Construction of a Superhydrophobic Sodium Alginate Aerogel for E ffi cient Oil Absorption and Emulsion Separation - Yang et al. - 2021 -

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pubs.acs.org/LangmuirArticleConstructionofaSuperhydrophobicSodiumAlginateAerogelforEfficientOilAbsorptionandEmulsionSeparationYushuangYang,XiupingChen,YimingLi,*ZichaoYin,andMutaiBaoCiteThis:Langmuir2021,37,882−893ReadOnlineACCESSMetrics&MoreArticleRecommendations*sıSupportingInformationABSTRACT:Bio-basedaerogelsserveaspotentialmaterialsinseparationofoil/watermixtures.Nevertheless,thereremainsomekeychallenges,includingexpensive/toxicorganiccross-linkers,unpromisingreusability,andpoorperformanceinemulsionseparation.Hereby,anovel,robust,andsuperhydrophobicsodiumalginate/grapheneoxide/siliconoxideaerogel(SA/GO/SiO2-M)wasfabricatedbysimplecalciumioncross-linkingself-assembly,freeze-drying,andchemicalvapordepositionmethodsbasedontherenewableandabundantrawmaterials.Theas-preparedSA-basedaerogelpossesseshighabsorbencyforvarietiesoforganicsolventsandoils.Importantly,itshowshighefficiencyintheseparationofsurfactant-stabilizedwater-in-oilemulsions.SA/GO/SiO2-Maerogelsdisplayexcellentreusabilityinbothabsorptionandseparationbecauseoftheirgoodmechanicalpropertiesintheairandoilphase,andthemechanisminemulsionseparationisdiscussed.ThisstudyshowsthatSA/GO/SiO2-Maerogelsareapromisingmaterialintreatingoilcontaminantsfromdifferentfields.■INTRODUCTIONanimalresiduesareinexhaustible,renewable,andenvironment-12−14friendly.SeparatingoilfromwaterisofsignificanceinresolvingtheTheaerogelforoil/watermixtureseparationusuallyneedsaticklerofoilspill,industrialoilyeffluent,andotheroil1,2properthree-dimensional(3D)architecturesubstrateandapollutionfields.Variousoil/waterseparationtechniquesselectivewettabilitysurface.Thepreparationofanaerogelhavebeendevelopedinrecentyears.Intermsofthesolutionsubstratemainlyincludestwosteps,namely,sol−gelandtooilspill,physicalabsorptionandseparationmethodshavedrying.Physicalorchemicalcross-linkingisusuallyemployedattractedmuchattentionfromresearchersbecauseoftheir3−5topromotetheformationofa3Dnetworkstructureintheconvenienceandrecyclability.Industrialoilwastewaterestablishmentofasubstrate.Jiangetal.adoptedgelatinastheusuallyexistsintheformofstableemulsionswithmicrometer3Dscaffoldmaterialandthenbranchedpolyethylenimineontoparticlesize(d<20μm).Acommonmethodtoseparate15ittoobtainacompositeaerogel.Zhangetal.attachedemulsifiedoilfromwateristoutilizeseparationmaterialswith6−8cyanuricchlorideontonanocrystallinecelluloseandusedDownloadedviaUNIVOFPRINCEEDWARDISLANDonMay16,2021at11:54:07(UTC).aspecificwettabilityandasuitableporesize.Therefore,chloropropyltriethoxysilaneasacross-linkertoobtainaSeehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.materialsthatpossessthecapabilityofabsorptionand16cellulose-basedaerogel.Thehydrophobicmodificationofseparationaregreatlyexpectedinthefieldofoil/watermixturetheobtainedaerogelsubstratemainlyreferstopyrolysisortheseparation.useofhydrophobicmodificationreagents.ThepyrolysisofAerogels,especiallyfunctionaloneswithspecialwettabilityaerogelsrequiresanextremelyhightemperatureandaninertandinterconnectedporousstructures,havebeenconsideredas17environment,implyingthatthemanufacturingprocessneedsoneofthepromisingmaterialstodealwiththeproblemofoil/muchcostandenergy.Bycontrast,hydrophobicmodificationwatermixtureseparationinrecentyearsowingtotheirreagentsareeasytocontrol,andtherefore,theyarewidelyfollowingadvantages:(1)therichporestructureandlarge18employedbyresearchers.Consideringtheactualapplicationspecificsurfaceareaareconducivetotheabsorptionand9inthecomplicatedconditionsofoil/watermixtureseparation,storageofoil;(2)intermsofseparation,aerogelsprovidealongpathofemulsionpenetration,andtheirsurfacewithaspecialwettabilityenhancestheinterceptionandcoalescenceReceived:November9,2020ofwaterdroplets;10(3)aerogelspossessadvantagessuchasRevised:December22,2020lowdensity,recyclability,lesssecondarypollution,andsoon.11Published:January8,2021Amongvarioustypesofaerogels,bio-basedaerogelshavebeenrecognizedasoneofthemostcutting-edgecandidatesowningtothefactthatbio-basedmaterialsfromnaturalplantsand©2021AmericanChemicalSocietyhttps://dx.doi.org/10.1021/acs.langmuir.0c03229882Langmuir2021,37,882−893

