew examples o women esea che s wo king on chi in and chi osan.
Fo una ely, many o he women a ound he wo ld a e doing excellen wo k on his opic
and inno a ing, as is he case o Insiya Ja e jee, who is he co- ounde and CEO a Shell-
wo ks (h ps://www. heshellwo ks.com, accessed on 2 No embe 2021), a London-based
s a -up ha is de eloping a me hod o ans o m chi in in o a no el bioplas ic.
2.3. Cellulose
2.3.1. Cellulose and Nanocellulose
We ha e been widely using cellulose as a sou ce o ene gy and as a ma e ial o hou-
sands o yea s. None heless, i s i s isola ion om plan ma e and chemical s uc u e
iden i ica ion was unde aken by he F ench chemis Anselme Payen in 1838. Since hen,
mul i udinous scien i ic and echnological s udies ha e been made by se e al scien is s
a ound he wo ld on i s ex ac ion om di e en sou ces, es ablishmen o i s chemical
and physical s uc u e and mo phology, de elopmen o di e en ma e ials om pulp
and pape , composi es and packaging, o medical ma e ials and high- ech applica ions,
chemoenzyma ic modi ica ion, cellulose de i a i es, new ins umen a ion, and mo e e-
cen ly, isola ion o nanoc ys als and nano ibe s [
80
–
83
]. He ein, we will highligh some
wo ks de eloped by emale scien is s on (nano)cellulose-based ma e ials om plan s and
bac e ia (Figu e 3a–c).
Cellulose is a polysaccha ide ha is he main cons i uen o plan cell walls (Figu e 3a–c)
and he mos abundan na u ally occu ing biopolyme in he biosphe e. This linea homo-
polysaccha ide is composed o epea ing
β
-D-glucopy anose molecules ha a e co alen ly
linked h ough ace al unc ions be ween he equa o ial -OH g oup o he C4 and o he C1
ca bon a om [
84
]. Cellulose is insoluble in wa e and in mos common sol en s due o i s
s ong in e - and in amolecula H-bonding be ween i s indi idual chain uni s. Despi e i s
poo solubili y, i is used o a wide a ie y o applica ions in pape making, coa ing, pack-
aging, cons uc ion ma e ials, composi es, ood addi i es, and in he biomedical ields [
80
].
Owing o hei p ope ies, namely, biocompa ibili y, biodeg adabili y, non oxici y and
ecyclabili y, and excellen mechanical p ope ies, cellulose and i s de i a i es such as
ca boxyme hyl cellulose (CMC), cellulose ace a e (CA), me hyl cellulose (MC), hyd ox-
ye hyl cellulose (HEC), and (hyd oxyp opyl) me hyl cellulose (HPMC) ha e gained a lo o
a en ion [81,82].
In na u e, i p esen s a semic ys alline ib illa s uc u e o cellulose chains assembled
oge he o o m mic o ib ils, nano ibe s, and ibe s in ol ed s ongly wi h hemicellulose,
lignin, and esidual ino ganic elemen s. Using chemical and physical ea men s and/o
enzyma ic-assis ed ex ac ion, i is possible o ex ac cellulose ibe s o use in he many
applica ion sec o s men ioned be o e [
85
]. The wo k de eloped by El i a Fo una o and he
esea ch g oup a he New Uni e si y o Lisbon, Po ugal, is an example o one impo an
applica ion o cellulose ibe s. They ha e been wo king on he de elopmen o pape -
based ansis o s as an al e na i e o silicon-based componen s. These pape ansis o s
could be used in di e en applica ions in daily li e such as ‘sma ’ packaging, biosenso s,
anima ed billboa ds, and ne wo ked shipping labels (Pa en : EP2235741, EP2059810) [
86
,
87
].
Mo eo e , hese ma e ials a e p oduced a oom empe a u e and a e biodeg adable, which
educes he nega i e impac on he en i onmen .
Using op-down app oaches, om cellulose ibe s, i is possible o isola e nanocel-
lulose, i.e., less han 100 nm in one dimension: cellulose nano ibe s (CNF) and cellulose
nanoc ys als (CNC) [
81
,
82
,
88
]. These nanocellulose o ms, aside om he cellulose ibe
p ope ies, also exhibi high su ace a ea and aspec a io, making hese cellulose nano o ms
e y in e es ing o he de elopmen o nanoma e ials.
