Organic-Inorganic Hybrid Materials

187 Pages·2021·20.819 MB·English

by  García-Martínez J.-M., Collar E.P. (ed.)

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Hybrid Materials
Edited by
Jesús-María García-Martínez and Emilia P. Collar
Printed Edition of the Special Issue Published in Polymers
www.mdpi.com/journal/polymers
Organic-Inorganic Hybrid Materials
Organic-Inorganic Hybrid Materials
Editors
Jesu´s-Mar´ıaGarc´ıa-Mart´ınez
EmiliaP.Collar
MDPI•Basel•Beijing•Wuhan•Barcelona•Belgrade•Manchester•Tokyo•Cluj•Tianjin
Editors
Jesu´s-Mar´ıaGarc´ıa-Mart´ınez EmiliaP.Collar
PolymerEngineeringGroup(GIP) PolymerEngineeringGroup(GIP)
PolymerScienceandTechnologyInstitute(ICTP) PolymerScienceandTechnologyInstitute(ICTP)
SpanishCouncilforScientificResearch(CSIC) SpanishCouncilforScientificResearch(CSIC)
Spain Spain
EditorialOffice
MDPI
St.Alban-Anlage66
4052Basel,Switzerland
ThisisareprintofarticlesfromtheSpecialIssuepublishedonlineintheopenaccessjournalPolymers
(ISSN2073-4360)(availableat:http://www.mdpi.com).
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ISBN978-3-0365-1301-0(Hbk)
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©2021bytheauthors. ArticlesinthisbookareOpenAccessanddistributedundertheCreative
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ThebookasawholeisdistributedbyMDPIunderthetermsandconditionsoftheCreativeCommons
licenseCCBY-NC-ND.
Contents
AbouttheEditors ........................................................................................................................................ vii
Jesu´s-Mar´ıaGarc´ıa-Mart´ınezandEmiliaP.Collar
Organic–InorganicHybridMaterials
Reprintedfrom:Polymers2021,13,86,doi:10.3390/polym13010086 . . . . . . . . . . . . . . . . . 1
CoroEcheverrı´a,MiguelRubioandDanielLo´pez
Thermo-ReversibleHybridGelsFormedfromtheCombinationofIsotacticPolystyrene
and [Fe(II) (4-Octadecyl-1,2,4-Triazole)3(ClO4)2]n Metallo-Organic Polymer: Thermal and
ViscoelasticProperties
Reprintedfrom:Polymers2019,11,957,doi:10.3390/polym11060957 . . . . . . . . . . . . . . . . . 5
WeiPeng,YingQian,TongZhou,ShenglinYang,JunhongJinandGuangLi
Influence of Incorporated Polydimethylsiloxane on Properties of PA66 Fiber and Its
FabricPerformance
Reprintedfrom:Polymers2019,11,1735,doi:10.3390/polym11111735 . . . . . . . . . . . . . . . . 21
XinxinSheng,SihaoLi,YanfengZhao,DongshengZhai,LiZhangandXiangLu
SynergisticEffectsofTwo-DimensionalMXeneandAmmoniumPolyphosphateonEnhancing
theFireSafetyofPolyvinylAlcoholCompositeAerogels
Reprintedfrom:Polymers2019,11,1964,doi:10.3390/polym11121964 . . . . . . . . . . . . . . . . 31
RosaBarranco-Garc´ıa,Jose´ M.Go´mez-Elvira,JorgeA.Ressia,LidiaQuinzani,EnriqueM.