1Langmuirpubs.acs.org/LangmuirArticleFigure1.SchematicillustrationofthesynthesisoftheSA/GO/SiO2-Maerogel.researcherscontinuallystriveforthedevelopmentofsimpleselectivewettability,oilabsorption,andemulsionseparationmethodstoobtainaerogelmaterialswithmaximumpotentialcapability,havebeeninvestigatedindetail.Asexpected,theforoilabsorptionandseparation.SA/GO/SiO2-Maerogelshowsaproperporousstructure,lowSodiumalginate(SA),extractedfrombrownalgae,isoneofdensity,selectiveoilabsorptioncapacity,andhighefficiencyofthemostabundantnaturalpolysaccharideswiththeadvantagesemulsionseparationforvariousoils.TheadvantagesofthisSA-oflowcost,biocompatibility,nontoxicity,andconvenientionicbasedaerogelalsoincludegoodmechanicalproperties,agreen19cross-linking.Studiesonalginate-basedhydrogelsandpreparationenvironment,andamildmodificationmethod,aerogelshavebeenextensivelycarriedoutinvariousfieldswhichdemonstratesthatSA/GO/SiO2-Misanattractive202122suchasfoods,medicine,andchemicalengineering,etc.candidateforoil/waterseparation.Mostimportantly,theNevertheless,poormechanicalpropertiesandhighhydro-mechanisminseparatingemulsionsbyaerogelsisdiscussed,philicitygreatlylimittherecyclabilityandoilseparationwhichenrichesworksinemulsionseparationapplicationsbycapabilityofalginate-basedaerogels.Toovercomethisaerogels.drawback,addingreinforcingagentsisagoodchoice.Twokindsofalginate-basedaerogelsSA/MBAandSA/CMChavebeenpreparedandusedasoil-absorptivematerials.23AnSA/■EXPERIMENTALSECTIONMaterials.SAandmethyltrimethoxysilane(purityof>98%,TiO2aerogelwithagoodantifoulingpropertyshowedan24MTMS)werepurchasedfromSinopharmChemicalReagentCo.,excellentoil/waterseparationperformance.Inthisstudy,Ltd.(China).Graphite,D-gluconicacidδ-lactone(DGL),andn-grapheneoxide(GO),oneofthemostprevalentcarbontetradecane(purityof>98%)weresuppliedbyAladdinHoldingsmaterialsinrecentyears,isemployedasareinforcingagentGroup(China).KerosenewaspurchasedfromMacklin(China).baseduponitsexcellentfeatures.GOwithrichhydroxyl,Dieseloilwaspurchasedfromalocalgasstation.Crudeoilinthisepoxy,andcarboxylgroupscanassemblewithSAthroughexperimentwastakenfromtheHaierstationintheShengliOilfieldinhydrogenbonding,whichmightgreatlypromotetheformationChina.OtherreagentsusedinthisstudywereobtainedfromShanghaiofaninterconnectivestructure.25GOalsocouldenhancetheHushiLaboratoryEquipmentLimitedCompany(China).Thewatermechanicalpropertyofaerogelsbecauseofitsrigidtwo-usedwasdeionizedwaterinallexperiments.26PreparationofGOandSiO2.Grapheneoxide(GO)wasdimensionalsheet-likestructure.Additionally,thelarge33preparedbyemployingamodifiedHummers’methodasfollows.specificsurfaceareaofGOisexpectedtobefavorablefor27First,graphite(3.00g),H2SO4(0.36L),andH3PO4(0.09L)wereabsorption.Toachieveselectiveoilabsorption,demulsifica-mixed.Then,KMnO(18.00g)wasdividedinto6equalportionsand4tion,andevenemulsionseparation,theobtainedSAaerogelslowlyaddedintothemixture,producingaslightexothermicreactionsubstrateneedstobeendowedwithsuperhydrophobic/thatshouldnotexceed35−40°C.Afterthat,thereactionwasheatedsuperoleophilicitycharacteristics.Theprocessofconstructingto50°Candthenstirredfor12h.Next,thereactionmixturewasasuperhydrophobicsurfaceencompassestwoessentialparts:28cooledtoroomtemperature,andice(0.40L)and30%H2O2(3.00(1)increasingsurfaceroughnessand(2)reducingsurfacemL)weredroppedintotheabovesolution.Thesolidmaterialswereenergy.Basedonthis,SiOnanoparticlesareselectednotonlywashedbywater,HCl,andethanolsuccessivelyandseparatedby2centrifugation.Thecleansedimentwasfreeze-driedat−60°Cunderbecauseoftheirpropernanoscaleformbutalsobecauseofvacuumfor24h.Whenused,thedriedGOwasdispersedintoatheirlowcost,nontoxicity,easymodification,andmechanical29suspension.ThecrystalstructureofGOwasanalyzedbyX-raystrengthproperties.Methyltrimethoxysilane(MTMS),adiffraction(XRD,D2PHASER,Germany)inthe2θrangefrom5tocommonsilanecouplingagent,ischosenasamodified80°withascanningrateof5°/min,andthecorrespondingspectraarereagent,andthestrongvolatilityofMTMSisusedtoachieveshowninFigureS1.3034chemicalvapordeposition(CVD)duetothemildreactionSiO2particleswerepreparedbasedupontheStöbermethod.temperatures,low-costchemicals,andsimplereactiondevicesBriefly,4.50mLofammonia,89.50mLofethanol,and31.00mLofoftheCVDmethod.31,32waterweremixed,andthen,7.95mLoftetraethylorthosilicatewasBasedontheaboveideas,inthiswork,bydispersingSiOslowlyaddedintothemixture.After2hstirringatarotationrateof2nanoparticlesinthemixedliquidofSAandGO,a150rpm,SiO2particleswereprepared.Theseparticleswereseparatedbycentrifugation(8000rpm,10min)andwashedwithethanolfivesuperhydrophobicSA-basedaerogel(SA/GO/SiO2-M)willtimes.Thefinalprecipitatesweredriedundervacuumat60°C.Thebefabricatedviaasimplecombinationofself-assembly,ionicSEMimageofSiO2isshowninFigureS2.cross-linking,freeze-drying,andtheCVDmethod.AseriesofPreparationoftheSA-BasedAerogelandHydrophobiccharacterizationsandtests,includingtheaerogelstructure,Modification.TheprocedureforpreparingSA-basedcomposite883https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