Polyme s 2022,14, 1420 7 o 20
Among he nume ous women wo king on his opic, K is iina Oksman (Luleå Uni e -
si y o Technology, Sweden), Aji Ma hew (S ockholm Uni e si y, Sweden), and A an xa
Eceiza (Uni e si y o Basque Coun y, Spain) ha e achie ed signi ican p og esses on
nanocellulose. These include: (i) he isola ion o nanocellulose (nano ibe s, nanoc ys-
als, o whiske s) om di e en o igins and sou ces such as mic oc ys alline cellulose
om No way sp uce, kena ibe s, beech pulp, and unbleached ice s aw among o he s
by using di e en isola ion app oaches, namely, chemical hyd olysis o physical o me-
chanical isola ion me hods such as e ining, high-p essu e homogeniza ion and ul a ine
g inde and hei cha ac e iza ion [
88
–
91
]; (ii) he p ocessing o unc ional ma e ials such
as nanocomposi es wi h in e es ing mechanical p ope ies [
92
–
94
], hyd ogels, ae ogels [
95
],
and memb anes o se e al applica ions [
96
,
97
]; and (iii) he cellulose-based ma e ial
de elopmen o biomedical applica ions; o example, as sca olds [83,98,99].
Pa icula a en ion has been ocused on cellulose-based nanocomposi es p esen ing
in e es ing mechanical p ope ies p epa ed using di e en app oaches. Fo ins ance, nanocom-
posi es made om cellulose nano ibe wi h s a ch powde we e in es iga ed by Oksman
eam. These composi es we e made using a win-sc ew ex usion p ocess. They ound ha
he mechanical p ope ies, as well as he mois u e sensi i i y o he he moplas ic s a ch,
we e imp o ed by p epa ing he nanocomposi es wi h he cellulose nano ibe s [
100
,
101
].
Fu he mo e, polylac ic acid-cellulose whiske nanocomposi es we e syn hesized by com-
pounding ex usion. The cellulose whiske s we e de eloped om mic oc ys alline cellulose
and he whiske s we e agg ega ed by s ong H-bonds [
93
]. These whiske s we e able o
imp o e he s o age modulus o polylac ic acid in he plas ic egion.
Much mo e wo k on cellulose-based ma e ials has been and will be ca ied ou by
bo h emale and male scien is s wo king oge he o indi idually [102–105].
2.3.2. Bac e ial Cellulose
On he o he hand, bac e ial cellulose (BC, Figu e 3a), also known as mic obial cellulose,
is a na u ally occu ing 3D ne wo k-based ma e ial p oduced as an exopolysaccha ide by
some ae obic bac e ia, such as hose om he genus Komaga aeibac e . This 3D ne wo k
is composed o nano- and mic o ib ils which a e 70–80 nm wide and 3–4 nm hick, being
100 imes hinne han ypical ege al cellulose ibe s [106].
The di e ence be ween plan -based cellulose and BC is pu i y, physicochemical and
mechanical p ope ies, and s uc u e. BC is o high pu i y ( ee o hemicelluloses and lignin
ha a e usually associa ed wi h plan cellulose), c ys allini y, and deg ee o polyme iza-
ion. Mo eo e , BC possesses ex emely highe wa e -binding capaci y, ensile s eng h,
and su ace a ea, as compa ed o he widesp ead plan -based coun e pa s [107–109].
The genus Komaga aeibac e is G am-nega i e ae obic and non-pho osyn he ic bac-
e ia capable o con e ing glucose, glyce ol, and o he o ganic subs a es in o cellulose
wi hin a pe iod o a ew days in he p esence o oxygen. BC can be p oduced using di e en
bac e ial cul u e media including s a ic, agi a ed, and bio eac o s. Gene ally, BC p oduc ion
in ol es expensi e cul u e media. Thus, he use o ag o o es y indus ial esidues could
o e come his limi a ion by se ing ca bon subs a es o he BC p oduc ion as demon-
s a ed by Ca men S R F ei e and collabo a o s a he Uni e si y o A ei o, Po ugal [
110
],
o by A an xa Eceiza and collabo a o s using pineapple ag oindus ial esidues [
111
]. An-
o he s udy epo ed on he possibili y o using esidues om he oli e oil p oduc ion
indus y as a ca bon sou ce o he p oduc ion o BC by Gluconace obac e saccha i [
112
].