Valle´s,ErnestoPe´rezandMar´ıaL.Cerrada
VariationofUltimatePropertiesinExtrudediPP-MesoporousSilicaNanocompositesbyEffect
ofiPPConfinementwithintheMesostructures
Reprintedfrom:Polymers2020,12,70,doi:10.3390/polym12010070 . . . . . . . . . . . . . . . . . 49
RuiP.C.L.Sousa,Ba´rbaraFerreira,MiguelAzenha,SusanaP.G.Costa,CarlosJ.R.Silva
andRitaB.Figueira
PDMS Based Hybrid Sol-Gel Materials for Sensing Applications in Alkaline Environments:
SynthesisandCharacterization
Reprintedfrom:Polymers2020,12,371,doi:10.3390/polym12020371 . . . . . . . . . . . . . . . . . 71
Adria´n Leone´s, Alicia Mujica-Garcia, Marina Patricia Arrieta, Valentina Salaris, Daniel
Lopez,Jose´MariaKennyandLauraPeponi
OrganicandInorganicPCL-BasedElectrospunFibers
Reprintedfrom:Polymers2020,12,1325,doi:10.3390/polym12061325 . . . . . . . . . . . . . . . . 89
SilviaVita,RicoRicotti,AndreaDodero,SilviaVicini,PerBorchardt,EmilianoPinoriand
MailaCastellano
Rheological, MechanicalandMorphologicalCharacterizationofFillersintheNauticalField:
TheRoleofDispersingAgentsonCompositeMaterials
Reprintedfrom:Polymers2020,12,1339,doi:10.3390/polym12061339 . . . . . . . . . . . . . . . . 105
NantikanPhuhiangpa,WorachaiPonloa,SareePhongphanphaneeandWirasakSmitthipong
Performance of Nano- and Microcalcium Carbonate in Uncrosslinked Natural Rubber
Composites:NewResultsofStructure–PropertiesRelationship
Reprintedfrom:Polymers2020,12,2002,doi:10.3390/polym12092002 . . . . . . . . . . . . . . . . 117
v
Ba`rbaraMico´-Vicent, MarinaRamos, FrancescaLuzi, FrancoDominici, Valentı´nViqueira,
LuigiTorre,AlfonsoJime´nez,DeboraPugliaandMarı´aCarmenGarrigo´s
EffectofChlorophyllHybridNanopigmentsfromBroccoliWasteonThermomechanicaland
ColourBehaviourofPolyester-BasedBionanocomposites
Reprintedfrom:Polymers2020,12,2508,doi:10.3390/polym12112508 . . . . . . . . . . . . . . . . 133
Jesu´s-Mar´ıaGarc´ıa-Mart´ınezandEmiliaP.Collar
OntheCombinedEffectofBoththeReinforcementandaWasteBasedInterfacialModifieron
theMatrixGlassTransitioniniPP/a-PP-pPBMA/MicaComposites
Reprintedfrom:Polymers2020,12,2606,doi:10.3390/polym12112606 . . . . . . . . . . . . . . . . 153
YuxiaLiang,XiaonanHuang,LanzhongYao,RuXia,MingCao,QianqianGe,WeibinZhou,
JiashengQian,JibinMiaoandBinWu
RegulationofPolyvinylAlcohol/SulfonatedNano-TiO2HybridMembranesInterfacePromotes
DiffusionDialysis
Reprintedfrom:Polymers2021,13,14,doi:10.3390/polym13010014 . . . . . . . . . . . . . . . . . 167
vi
About the Editors
Jesu´s-Mar´ıa Garc´ıa-Mart´ınez holds a Ph.D. in Chemistry (Chemical Engineering) by the
UniversidadComplutensedeMadrid(1995). Additionally, heholdstwoM.Sc. leveldegreesand
hascompletedmorethan70highlyspecializedcoursesinindustrialchemistry;polymerscienceand
technology; quantitative research; environmental science; materials science and characterization;
R+D+i management, modelling of processes; quality systems in R+D+i, educational sciences,
philosophyofscience,andsoon. HeisaTenuredScientistattheInstituteofPolymerScienceand
Technology(ICTP)oftheSpanishNationalResearchCouncil(CSIC).Since1992,withinthePolymer
Engineering Group (GIP), he has co-authored more than 175 scientific and/or technical works
in the topics related to polymer engineering, chemical modification of polymers, heterogeneous
materials based on polymers, interphases and interfaces, polymer composites blends and alloys,
organic-inorganic hybrids materials, polymer recycling, quality, and so on. Dr. Garc´ıa-Mart´ınez
has participated in more than 31 research projects financed with either public (national and
internationalprograms)orindustrialfunds,andisco-authorofonecurrentlyactiveindustrialpatent
onpolymerrecycling. Asanadditionaltasktohisscientificresearch, intheperiod2000–2005, he
assumedthepositionofQualityDirectorfortheICTP(CSIC)ISO17025AccreditationProjectofthe
ICTP Laboratories (ACiTP) under the auspices of the ICTP (CSIC) Directorate. Additionally, Dr.