2Langmuirpubs.acs.org/LangmuirArticleFigure2.SEMimagesof(a)SAaerogelandSA/GO/SiO2-MaerogelwhenthemassratioofGOandSAis(b)4:100,(c)8:100,and(d)10:100.(e,f)RoughsurfaceoftheSA/GO/SiO2-M(8:100)aerogelwithdifferentmagnifications.(g,h)SEM-EDSelementalmappingoftheSA/GO/SiO2-M(8:100)aerogelforC,O,Si,andCaelements.(i)PhotographoftheSA/GO/SiO2-Maerogel.aerogelsisshowninFigure1.First,0.20gofSiO2nanoparticlesandMicromeritics,USA).Theviscosityoftheoilphasewasmeasuredby0.15gofCaCO3powderwereultrasonic-dispersedintheas-preparedanHAAKEMARSIII(ThermoHaakeCo.,Ltd.,Germany)usingaparallelplate(P60TiL,0.4mmgapsetting)undera1000s−1shearSAsolution(30.00mL,0.75g)toobtainahomogeneoussuspension.Then,aGOsuspension(10.00mL)withdifferentmassfractionswasrateat25°C.addedintotheabovesolutionwhilestirring.ThemixturewasfurtherAbsorptionTest.TotesttheoilabsorptioncapabilityoftheSA/dispersedbyanultrasonicmethodfor20min.Finally,DGLsolutionGO/SiO2-Maerogel,thesamplewasimmersedinvariousorganic(10.00mL,0.30g)wasaddedunderstrongstirring.Thefinalmixturesolvents/oilsfor1mintoensureitssaturatedabsorption.Thesamplewasquicklypouredintoamoldandkeptstandingfor30mintoshapewasweighedupbeforeandafterabsorption.Theabsorptionability(gg−1)wascalculatedbythefollowingequationthegel.Afterthegelgotfrozenat−80°Candfreeze-driedat−60°Cundervacuumfor24h,theSA-basedaerogelwasobtained.ThissamplewaslabeledasSA/GO/SiO2.Inthiswork,theSA-based()mm−0Q=aerogelswithdifferentmassratiosofGOtoSA(4:100,6:100,8:100,m0(1)and10:100)wereprepared.Forcomparison,wealsopreparedtheSA/GOaerogelandthepureSAaerogelaccordingtothesamewherem0andmrepresentthemassofthesamplebeforeandaftermethod.saturatedabsorption,respectively.TheSA-basedaerogelwasplacedinabighermeticcontainer.TwoAlloilabsorptionexperimentswereconductedatroomtemper-smallopenvialsofwaterandMTMSwereaddedintothecontainer.ature,andeachtestwasaccomplishedthreetimesrepeatedlytoobtainThehermeticcontainerwasheatedinanovenat60°Cfor12htoanaveragevalue.Thesaturatedaerogelwasweighedquickly,withanachievethesalinizationreaction.SamplesmodifiedbyMTMSwereaimtoavoidtheevaporationoftheabsorbedoilororganicsolvent.labeledwithMtodistinguishunmodifiedsamples.Forexample,theTheabsorption-squeezeapproachandtheabsorption-evaporationSA/GO/SiO2-MaerogelimpliestheSA/GO/SiO2aerogelthathasapproachwereemployedtotestthereusabilityofaerogels,andbeenmodifiedbyMTMS.carbontetrachloridewasselectedasthemodeloil.BasedupontheCharacterizations.ThesurfacemorphologyoftheSA-basedabsorption-squeezeapproach,theabsorbedsolventwasremovedfromaerogelwassprayedwithaurumandobservedunderafieldemissiontheaerogelbyasimplemechanicalsqueeze.Thesqueezedaerogelwasscanningelectronmicroscope(SEM,S-4800,Hitachi,Japan).Theabletoabsorbthesolventagainwithoutanypost-treatment.Inthesurfaceelementsoftheoptimumsamplewereidentifiedbyafieldabsorption-evaporationapproach,theaerogelwasplacedinanovenatemissionscanningelectronmicroscope(SEM,QUANTAFEG250,60°Cfor3.0htoremovetheabsorbedsolvent,andthen,itcouldFEI,USA)equippedwithenergydispersiveX-rayspectroscopyworkagain.(EDS).FunctionalgroupsofsampleswereanalyzedbyanFTIRWater-in-OilEmulsionSeparation.Topreparethewater-in-oilspectrophotometer(ATR-FTIR,MAGNA-560,Nicolet,USA)intheemulsion(W/O),0.10gofspan-80wasfirstdissolvedinto99.00mLrangeof400−4000cm−1.Thesurfacechemicalpropertyoftheofoil,and1.00mLofwaterwasthenaddedintotheoilphase.samplewasidentifiedbyanX-rayphotoelectronspectrometer(XPS,Subsequently,themixturewasemulsifiedbyahigh-speedEscalab250Xi,ThermoFisherScientific,USA).Thethermalstabilityhomogenizer(16,800rpmfor5min,Ultra-TurraxT10,IKA,wasmeasuredonathermogravimetricanalyzerinstrumentGermany).Accordingtothetypesofoilsused(cyclohexane,carbon(TGA&DTG,SDTQ600,TAInstruments,USA)underanitrogentetrachloride,kerosene,anddieseloil),emulsionswerenamedasW-flow(100mLmin−1).Hydrophobicityoftheaerogelswasmeasuredin-H,W-in-C,W-in-K,andW-in-D,respectively.Thedropletsizesofbyacontactangle-measuringdevice(OCA20,DataPhysicsES,theemulsionswereobservedandmeasuredbyopticalmicroscopy.Germany)atroomtemperature.ThewatercontentoftheemulsionTotesttheseparationperformanceoftheaerogel,theemulsionsfiltrateswastestedbyaKarlFischermoisturemeter(C10S,werepouredontotheaerogel,whichwasfixedintoasyringe,andMETTLERTOLEDO,Switzerland).Theporediameterofthethen,theW/Oemulsionswereseparateddrivenbygravity.Theaerogelwasanalyzedbyamercuryporosimeter(AutoPoreIV9500,separationefficiency,S,wasdeterminedby884https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

3Langmuirpubs.acs.org/LangmuirArticleFigure3.(a)FTIRspectraoftheSA,SA/GO,SA/GO/SiO2,andSA/GO/SiO2-Maerogel.(b)XPSspectra,(c)high-resolutionC1sspectrum,and(d)high-resolutionSi2pspectrumoftheSA/GO/SiO2-Maerogel.(e)TGAweightlossandDTGcurvesoftheSA/GO/SiO2-Maerogel.