Fu he mo e, he by-p oduc s o cide , when he apple pomace is mixed wi h suga cane,
was ound o be a po en ial ca bon sou ce o Gluconace obac e medellinensis [113].
When combined wi h o he ma e ials such as algina e, silk ib oin, chi osan, xy-
lans, and s a ch o o m biocomposi es, he mechanical and biological p ope ies o bac-
e ial cellulose-based unc ional ma e ials can be enhanced [
7
,
114
–
117
]. Cellulose-based
unc ional ma e ials a e gaining inc easing in e es in se e al indus ial ields such as
biomedicine, cosme ics, and bioelec onics [109,118].
Polyme s 2022,14, 1420 8 o 20
Ca men S R F ei e and collabo a o s ha e g ea ly con ibu ed o he esea ch ela ed o
BC-based ma e ials, namely, nanocomposi es, memb anes, ilms, e c., by using di e en ap-
p oaches such as physical and chemical modi ica ion, and polyme iza ion. These ma e ials
p epa ed using mainly BC p oduced by Ace obac e xylinum showed se e al encou aging
p ope ies such as a high mechanical s eng h and con olled d ug loading, making i a
p omising biopolyme o he p oduc ion o bioma e ials such as op ically anspa en
nanocomposi es o di e en kinds o applica ions [
7
,
114
–
117
,
119
–
123
]. As men ioned
abo e, hey chemically modi ied he s uc u e o BC o imp o e i s p ope ies. Fo example,
Tome e al. s udied BC memb anes wi h ailo ed su aces as well as ba ie p ope ies o
gases using con olled he e ogeneous es e i ica ion wi h hexanoyl chlo ide [
124
]. Mo eo e ,
Fe nandes e al. we e bio-inspi ed by he an imic obial p ope ies o chi osan, and chemi-
cally g a ed aminoalkyl g oups on he BC su ace, wi h he ensuing nano ib illa ne wo k
e ealing in e es ing an imic obial ac i i y and good mechanical p ope ies [116].
Figuei edo e al. om CICECO Labo a o y a he Uni e si y o A ei o, Po ugal,
p epa ed BC-poly(2-hyd oxye hyl me hac yla e) nanocomposi e ilms by in si u adical
polyme iza ion o 2-hyd oxye hyl me hac yla e, using poly (e hylene glycol) diac yla e
as c osslinke . The ilms hus o med we e diaphanous compa ed o BC and showed
imp o ed mechanical pe o mances as well as he mal s abili y when compa ed o poly
(2-hyd oxye hyl me hac yla e). As his nanocomposi e has p o en non- oxici y o hu-
man adipose-de i ed mesenchymal s em cells, i could be used o d y d essing applica-
ions [
123
]. BC-polycap olac one nanocomposi e ilms we e success ully syn hesized by
inco po a ing a iable amoun s o polycap olac one powde in o a BC cul u e medium.
The nanocomposi es hus o med could be used o ood packaging applica ions [125].
Figu e 3.
(
a
) Ex usion o a ne wo k o bac e ial cellulose nano ib ils wi h associa ed (nano) ib il c oss-
sec ional mo phology. (
b
) Mechanical disin eg a ion o plan ma e o p oduce NFC wi h associa ed
c oss-sec ional mo phology ha co esponds o a bundle o indi idual cellulose mic o ib ils. Cellulose
mic o ib ils a e p esen in he cell wall o wood, along wi h hemicelluloses, p o ein, and lignin.
(
c
) Biomechanical ho spo s occu a junc ions be ween wo o mo e mic o ib ils, o upon close
cellulose–cellulose con ac , media ed by ma ix polysaccha ides, such as coiled xyloglucan. Rep in ed
om e . [126].