Garc´ıa-Mart´ınezplaysaveryactiveroleinreviewingtasksforWOSandSCOPUSindexedjournals,
withmorethan250reportsinthelastyears. Infact,hehasbeenawardedtwicewiththePublons
Reviewer Awards (2018, and 2019), and once with the POLYMERS Outstanding Reviewer Award
(2019)fortheseactivities. Since2016,heistheHeadoftheDepartmentofChemistryandProperties
ofPolymerMaterialswithintheICTP(CSIC).
EmiliaP.Collar, Ph.D.inIndustrialChemistry(U.Complutense, 1986), joinedin1990atthe
permanentstaffattheConsejoSuperiordeInvestigacionesCient´ıficas(CSIC),servingasaTenured
Scientist, after two-years (1986–88) as CSIC’s postdoc fellow, and one more (1989) as Chemical
EngineeringAssistantTeacherattheUniversidadComplutensedeMadrid. AtthePolymerScience
andTechnologyInstitute(InstitutodeCienciayTecnolog´ıadePol´ımeros), ICTP/CSIC,sheworks
at the Polymer Engineering Group (GIP), founded in 1982 by Prof. O. Laguna, being the GIP’s
Headfrom1999. Between1990and2005,shesupervisedsixdoctoralthesesandfivepost-graduate
ones,developedunder14researchprojects(publicfundssupported),aswellas18researchcontracts
(privatefundssupported),issuing53technicalreportsfordifferentcompanies.From2001to2005,she
performedthepositionsofTechnicalDirectorofthePhysicalandMechanicalPropertiesLaboratory,
LFM,andDeputy-TechnicalDirectoroftheThermalPropertiesLaboratory,LPT,underthesuccessful
ISO17025AccreditationProjectfortheCSIC/ICTP’sLaboratories,ACiTP,commandedbytheICTP’s
Head.Authorandco-authorofmorethantwentychaptersonbooks,twocurrentlyactiveindustrial
patentsonpolymerrecycling,andmorethanonehundredandfiftyresearchpapersmostlyonSCI
Journals,herresearchworklinesdealwithpolymersandenvironmentunderthegeneralframeof
heterogeneousmaterialsbasedonpolymers(PolymersandEnvironment; PolymerRecycling; Polymer
Blends; Composites; Interface Optimization; Interfacial Agents; Chemical Modification of Polymers; Blend
Technologies;MorphologyandModeling).From2006todate,shehasparticipatedinthreeSpanishpublic
fundedresearchprojectsandoneEUpublicfundedprojectunderits7thFrameworkProgram.
vii
polymers
Editorial
Organic–Inorganic Hybrid Materials
Jesús-MaríaGarcía-Martínez*andEmiliaP.Collar*
PolymerEngineeringGroup(GIP),PolymerScienceandTechnologyInstitute(ICTP),
SpanishCouncilforScientificResearch(CSIC),C/JuandelaCierva,3,28006Madrid,Spain
* Correspondence:[email protected](J.-M.G.-M.);[email protected](E.P.C.)
AccordingtotheIUPAC(InternationalUnionofPureandAppliedChemistry),ahy-
bridmaterialisthatcomposedofanintimatemixtureofinorganiccomponents,organic
components,orbothtypesofcomponentswhichusuallyinterpenetrateonscalesofless
than1μm[1].Thisdefinitionmatchesthesubjectofallthearticlespublishedinthisspecial
issue.Thus,theconceptoforganic–inorganichybridmaterialscanbeappliedtoabroad
numberofapproaches.Inthesameway,theso-calledorganic–inorganicmaterialscanbe
revealedasmulti-componentcompoundshavingatleastoneoftheirorganic(thepolymer)
orinorganiccomponentinthesub-micrometricand,moreusually,inthenano-metricsize
domain[2].Further,theorganic–inorganichybridsystemscanbeclassifiedintotwoclasses
namedclassIandClassII,dependingoniftheinteractionofthephasesisweakorstrong,
respectively[2].Thelatterdependsonthetypeofinteractions:VanderWaals,hydrogen,
electrostatic,andotherinteractionsforClassI,andduetorealchemicalbondsbetween
phases(ClassII),thecoexistenceofbothtypesofinteractions(IandII)inthesamesystemis
possible[2].Insuchascenario,thisissueincludesawiderangeoftopicscoveringthesedef-
initions.Consequently,theorganic–inorganicmaterialsarerevealedasmulti-component
compoundshavingatleastoneoftheirorganic(thepolymer)orinorganiccomponent
inthenano-metricsizedomain,andusuallyoffersmuchbetterperformancethantheir
non-hybridcounterparts[2–6].