()CC0−structurewithinterconnectiveporesinsideandoutside,S=C0(2)indicatingthatGOissuccessfullyintroducedtoparticipateintheformationofporesandnetworkstructures.ThewhereC0andCrepresentthewatercontentinemulsionsbeforeandintroductionofSiO2andMTMSexertsnoobviousimpactafterseparation,respectively.ontheformationofporestructuresandporesizecomparedwithSA/GOaerogelsasshowninFigureS3.Thisfurther■RESULTSANDDISCUSSIONillustratesthattheself-assemblybetweenGOandSAplaysaCharacterizationoftheSA/GO/SiO2-MAerogel.Asleadingroleintheformationofporousstructure.Withtheobservedfromlower-magnificationSEMimagesshowninincreaseintheGOamount,thenumberofpolygonalholesFigure2a−d,aerogelswithdifferentmassratiosofGOandSAincreasessignificantly,andtheholesbecomeevensmaller.showdifferentstructures,demonstratingthatGOhasbeenSpecifically,whenthemassratiois4:100(Figure2b),a3DembeddedintheSAmatrixandisabletocontrolthestructureporousnetworkstructurebeginstoformintheaerogel.Whenasexpected.AsillustratedinFigure2a,thepureSAaerogelthemassratioincreasesto8:100(Figure2c),theaerogelprimarilyshowsanirregularlamellarstructurewith30−70μmexhibitsaperfectcellularporousstructurewithporesofinterlamellarspacing,andtherearefewlargeporestructures,connectedtoeachother.Theporeswithanaveragesizeof1,4,12,14whichmainlyresultfromthelinkedSAchainsasawhole50−100μmaresuitableforthestorageofliquids.duringthefreezingprocess.WhenGOnanosheetsarepresent,However,whenthemassratiorisesto10:100(Figure2d),theSA/GO/SiO2-Maerogelsshoweda3Dporousnetworkporestructurecollapsesandbreaksupslightly.FigureS4885https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

4Langmuirpubs.acs.org/LangmuirArticleshowstheporesizedistributionoftheSA/GO/SiO2-MFurthermore,weobservedtheintensifiedpeaksat880,1250,(8:100)aerogel.Theresultsshowthattheporediameterand1000−1130cm−1afterMTMSmodification,andthepeaksrangesfrom10to100μmandisconcentratedat60μm,theareconcernedwithSi−C,Si−O,C−H,andSi−O−Si,averageporediameteris45.7μm,andtheporosityis97%,resultingfromthecharacteristicvibrationsofpolysiloxane38whichindicatethattheSA/GO/SiO2-M(8,100)aerogelhasaafterMTMShydrolysis.TheseFTIRspectralresultsrevealhierarchicalporousstructureandhaspotentialfortheoilthesuccessfulconstructionoftheSA/GO/SiO2-Maerogel.absorptionandemulsionseparation.ThesurveyspectraofXPSwereusedtodeterminetheThesurfaceoftheSA/GOaerogelissmooth,andthereissurfacechemicalbondingstateofO,C,andSielementsinthesomeslightcorrugation,whichisdisadvantageoustosuper-SA/GO/SiO2-Maerogel(Figure3b−d).TheC1speakhydrophobicitymodification(FigureS3a).However,theelectronspectralfittingwasfractionatedasshowninFigure3c.surfaceofSA/GO/SiO2-MaerogelsbecomesroughnoticeablyThreepeaksat284.9eV(C−CandCH3bonds),286.4eVbecauseoftheadditionofSiO2nanoparticles(FigureS3band(C−Sibonds),and287.9eV(C−Obonds)were31,35Figure2e,f).Itcouldbeclearlyobservedthatmicro-nanoobserved.Alltheseresultsconfirmthesuccessful39bulgesareevenlydistributedonthesurfaceoftheaerogel,andintroductionofsilanechains.theyconstitutedthestructuralfoundationofsuperhydropho-ThethermalstabilityoftheSA/GO/SiO2-MaerogelwasbicityduetotheSiO2nanoparticles.ThechemicalinvestigatedthroughTGAandDTGanalysisasshownincompositionofSA/GO/SiO2-MaerogelsonthesurfaceandFigure3e.Thecurvesdemonstrateathree-stageprocess:fromthedistributionofpaintcoatwereidentifiedwiththehelpof30to150°C,18.4%oftheoriginalweightislost,whichwas35EDSspectroscopy(Figure2g,h).ThepeaksofC,O,Si,andCacausedbythelossofadsorbed/hydratedwater;from200toelementswereobservedfromthecorrespondingSEM-EDS300°C,thereappearsa23.8%lossoftheoriginalweight,mappingimages.TheelementsCandOweremainlyfromthewhichwasattributedtothehydrogenbondfractureaswellasSA-basedaerogelsubstrate.TheelementSiwasobtainedfromthedehydroxylationandthepreliminarydecompositionof40SiO2nanoparticlesandMTMScoating.Also,thehomoge-SA;thelossofweightdeclinesslowlybetween350and550neousdistributionoftheCaelementsuggeststhattheaerogel°C,anda15.8%lossoftheoriginalweightwasattributedto35iscross-linkeduniformly,whichisimportantforthethefurtherdegradationofSAandthecarbonationofGO.mechanicalstrengthofthepreparedaerogel.OilAbsorptionCapability.ThespecialwettabilityofWiththeincreaseintheGOamount,thedensityofthematerialsisessentialforselectiveseparationofoil/wateraerogelgrowsgraduallyduetotheincreaseinrawmaterialsmixtures.Figure4a,bshowsthespecialwettabilityoftheSA/(FigureS5a),whiletheaerogelwiththegreatestGOmasscanstandonthetopofadandelion(Figure2i).ThoughtheadditionofGOenlargesthespecificsurfacearea,theoilabsorptioncapacitiesofSA/GO/SiO2-Maerogelsforcyclo-hexaneandcarbontetrachlorideareweaklyinfluencedbytheGOamount(FigureS5b)becausetheoilabsorptionisacomprehensiveresultofmanyfactorsincludingspecificsurfacearea,oilstoragespace,andaerogels’mass.WhenthemassratioofGOtoSAremains8:100,aerogelsdisplaythemostexcellentabsorptioncapacity,whichisconsistentwiththeresultofSEM.Consideringthesuitableporestructureandabsorptioncapacity,themassratioof8:100isconsideredasthebestratioofGOtoSA,andtheSA/GO/SiO2-Maerogelwiththisratioischosenasthebestsampleforsubsequentcharacter-izationandperformancetests.Figure3ashowstheFTIRspectraofSA(a1),SA/GO(a2),SA/GO/SiO2(a3),andSA/GO/SiO2-M(a4)aerogels.FortheFigure4.(a)AmphiphiliccharacteristicsoftheSA/GO/SiO2aerogel.SAspectrum(a),thepeakat3650cm−1isduetothe(b)SuperoleophilicityoftheSA/GO/SiO-Maerogel.(c)Water12stretchingvibrationofO−H.Thepeaksat1600and1420contactangleoftheSA/GO/SiO2-Maerogel.