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Formygrandchildren,AlexandreVargel,RomainVargel,AlexandraBourgoin, andLaureBourgoin
Foreword Ifthereisametalofthefuture,itisaluminium.
Aluminium’ssuccesshasbeenconsistentforover100years.Mostrecently,atthestartofthe21st century,annualconsumptionofaluminiumreached29millionmetrictons;by2017,thatfigurehad risento80millionmetrictons.Andsomearepredictingconsumptioncouldreachabout120million metrictonsin2030.
Thisishardlyasurprise.Aluminium’sintrinsicpropertiesmakeitauniqueandextremelyvirtuous materialthatrespondstonumerouschallengesinoursocietylinkedtoclimatechangeandresponsible managementandprotectionoftheEarth’sresources.Aluminium’sabilitytobeendlesslyrecyclable withoutlosingitsinitialpropertiesisanexcellentexampleofthis.
Furthermore,thankstoitslightweightcapability,aluminiumallowstransportationvehiclesonland, intheairandatseatosignificantlydecreasefuelconsumptionandthusdrasticallyreduceemissionsof greenhousegases.Italsocombinesductilityandahighlevelofresistancetobothimpactsand corrosion.
Beyonditsspecificproperties,theinexorablefascinationwithaluminiumisfirstandforemostthe resultofdecadesofresearchandinnovation.Generationsofresearchershaveworkedonthedevelopmentofincreasinglyadvancedalloysandever-moreinnovativemanufacturingprocesses.
Thisisparticularlythecasewiththetechniqueoffrictionstirwelding,whichmakesitpossibleto assembledifferentmaterialswithouttheneedforrivetsoradditivemanufacturingprocesses,also knownas3Dprinting.
AtConstellium asuccessorofthePechiney,AlcanandAlusuissegroupsandagloballeaderin innovative,highvalue-addedaluminiumsolutions wemakesureengineersandtechniciansinour R&Dcentrehaveaccesstothemostsophisticatedresourcesandmethodsavailable.Thanksto manyclosecollaborativeprojectswithourcustomersandnumerouslaboratoriesanduniversities worldwide,ConstelliumhasdesigneduniqueandrevolutionarysolutionssuchasAirwarefortheaerospacesector,SecuralexandHSA6fortheautomotiveindustryandAeralforaerosolpackaging.
Althoughtheyareusedindifferentapplicationsandcomefromawiderangeoffamiliesofalloys, thesenewproductshighlightourindustry’squestforexcellenceandourabilitytoimaginetheworldof thefuturethroughcontinuousoptimizationofthepropertiesofaluminium.
Oneofthefundamentalareasofresearchiscorrosion,thesubjectofthisbook.Althoughitis naturallyresistant,aluminiumneedstoofferever-higherperformance.ThisneweditionofChristian Vargel’sbook, CorrosionofAluminium,reflectstheknowledgehehasaccumulatedoverhis40yearsat Pechineyasanengineerinourresearchcentre.Asaspeakerandauthorofseveralbooksonthemetal, ChristianVargelisarecognizedexpertinthefieldofaluminiumcorrosion,orashewouldputit,a corrosionpractitioner.
Thankstoitsscientificapproachtothetopic,thisbookisbothanexplorationofthephenomenonof aluminiumcorrosionandapracticalguidetotheuseofaluminiumalloysbasedontheircorrosion properties.Aimedatbothacademicsandprofessionals,itisunrivalledinitsfieldandIwouldlike tooffertheauthormywarmestthanksforentrustingitsforewordtome.
Jean-MarcGermain ChiefExecutiveOfficer,Constellium
Forewordtotheoriginaledition Withanannualconsumptionof25millionmetrictons,aluminiumisthesecondmostcommonlyused metalintheworldaftersteel.Itslightnessisveryoftenthemostimportantadvantageforthecommercialdevelopmentofaluminium,whichexplainswhyitisextensivelyusedforgroundtransport, aerospaceandshipbuilding.Thisisalsothereasonwhytheautomotiveindustryiscurrentlyveryinterestedinaluminium:lightnessisbecomingapriority.