Polyme s 2022,14, 1420 9 o 20
2.4. Collagen
F om he i s use o deg aded collagen as a glue mo e han a hund ed yea s ago o
oday’s cell he apy, wen y-eigh collagen ypes ha e been iden i ied and cha ac e ized
a molecula le el [
127
]. S uc u al cha ac e iza ion o collagen s a ed in he 1930s and
was g ea ly implemen ed by esea che s such as Ramachand an, he Nobel lau ea e C ick,
Pauling, Rich, and Yona h, and o he s including B odsky and Be man [
128
]. In 1985,
Mieczysław Sk odzki, An oni Michniewicz, and Hen yk Kujawa we e he i s o de elop
a me hod o isola e collagen di ec ly om ish skins. In he las 40 yea s, he esea ch on
collagen has g ea ly inc eased and has led o oday’s collagen he apeu ic applica ions.
Collagen is he mos abundan ib ous p o ein ound in he connec i e issues o a wide
ange o e eb a es and in e eb a e species. I is esponsible o p o iding s abili y
as well as s eng h o he issues and he eby gi es hem hei s uc u e [
129
]. Collagen
is a he e opolyme composed o h ee polypep ide chains in a iple-helical s uc u e.
Two o he h ee chains a e iden ical chains and he emaining one di e s in i s chemical
composi ion [
130
]. Collagen has widesp ead applica ions in nume ous ields, such as
pha maceu ical, medical, biomedical, ood indus y, cosme ics, e c. Majo ly, collagen has
been used o he cosme ic indus y, p ima ily o inc ease skin hyd a ion and p e en aging
o skin [131].
Collagen has been ex ac ed om a ious sou ces, mainly bo ine, po cine, and mu ine
animals. None heless, ma ine o ganisms a e now conside ed as an in e es ing al e na-
i e sou ce o collagen as hey a e sa e and easie o ex ac in compa ison o e es ial
sou ces [
132
]. The adi ional ex ac ion me hod o ob ain collagen om e es ial animal
sou ces is a mul i-s ep p ocess in ol ing he emo al o p o eins and pigmen s, a demine -
aliza ion wi h HCl o ace ic acid, as well as a inal diges ion using acid o an enzyme [
130
].
In he eigh ies, Syl ie Rica d-Blum and he eam s a ed wo king on he biochemical and
physicochemical cha ac e iza ion o collagen ex ac ed om e al cal ca ilage. The mino
disul ide-bonded collagen was isola ed using pepsin ea men [
133
]. Clai e Le hias’s
esea ch g oup om he F ench Na ional Cen e o Scien i ic Resea ch (CNRS) has been
ac i ely wo king on he isola ion o ma ine collagen om jelly ish such as Au elia au i a,
Co ylo hiza ube cula a,Pelagia noc iluca, and Rhizos oma pulmo om he Medi e anean sea
coas . The bes collagen yield was ob ained om Rhizos oma pulmo, and his ma e ial was
ound o ha e applica ions in he biomedical ield, such as o cell adhesion, p oli e a ion,
e c. [134–138].
Recen ly, Sionkowska e al. s udied he in luence o UV ligh on he heological p ope -
ies o collagen ex ac ed om he skin o he sil e ca p ish. They ound ha all he ace ic
acid collagen solu ions hey p epa ed we e showing a shea - hinning low beha io a e
UV i adia ion. They concluded ha , depending on he du a ion o he UV ea men ,
he collagen could be subjec ed o pho o-deg ada ion o c osslinking. These esul s we e
in e es ing as physically c osslinked collagen can be used o applica ions in he biomedical,
cosme ic, as well as in he ood indus ies [131,139,140].
Table 1summa izes he o igin, ex ac ion me hods, and applica ions o he desc ibed
biopolyme s.
Table 1. Biopolyme s’ o igin, ex ac ion me hods, and applica ions.
Biopolyme s O igin and Ex ac ion Me hods Re e ences
Aga
F om ed seaweeds o he o de Gelidiales and G acila iales
Ex ac ion me hods:
- ho wa e ex ac ion o se e al hou s [20]
- ul asound assis ed me hods [21,22]
- mic owa e-assis ed me hods [24–26]
Polyme s 2022,14, 1420 16 o 20
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