(d)Photographsofthecm−1areassociatedwiththeasymmetricandsymmetricSA/GO/SiO2aerogelandtheSA/GO/SiO2-Maerogelinwater.Photographsshowing(e)removalofcyclohexanefromthewaterstretchingvibrationof−COOHgroups,respectively.Thepeak−1surfaceand(f)carbontetrachlorideabsorptionunderwaterbythenear1050cmiscausedbyC−Obending.Thepeakat820−135SA/GO/SiO2-Maerogel.cmisattributedtotheCa−alginatelinkage.AftertheadditionofGO(a),thepeakaround3650cm−1weakens2becauseofthehydrogenbondinteractionsbetweenGOandGO/SiO2aerogelandtheSA/GO/SiO2-Maerogel,respec-SA.Simultaneously,thepeaksat1600,1420,and1050cm−1tively.Bothwaterandoilturnouttobecompletelywettedandbecomestrongerobviously,whichmightbecausedbytheC−permeateintotheSA/GO/SiO2aerogel,onlyleavingablueCstretchingmodeofthesp2network,theC−O−Cstretchingwatermarkandaredoilmark(Figure4a).Thisrevealsthat35,36mode,andtheC−Obendingmode.FortheSA/GO/SiO2theSA/GO/SiO2aerogelpossesseshydrophilicityandlip-spectrum(a),thenewpeakat461cm−1isattributedtoSi−3ophilicity.Nevertheless,fortheSA/GO/SiO2-Maerogel,itO−Si,indicatingthatSiO2issuccessfullyloadedintheshowssuperhydrophobicityandsuperoleophilicitythatmight37aerogels.ThemaindifferenceinFTIRspectrabetweenthebeattributedtothehighsurfaceroughnessandlowsurfaceSA/GO/SiO2andSA/GO/SiO2-Maerogelisat400−1600energy;thus,itcanonlybethoroughlywettedandpermeatedcm−1.Anewpeakat780cm−1causedbytheSi−CHbondisbyoil(Figure4b).OnthesurfaceoftheSA/GO/SiO-M32observedintheFTIRspectraoftheMTMS-modifiedaerogel.aerogel,thewatercontactangleis154°(Figure4c),886https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

5Langmuirpubs.acs.org/LangmuirArticleFigure5.(a)AbsorptioncapacityoftheSA/GO/SiO2-Maerogelforvariousoilsororganicsolventsand(b)absorptioncapacitiesmarkedwithdensityofsolvents.manifestingprominentwaterrepellency.WhentheSA/GO/theorganicsolvents/oilscorrespondingtotheminimum27,44SiO2aerogelandtheSA/GO/SiO2-Maerogelwereplacedinabsorptioncapacityareoflowerdensity,suchashexane45,46watersimultaneously(Figure4d),theSA/GO/SiO2aerogelandgasoline.Onthecontrary,theorganicsolvents/oilsabsorbswaterandthenbeginstosink,whiletheSA/GO/SiO2-correspondingtothemaximumoneareofhigherdensity,4746Maerogelcontinuestofloatbecauseofitshydrophobicityincludingdichloromethaneandcarbontetrachloride.So,evenonehourlater.TheseresultsindicatethatMTMSboththedensityoforganicsolvents/oilsandthequalityofthemodificationmakestheSA-basedaerogelshowexcellentaerogelitselfgreatlyinfluencethevaluesoftheabsorptionselectivewettability,whichisofgreatimportanceforoil/capacity.AsshowninTable1,theabsorptioncapacityofthewaterseparation.SA/GO/SiO2-MaerogeliscomparabletoorweakerthanthatCyclohexaneandcarbontetrachloridewereselectedasofsomenon-SAbio-basedaerogelsandcarbonaerogels.representativesoffloatingoilandsinkingoil,respectively,forHowever,comparedwithSA-basedaerogels,SA/GO/SiO2-MthepurposeofevaluatingthepotentialoftheSA/GO/SiO2-Mshowsaremarkablyhigherabsorptioncapacity.Importantly,aerogelasanoilabsorbent.AsshowninFigure4eandVideobesidesthehighlyefficientoilabsorptionability,theSA/GO/S1,whentheSA/GO/SiO2-MaerogelwasplacedintotheSiO2-Maerogelsimultaneouslypossessesanexcellentemulsionmixtureofcyclohexaneandwater,cyclohexanefloatingontheseparationabilitythatwewilldiscusslater.Nevertheless,thesurfaceofwaterwascompletelyandquicklyabsorbedwithinSA-basedaerogelsreportedintheliteratureseemtohaveonlynomorethan10s.Moreover,asshowninFigure4fandVideoasinglecompetency.Whatismore,thosereportedSA-basedS1,theSA/GO/SiO2-Mcanselectivelyabsorbcarbonaerogelscouldnotseparatestableoil−wateremulsionswithtetrachlorideratherthanwaterwithinlessthan10s.Itissmallerdropletsize.Somecarbonaerogelsshowexcellentnoteworthythatwhentheaerogelwasimmersedintowater,performanceonbothoilabsorptionandemulsionseparation,themirror-likeonthesurfacedirectlyreflectsthehydro-asindicatedinthetable.TheabsorptioncapacityoftheSA/41phobicity,andthebubblesformedintheabsorptionprocessGO/SiO2-Maerogelseemsweakerthanthatofthecarbondirectlydisplaythegreatoilstoragespaceinsidetheaerogel.aerogelpreparedfromwastepaper/bananapeel(35−115gTherefore,theSA/GO/SiOaerogelisconsideredasanidealg−1,aerogeldensityof15mgcm−3)48orPlatanusorientalis2absorbentforoilspilltreatmentandoilywastewaterfibers(30−150gg−1,aerogeldensityof8.3mgcm−3).49remediation.Specifically,thedensityoftheSA/GO/SiO2-Maerogel(36.6Inthisexperiment,elevenkindsoforganicsolventsoroilsmgcm−3)is2−4timeshigherthanthatofthecarbonaerogel,includingcrudeoilwereusedtoevaluatetheabsorptionwhilethemassabsorptioncapacityofthecarbonaerogelis2−capacityoftheSA/GO/SiO2-Maerogel.Figure5ashowsthe3timeshigherthanthatoftheSA/GO/SiO2-Maerogel.ItcanabsorbencyoftheSA/GO/SiO2-MaerogelforvariousoilsbeestimatedthatthelowerabsorptioncapacityvalueofSA/rangingfrom17.92to43.92gg−1.WiththeincreaseintheoilGO/SiO2-Maerogelsismainlyattributedtothehigherdensitydensity,theabsorptioncapacitypresentsarelativelygooditself.linearrelationship(Figure5b).TheabsorptioncapacityisevenOilDesorptionCapacityandRecyclability.TheSA/asstrongassomesponges,likeasuperhydrophobicattapulgite-GO/SiO2-Maerogelshowsexcellentcompressibility,whichiscoatedPUspongefabricatedbyLietal.