(cid:2)(cid:3)(cid:4)(cid:2)(cid:5)(cid:6)(cid:7)(cid:8)(cid:9)
(cid:2)(cid:3)(cid:4)(cid:5)(cid:6)(cid:7)(cid:8) Undertheabove-mentionedpremises,thisspecialissuecompiles11articleswrittenby
expertsinthefieldandaredevotedtotheverydifferentapproachescoexistinginthefield.
Citation:García-Martínez,J.-M.; Inthiscontext,thefirstarticlebyEcheverría,Rubio,andLópez[7]studiesofthermo-
Collar,E.P.Organic–InorganicHybrid
reversibleorganic–inorganichybridgelsbymeansofthermalandviscolesticproperties.
Materials.Polymers2021,13,86.
Forsuchpurposes,theyusedsynthetizedhybridthermo-reversiblegelsbycombining
https://doi.org/10.3390/
a metallo-organic polymer and isotactic polystyrene with the purpose of solving the
polym13010086
poormechanicalpropertiesofthesetypesofcompounds. Theywereabletodetermine
Received:24December2020 threetransitionsuponheating(monotectictransitionoftheiPSgel,meltingoftheiPSgel,
Accepted:25December2020 andmeltingofthemetal-organicpolymergel)suggestingthatthetwopolymersareformed
Published:28December2020 independentlyinthehybridgel,concludingthatthesehybridgelsareinterpenetrated
organic/metallo-organicnetworks.
Publisher’sNote: MDPIstaysneu- Lietal.[8]investigatedtheinfluenceofincorporatingpolydimethylsiloxaneonthe
tralwithregardtojurisdictionalclaims propertiesofPA66fiberfabrics,obtainedbymeltblendspinning,byproducingfiberswith
inpublishedmapsandinstitutional excellentmechanicalpropertiesandreducedhotshrinkage,withoutremarkableeffecton
affiliations. crystallizationandmeltingbehaviorofPA66.Thus,theeffectoftheadditiveonthesurface
tensionsuggeststheantifouling,waterproof,andstain-resistantabilityofthefiberandits
fabric.Theseresultsarecomparedwithsilicon-coatedfibers,resultingintheproposition
bytheauthorsofthecompoundshavingmanypropertiesbesidesbeingecofriendly.
Copyright:©2020bytheauthors.Li-
Relatedtothehottopicoffireresistancematerials,Sheng,Lu,andco-workersreport
censeeMDPI,Basel,Switzerland.This
astudyaboutit[9].So,thisarticleisdevotedtofireandsmokesuppressionsofpolyvinyl
articleisanopenaccessarticledistributed
alcohol(PVA)aerogelsinordertoavoidthefirehazardthattheypresent. Forthispur-
underthetermsandconditionsofthe
CreativeCommonsAttribution(CCBY) pose,theauthorsuseda2Dtransition-metalcarbideforenhancingtheflame-retardant
license(https://creativecommons.org/ performanceofPVA/ammoniumpolyphosphate-basedcomposites.Theresultsdemon-
licenses/by/4.0/). stratedthatthepresenceofthecarbideinlowamountscanboosttheflameretardanceof
1
Polymers2021,13,86.https://doi.org/10.3390/polym13010086 https://www.mdpi.com/journal/polymers
Polymers2021,13,86
thecompositesevenastopassasV-0rated.Furthermore,theauthorsdemonstratethat
thepresenceofthecarbidegreatlyreducesthereleaseofheatandsmoke,provingthe
synergisticeffectoftheammoniumphosphateandthecarbideusedfortheobjectiveof
thestudy.