(17−45gg−1for7essentialfortherecoveryofabsorbedoilandreusabilityof42kindsofoils)andaseriesofsilane-functionalizedpolyvinylmaterials.AsshowninFigure6a,bandVideosS2andS3,thealcoholformaldehydespongessynthesizedbyWangetal.(4−SA/GO/SiO2-Maerogelexhibitsexcellentrecoverability.Ina14gg−1for7kindsofoils).43Table1comparestheabsorptiondrycondition,therecoveryoftheaerogel’sshapeiseasyandcapacitiesoftheSA/GO/SiO2-Maerogelwithothertypesofrapidafterbeingcompressedbyaweightof100g.FigureS6abio-basedaerogelmaterialsreportedrecently.Becauseawidershowsthatthevolumechangeunder100gweightvarietyoforganicsolvents/oilswerecoveredintheseliteraturecompressionisabout65%.FigureS6bshowsthestress−strainstudies,inTable1,weonlylisttheorganicsolvents/oils,forcurveundera70%volume.Theaerogelpresentedabout26whichtheabsorbentshowstheminimumandmaximumkPaofcompressivestressata70%strain,andthisvaluewasabsorptioncapacity.Therangebetweenthesetwovaluesishigherthanthatofgreenaerogelsinpreviousliterature53,54usedtoevaluatetheremovalcapacitiesofvariousreportedstudies.ThehighcompressivestresswouldbebeneficialaerogelmaterialsandSA/GO/SiO2-M.Itcanbefoundthatfortheintegritymaintenanceinpracticalapplications.Inthe887https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

6Langmuirpubs.acs.org/LangmuirArticlework47274446393845484923235051245299.53this99.799.65−−−ciency(%)ref.separationffie=1:1)=1:1)98.798.6=1:99)=1:20)99.699.99oiloil=1:99)98.99oiloiln02/10/40andfi:V:Voil:V:V:VwaterwaterVVwaterwaterwaterVVVchloroformkeroseneoilsoybeanoil,andbenzeneandkeroseneoil(4):toluene,hexadecane,diesel,andsurfactant:Tween80(1mg/mL)oil(4):PolyAlphaOlesurfactant:noneoil/watermixture(oil(4):hexane,soybeanoil,kerosene,andpumpoil/watermixture(oil(5):gasoline,petroleumether,hexane,oil(4):hexane,dieseloil,carbontetrachloride,surfactant:Tween80(1mg/mL))mixture1−486863124234−−197−−−115W/Oemulsion(150W/Oemulsion(−25.9939−28.20−20−−13.25−13.98−−43.92−W/Oemulsion(803011.2absorption13.7710.2010.9817.92capacity(ggThecarbonaerogelsherearenotonlypyrolyzedintheprocessofproductionbutalsomadebn40,fiabsorptionseparationadichloromethane,etc.(10)etc.(11)etc.(11)tetrachloride,etc.(10)(10)etc.(6)oil,etc.(4)oil,etc.(4)etc.(10)etc.(11)hexane,tetrachloromethane,)oil3−57methylsiliconeoil,peanut86methylsiliconeoil,peanut−−density72.810cyclohexane,5.9hexane,dichloromethane,55hexane,dichloromethane,27.1112gasoline,carbon16.2hexane,chloroform,etc.(9)hexane,phenoxin,etc.(15)15gasoline,chloroform,etc.DMF,pumpoil,etc.(11)318.35diesel,PolyAlphaOle35354136.6hexane,carbontetrachloride,(mgcm°erentAbsorbentMaterialsff°°°°°°°°°°°°°°superoleophobicity,<145.7superoleophobicity,>155157150.3149.3151underwaterunderwaterber<125fi-M15422berscellulose/silicagraphenebananapeelfichitosanESO/cellulosegraphene/132.6cellulose/chitosan/cellulose152.8chitosancellulosenanobamboofungus152.3wastepaper/154.2PlatanusorientalisSA/CMCSA/celluloseSA-Ca-Zr120148.7SA/TiO140.5SA/N-succinylSA/GO/SiOhexane,chloroform,etc.(7)17bspeciesmaterialswettabilityaerogelTable1.ComparisonofthePropertiesofDinon-SAbio-basedcarbonaerogelSA-basedaerogelSA/MBA129aIntheoilcolumnoftheform,thenumbersinparenthesesrepresentthenumberoftypesofoilsabsorbed.bybiomassmaterials.888https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

7Langmuirpubs.acs.org/LangmuirArticleFigure6.(a)ShaperecoveryoftheSA/GO/SiO2-Maerogelafterbeingcompressedbyaweightof100g.(b)Photographsshowingtheprocessofrecyclingtheaerogelbysqueezingincarbontetrachloride.OilrecoveryabilityofSA/GO/SiO2-Mover10cyclesofabsorptionanddesorptionby(c)evaporationand(d)mechanicalsqueezing.oilphase,thecompressedaerogelcouldabsorboilandrecoverseriesofwater-in-oilemulsionsstabilizedbysurfactants,suchitssaturationstate.ToinvestigatethereusabilityoftheSA/aswater-in-cyclohexane(W-in-H),water-in-carbontetrachlor-GO/SiO2-Maerogel,twocommonmethods,namely,evapo-ide(W-in-C),water-in-kerosene(W-in-K),andwater-in-dieselrationandmechanicalsqueezing,wereemployedtoremoveoil(W-in-D).Fromtheopticalmicroscopicimagesoftheabsorbedoil.Carbontetrachloridewasselectedasamodelemulsions,theaveragediametersofwaterdropletsforW-in-oilphase.SampleswereweighedupbeforeandafterH,W-in-C,W-in-K,andW-in-Demulsionswere4.36,2.01,evaporationormechanicalsqueezingtocalculatetheamount3.87,and3.42μm,respectively(FigureS8).Afterfiltrationbyofoilabsorbedbytheaerogelintherecyclabilityexperiments.theaerogel,themilkywater-in-oilemulsionsbecametrans-AsshowninFigure6c,theabsorbedoilisthoroughlyremovedparent,andwaterdropletswerenotobservedintheopticalaftereachevaporationat60°Cfor3h.About89.8%ofitsimagesasshowninFigure7a−d.Theemulsionseparationinitialabsorbencyremainsafter10cycles.ThismethodcanbeprocessisshowninVideoS4.ThedifferenceinseparationappliedtodesorboilthathasalowboilingpointandisratesisexplainedbrieflyinTableS1intheSupportingevaporable.Figure6dshowsthataround24%oftheoilhasInformation.Figure7e,fdemonstratestheseparationefficiencybeenleftintheaerogelaftereachmechanicalsqueezingcycle.oftheSA/GO/SiO2-Maerogelforfourtypesofoil-in-waterEighty-ninepercentoftheoriginalabsorptioncapabilityemulsionsandtheircorrespondingwatercontentsintheremainsafter10cycles.Thedeclinedabsorptioncapacityfiltrates.TheseparationefficiencyiscomparablewiththemayresultfromtheslightcollapseofthestructureinthereportedcarbonaerogelsshowninTable1,butthepreparationrecoveryprocess,whichishardlyavoidable.FigureS7showsconditionsofSA/GO/SiO2-MaerogelsaremilderandthetheSEMimageoftheaerogelafter10cyclesofmechanicalcross-linkingmodeismuchgreenerthanthatusedinpreparing48squeezingandabsorption.Itcanbeseenthatthestructurehascarbonaerogels.Althoughanunderwatersuperoleophobicnoobviouschange,whichshowsthegoodmechanicalstrengthSA/TiO2aerogelandSA/N-succinylchitosanaerogelwereoftheaerogel.Althoughthemechanicalsqueezingmethodfailsusedtoseparatesimpleoil/watermixturesasTable1shows,ittoremoveabsorbedoilcompletely,itcanrecycleoilrapidlyisworthmentioningthatSA-basedaerogelsarerarelyinvolvedwithlowercostandissuitablefornearlyalltypesofoils.So,inemulsionseparation.WealsomadeasimplecomparisontheexcellentperformanceoftheSA/GO/SiO2-Maerogelinwithothermaterialsontheemulsionseparationefficiency,andmechanicalsqueezingdemonstratesthattheaerogelpossessestheseparationefficiencyoftheSA/GO/SiO2-Maerogelgreatpotentialforthepracticalapplicationtotheseparation(Voil:Vwater=99:1,98.99−99.53%)isnolessthanthatofandrecoveryofoilsandorganicsolventsfromwater.othermaterials,suchasasuperhydrophobicSiO2/poly-EmulsionSeparationPerformance.Inadditiontothe(vinylidenefluoride)compositemembrane(Voil:Vwater=55goodabsorptioncapacityandexcellentcompressibility,99:1,98.7−99.78%),ametalmeshcoatedbycopper56anotheradvantageoftheSA/GO/SiO2-Maerogelisitsgreathydroxide(Voil:Vwater=50:1,>99.0%),andawoodslice57potentialinemulsionseparation.Efficientemulsionseparationcoveredbycopperhydroxide(Voil:Vwater=50:1,>98%).inaneco-friendly,efficient,andlow-costmannerisstillagreatConsideringtheadditionaladvantagesoftheaerogel,likeitschallenge,especiallyinthepresenceofsurfactants.TotestthesimplerpreparationmethodanditcanbecustomizedintheseparationperformanceoftheSA/GO/SiO2-Maerogelforformofinjectionmolding,theSA/GO/SiO2-Maerogelshowsemulsion,itwasfixedintoasyringeandthenusedtoseparateagreatpotentialinpracticalapplication.889https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

8Langmuirpubs.acs.org/LangmuirArticleFigure7.Digitalimageandopticalimageofthesurfactantstabilityemulsionseparationperformance:(a)water-in-cyclohexane,(b)water-in-carbontetrachloride,(c)water-in-kerosene,and(d)water-in-dieseloil.(e)Separationefficiencyand(f)watercontentinfiltratesofvarioussurfactant-stabilizedW/Oemulsions.Inordertofurtherinvestigatetheseparationabilityoftheaerogelforemulsions,0.1goftheSA/GO/SiO2-Maerogelwasutilizedforacontinuousseparationofthewater-in-carbontetrachlorideemulsion.Duringtheseparation,every10mLofthefiltratewascollectedandputinavialmarkedwithaserialnumber.AsFigureS9reveals,thefirst40mLofthefiltrateinbottles1,2,3,and4istransparent,indicatinganapproximate400mLemulsionseparationabilitypergramoftheaerogel.Thefiltratesinbottles5,6,and7becometurbidgradually,butthediameterofwaterdropletsinbottle6or7ishigherthanthatbeforefiltration(FigureS9b−e).ItisworthytonotethatFigure8.Water-in-oilemulsionseparationmechanismthroughtheSA/GO/SiO2-Maerogel.aftertheaerogelwascleanedwithdichloromethane,itstillshowedefficientseparationforemulsionsasshowninFigureS10,whichdemonstratesthegoodcyclestabilityoftheSA/theaerogelisajaggedporousstructure,sosmallwaterdropletsGO/SiO2-Maerogel.Also,thewatercontentresultafterfivecouldbeadheredtootherdropletsinthelongandcyclesshowsthattheaerogelcanretain98.3%separationinterconnectedmicrochannelsofaerogels,thusforminglargerefficiency.onestoachievedemulsificationandseparation.TheprocessTogainamorecomprehensiveunderstandingonthecanexplainwhytheSA/GO/SiO2-Maerogelcanalsoseparationmechanismofwater-in-oilemulsionsbytheSA/effectivelyseparatevarioussurfactant-stabilizedwater-in-oilGO/SiO2-Maerogel,anillustrationoftheseparationprocessisemulsionsdrivenbygravitywhenthesizesofemulsifiedindicatedinFigure8.WhentheW/Oemulsionsarepoureddroplets(2−5μm)arefarsmallerthantheporesizeoftheontotheaerogel,thecoalescenceofemulsifiedwaterdropletsaerogel(60μm).Astheamountoftheemulsionincreases,theandthesize-sievingfiltrationintheaerogeloccur.Specifically,surfaceoftheaerogelcouldbepollutedbysurfactants,thusthemicrowaterdropletsarerepelled,buttheoilphaseleadingtoadecreasedseparationability.Aftertheaerogeliscontinuouslypassesthroughtheaerogelbecauseofthecleaned,theaerogelregainsitsexcellentabilitytoseparatesuperhydrophobic/superoleophilicproperties.Theinteriorofemulsions.890https://dx.doi.org/10.1021/acs.langmuir.0c03229Langmuir2021,37,882−893