Aninvestigationaboutthechangesobservedontheultimatepropertiesofisopropylene–
mesoporoussilicananocompositesobtainedbyextrusioncausedbytheeffectofthepoly-
mersconfinementwithinthemesostructuresisthesubjectofthearticlebyCerradaand
workinggroup[10].Thestudyconcludesthekeyroleofporesizeintheconfinementof
iPPchainswithinthenanometricmesostructuresofthesilicasused,affectingthethermal
stabilityandtheultimatepropertiesofthematerials.Themainconclusionsofthework
weretherelatedeffectofthesilicaonthepolypropyleneobservedthroughthedegradation
andtherheologicalbehaviorofthecomposites,whichisexplainedbyvariationsinthe
inclusionofthepolymerchainswithinthemesostructuresofthesilicasused.Thelatter
wasdemonstratedbysynchrotronSAXSmeasurements.
Sincethecarbonationofconcreteisaprimeproblemincivilengineering,thepaperby
Sousa,Ferreira,andco-workers[11]isrelatedtothereductionofthisconcretedegradation
bytheeffectoforganic–inorganichybridfilmsforthepotentialfunctionalizationofoptical
fibersensorstobeappliedinconcretestructures. Virginfilmsandthosedopedwith
phenolphthaleinwerecharacterizedbyaseriesoftechniquesandtheresultsobtained
werehighlypromisingregardingthepropertiesunderhighalkalinescenarioscausing
concretecarbonation.
Byconsideringtheincreasingimportanceofadditiveprocessing,theworkbyPeponi
etal.[12]isfocusedonthefabricationoforganicandinorganicpoly(e-caprolactone)-
basedelectrospunfibersinordertoobtaindifferentnanocompositematsbasedonpoly(e-
caprolactone),PCL,reinforcedwithaseriesofbothorganicandinorganicnanoparticles
(just1%). Asorganicparticles, theauthorsusedcellulosenanocrystals(producedby
them)andcommercialchitosanandgraphene,whiletheinorganiconesweresilverand
hydroxyapatiteparticles.Theauthorsfoundnoappreciabledifferencesintermsofthermal
parameters. The authors conclude that while the flexibility of the mats increases for
whatevertypeofparticleincorporated,thestiffnessofthesystemincreasesonlyinthecase
ofsilverorgrapheneparticleispresentinthemat.
Theeffectofthedispersingagentswithanionicorstericactionontheinteractions
betweenhollowglassmicrospheresandanepoxy-polyamideresinoncompositematerials
fornauticalapplicationsarestudiedbyDodero,Vicini,andcolleagues[13].Thecomposites
areevaluatedbymeansoftherheologyoftheun-crosslinkedmaterialaswellasmechanical
andmorphologicalpropertiesofthecrosslinkedcomposites.Theauthorsconcludethat
stericdispersingagentsoffermuchbettercompatibilitythanioniconesbasedontheir
hindrancecapability,andsoabetter-performingcompositewithaless-markedPayneeffect
isobtained.Theauthorsclaimtobethepioneersinstudyingtheroleofdispersingagents
forthistypeofmaterialincomparisontothemerelyempiricalapproachesfollowedforthe
preparationoffillersforthistypeofcomposite.
Smitthipongandcoworkers[14]studiedtheperformanceofnano-andmicro-calcium
carbonatefillersinthefinalpropertiesofun-crosslinkednaturalrubbercompounds,bypay-
ingattentionthehighcostreductionforindustryandthehalfreinforcingcharacterof
thistypeoffillerspromotingbettermechanicalproperties. Theauthorsfoundasimilar
tendencyofresultswiththeindependenceofthenanoormicrocharacterofthenano-filler
used;theyalsoshowtheimportanceandinfluenceofthespecificsurfacearea.However,
theauthorsconcludetheeffectofthespecificsurfaceareaonthefinalproperties,aswellas
thetheoreticalmodelswhichagreewiththeresults.Additionally,theyshowed(through
time–temperaturesuperpositionmastercurves)wherethehigherfilledcompositesex-
hibited lower free volume. Finally, they conclude about the real possibility of using
nano-calciumcarbonatematerialfortheproductionoftailorrubber-basedproducts.