9Langmuirpubs.acs.org/LangmuirArticle■CONCLUSIONSChina,Qingdao266100,P.R.China;orcid.org/0000-0002-1595-4769Insummary,thisstudydemonstratesafacilemethodtoprepareasuperhydrophobicSA-basedaerogelviaacombina-Completecontactinformationisavailableat:tionofcalciumioncross-linkingself-assembly,freeze-drying,https://pubs.acs.org/10.1021/acs.langmuir.0c03229andCVDhydrophobicmodification.TheobtainedSA/GO/SiO2-MaerogelshowsaporousandsuperhydrophobicNotesstructureasexpected,whichendowstheaerogelwithanTheauthorsdeclarenocompetingfinancialinterest.excellentoilabsorptioncapacity.Theaerogelcanseparatevarioussurfactant-stabilizedwater-in-oilemulsionswithhigh■efficiency(98.99−99.53%)undertheactionofgravity.TheACKNOWLEDGMENTSSA/GO/SiO2-MaerogelexhibitsexcellentcompressibilityandThisresearchissupportedbytheNationalNaturalSciencegoodrecyclability,whichmatchperfectlywiththerequire-FoundationofChina(21773219),theQingdaoNationalmentsfortherecycleofoilpollutants.Moreover,theSA-basedLaboratoryforMarineScienceandTechnologyaerogelisenvironmentallyfriendlyandlow-cost,andthe(QNLM2016ORP0308),andtheShandongKeyLaboratorypreparationprocessismildandsimple,thusgreatlyloweringofWaterPollutionControlandResourceReuse(2019KF03).thepotentialpollutionriskandapplicationcost.Therefore,theThisisMCTLcontributionno.240.SA/GO/SiO2-Maerogelobtainedinthisworkshowsgreatprospectsinpracticaloilpollutiontreatments,includingoil■REFERENCESspillcleanup,fuelpurification,andemulsionseparation.(1)Ge,J.;Zhao,H.-Y.;Zhu,H.-W.;Huang,J.;Shi,L.-A.;Yu,S.-H.AdvancedSorbentsforOil-SpillCleanup:RecentAdvancesand■ASSOCIATEDCONTENTFuturePerspectives.Adv.Mater.2016,28,10459−10490.*sıSupportingInformation(2)Chen,C.;Weng,D.;Mahmood,A.;Chen,S.;Wang,J.TheSupportingInformationisavailablefreeofchargeatSeparationMechanismandConstructionofSurfaceswithSpecialhttps://pubs.acs.org/doi/10.1021/acs.langmuir.0c03229.WettabilityforOil/WaterSeparation.ACSAppl.Mater.Interfaces2019,11,11006−11027.PhotographofaGOsuspensionandanXRDpatternof(3)Wang,Y.;Yang,H.;Chen,Z.;Chen,N.;Pang,X.;Zhang,L.;GO;SEMimageofSiO2nanoparticles;SEMimagesofMinari,T.;Liu,X.;Liu,H.;Chen,J.RecyclableOil-AbsorptionFoamstheSA/GOaerogelandtheSA/GO/SiO2-MaerogelviaSecondaryPhaseSeparation.ACSSustainableChem.Eng.2018,6,withdifferentmagnifications;porediameterfortheSA/13834−13843.GO/SiO2-MaerogelwhenthemassratioofGOandSA(4)Li,Z.;Zhong,L.;Zhang,T.;Qiu,F.;Yue,X.;Yang,D.is8:100;density,contactangle,andabsorptioncapacitySustainable,Flexible,andSuperhydrophobicFunctionalizedCellulosedata;volumechangesandthestress−straincurvedata;AerogelforSelectiveandVersatileOil/WaterSeparation.ACSSustainableChem.Eng.2019,7,9984−9994.SEMimageoftheSA/GO/SiO2-Maerogelafter10(5)Qiu,S.;Li,Y.;Li,G.;Zhang,Z.;Li,Y.;Wu,T.Robustcyclesofmechanicalsqueezingandabsorption;diameterSuperhydrophobicSepiolite-CoatedPolyurethaneSpongeforHighlydistributionofwaterdropletsintheemulsions;filtratesEfficientandRecyclableOilAbsorption.ACSSustainableChem.Eng.afteracontinuousseparationdata;reusabilityofthe2019,7,5560−5567.aerogelforemulsionseparation;densityandviscosityof(6)Zhan,H.;Zuo,T.;Tao,R.;Chang,C.RobustTunicateCellulosetheoilphase;references(PDF)Nanocrystal/PalygorskiteNanorodMembranesforMultifunctionalFloatingoilandsinkingoilabsorption(MP4)Oil/WaterEmulsionSeparation.ACSSustainableChem.Eng.2018,6,Shaperecoveryoftheaerogelafterbeingcompressedby10833−10840.(7)Ye,H.;Chen,D.;Li,N.;Xu,Q.;Li,H.;He,J.;Lu,J.Durableaweightof100g(MP4)andRobustSelf-HealingSuperhydrophobicCo-PDMS@ZIF-8-Processofrecyclingtheaerogelbysqueezing(MP4)CoatedMWCNTFilmsforExtremelyEfficientEmulsionSeparation.Emulsionseparationprocess(MP4)ACSAppl.Mater.Interfaces2019,11,38313−38320.(8)Guan,Y.;Cheng,F.;Pan,Z.SuperwettingPolymericThree■Dimensional(3D)PorousMaterialsforOil/WaterSeparation:AAUTHORINFORMATIONReview.Polymer2019,11,806.CorrespondingAuthor(9)Ieamviteevanich,P.;Palaporn,D.;Chanlek,N.;Poo-arporn,Y.;YimingLi−KeyLaboratoryofMarineChemistryTheoryandMongkolthanaruk,W.;Eichhorn,S.J.;Pinitsoontorn,S.CarbonTechnology,MinistryofEducation,OceanUniversityofNanofiberAerogel/MagneticCore−ShellNanoparticleCompositesasChina,Qingdao266100,P.R.China;orcid.org/0000-RecyclableOilSorbents.ACSAppl.NanoMater.2020,3,3939−3950.0003-0437-1661;Email:liym@ouc.edu.cn(10)Si,Y.;Fu,Q.;Wang,X.;Zhu,J.;Yu,J.;Sun,G.;Ding,B.SuperelasticandSuperhydrophobicNanofiber-AssembledCellularAuthorsAerogelsforEffectiveSeparationofOil/WaterEmulsions.ACSNanoYushuangYang−KeyLaboratoryofMarineChemistry2015,9,3791−3799.TheoryandTechnology,MinistryofEducation,Ocean(11)Yang,W.;Wang,N.-N.;Ping,P.;Yuen,A.C.-Y.;Li,A.;Zhu,S.-UniversityofChina,Qingdao266100,P.R.ChinaE.;Wang,L.-L.;Wu,J.;Chen,T.B.-Y.;Si,J.-Y.;Rao,B.-D.;Lu,H.-D.;XiupingChen−KeyLaboratoryofMarineChemistryTheoryChan,Q.N.;Yeoh,G.-H.Novel3DNetworkArchitecturedHybridandTechnology,MinistryofEducation,OceanUniversityofAerogelComprisingEpoxy,Graphene,andHydroxylatedBoronNitrideNanosheets.ACSAppl.Mater.Interfaces2018,10,40032−China,Qingdao266100,P.R.China40043.ZichaoYin−KeyLaboratoryofMarineChemistryTh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