Sincebio-basednanocompositeshaveemergedasahottopic,Garrigos,Puglia,andcol-
leagues[15]havestudiedtheeffectofchlorophyllhybridnanopigmentsobtainedbycom-
2
Polymers2021,13,86
biningchlorophylldye(obtainedfromagro-foodwastes),calcinedhydrotalcite,andmont-
morillonitenanoclay,onthefinalcolorandthermomechanicalproperties,byusingstatisti-
caldesignofexperiments,DOEs.Inthisway,theauthorswerecapableofidentifyingthe
moreimportantparametersinfluencingthemechanical,thermal,structural,morphological,
andcolorpropertiesofthebionanocompositesstudied.Hence,thepotentialuseofgreen
naturaldyesfrombroccoliwastes,adsorbedintonanoclays,havebeenproventobevery
interestinginthedevelopmentofnaturallycoloredbionanocomposites.
Attending to the fact that the interphase between the organic and the inorganic
componentsofthehybridmaterialiswhatgovernstheirultimatebehavior,García-Martínez
andCollar[16]investigatedthecombinedeffectofthereinforcementandtheinterfacial
agentinapolypropylene-basedcomposite.Inthearticle,theauthorsstudiedmicaplatelets
andapolymerwasteinterfacialmodifierconsistingofagraftedatacticpolypropylenewith
attachedp-phenylen-bis-maleamicacidpolargroups,bypayingattentiontothechangesof
theglasstransitiontemperature.ByusingBox–Wilsonexperimentaldesigns,thearticle
focusesonthepredictionofhowthisparameterchangesasafunctionofboththeinterfacial
agentandthenano-reinforcementbytakingintoconsiderationthecomplexcharacterof
theiPP/aPP-pPBMA/micasystem,whereintheinteractionbetweenthecomponentswill
definethefinalbehavior,andthattheglasstransitionisadesignthresholdfortheultimate
propertiesofpartsbasedinthistypeoforganic–inorganichybridmaterials.Hence,thefinal
purposeoftheworkisthepredictionandinterpretationoftheeffectofbothvariables
onthiskeyparameter, beingidentifiedthesamecriticalpointsasbyotherproperties
suchasflexural,tensile,impact,andthermalproperties,asdeterminedpreviouslyby
theauthors[16].
Finally,byfocusingtheattentiononthefactthatistheadjustmentoftheorganic–
inorganic interfacial chemical environment which plays a key role for the separation
performanceofcompositematerials,Miau,Wuetal.[17]focusedtheirattentiononthe
regulationabouthowapolyvinylalcohol/sulfonatednano-TiO2hybridmembranesinter-
facepromotesdiffusiondialysis.Forsuchpurposes,theauthorsinvestigatedthebehavior
ofaseriesofhybridmembranesfabricatedbycombiningpolyvinylalcohol(PVA)and
sulfonatednano-TiO2(SNT).Infact,theyregulatetheeffectsoftheinterfacialchemicalsur-
roundingsoniontransferasafunctionoftheSNTcontenttoaffectthedialysiscoefficients
ofboththehydroxylionsandtheseparationfactorsinordertobeofanadequateinterval
astomakethesulfonicgroupsintheinterfacialregionsandthehydroxylgroupspresent
inthePVAmainchain.Thiscanhaveimportantrolesduringthetransportofsodiumand
hydroxylions.Moreover,theauthorsidentifiedamembranewithoptimalperformancein
thecaseof3%ofSNT.
Heterogeneousmaterialsbasedonorganicpolymers(asawholeorasapart)can
playanessentialrolesinthefightagainstCOVID-19.Infact,theycanbekeymaterialsfor
fabricatingpreventiveandisolationclothingforthemedicalteamsinclosecontactwith
illpatients,forlifesupportequipment,containment,andtransportthereof.Additionally,
organic–inorganichybridmaterialsremaintherealmforotherdiverseapplicationssuchas
controlleddosingofdrugs,membranesystems,multi-componentpackaging,andamyriad
ofaccessoriesandsanitaryitemsingeneral. Thechallengeofcontinuallyattendingto
newdemandsremains.Thelatterconstitutestheprimemotivationandconcernforhybrid
materialsresearch.Thisextensivelyappliestotheworkscompiledinthisspecialissue.
Wethankalltheauthorsfortheircontributionsandencouragethemtopursuewith
theirresearch.
Funding:Thisresearchreceivednoexternalfunding.
ConflictsofInterest:Theauthorsdeclarenoconflictofinterest.
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