Thesecondadvantageofaluminiumisitscorrosionresistance.Thisexplainsitsimportantposition inconstruction,civilengineering,transport,heatexchangersandsoon.
In1890,navalarchitectshadconsideredaluminiumforreducingweightinvessels.Butinorderfor aluminiumtobeuseableforshipbuilding,metallurgistsandcorrosionspecialistsinthe1930sfirsthad todevelopaluminiummagnesiumalloys.Thesealloyshaveanexcellentcorrosionresistanceinthe marineenvironment,andtheyareweldable.Since1960,allhigh-speedferrieshavebeenbuiltinthese alloys.
Asimilartrendwasobservedwithheatexchangers:aluminiumwasrecognizedasanobvioussolution,especiallyforautomotiveheatexchangerssince1970.Infact,severalalloyshaveverygoodthermal conductivityandexcellentresistancetoenginecoolants,makingitpossibletomanufactureheat exchangersthatarecheaperandofcourselighterthantraditionalheatexchangersincopperalloys.
Projectsfordevelopingrenewableenergysources(solar,etc.)haveoftenbeenbasedontheuseof aluminiumheatexchangersforseveralreasons:amuchlowercostthantitanium,goodthermal conductivityandexcellentcorrosionresistance.
ChristianVargel,throughouthislongcareerwithinPechiney,hasbeenapractitionerofaluminium corrosionandarecognizedexpertinthisfield.Hisfirstbook, LeComportementdel’Aluminiumetde SesAlliages (TheBehaviorofAluminiumandItsAlloys),waspublishedbyDunodin1979.
Sincethen,hisexperiencehasgrownsteadily.Hehasfollowedmarineapplicationsandautomotive heatexchangersandhasparticipatedinmanydamageassessmentsinvolvingcorrosioninservice.He hasalsogivenmanytalksonthecorrosionresistanceofaluminium,andhascontributedtomanyof PechineyRhenalu’stechnicaldocumentsandbrochures,suchas‘AluminiumandtheSea’and ‘AluminiuminIndustrialVehicles’.Wethereforeencouragedhiminhisprojecttowriteasecond book:hisrecognizedexperienceinthefieldofaluminiumcorrosiondeservedtobemorewidelyknown anddisseminated.Thisbookwillcertainlycontributetomeetingthisgoal.
Corrosionisadifficulttopic.Iamdeeplyconvincedthatthepractitioner’sapproach,basedon expertiseandexperience,isbestforassessingthecorrosionresistanceofaluminium,anassessment thatisobviouslyoneofthemainconditionsforthedevelopmentofmanyusesofaluminiumin transportandconstructionpowertransmission.
ChristianVargel’sbookpresentsthereaderwithaglobalapproachtocorrosion,comprisingthe selectionofalloys,designprinciplesandserviceconditions.Iamconvincedthatitwillcontribute tothedevelopmentofaluminiuminthosefieldswhereresistancetocorrosionisanessentialproperty.
BernardLegrand FormerDeputyChiefExecutiveOfficer
Pechiney,September1998 xxxvii
Preface MylongcareerinthePechineyGroupfrom1957to1997andsubsequentlyasanindependentconsultantprincipallyfocusedonaluminiumcorrosionhasenabledmetoacquireextensiveexperienceinthis field.
Myexperienceisbasedonthetreatmentofthemanycasesofin-servicecorrosionthatIhavehadto dealwithoverthepast50years,andontheelectrochemicalandmetallurgicalfundamentalsof aluminiumcorrosion.
Thisdualapproachhasmademeacorrosionpractitioner,inthesensethatIhadtofindanexplanationforcasesofcorrosioninserviceorthatIhadtoplanhowtoavoiditthroughthechoiceofalloys, operatingconditionsandsoon.
Indeed,corrosionremainsacomplexsubjectbecauseitdependsonmanyparameters,whichmakes itnecessarytohaveapracticalapproachtobeusefulandexplainableonthebasisoffundamentaldata.
Thisengineeringactivityhasallowedmetoacquirewideexperienceinaluminiumapplications, particularlywherethequestionofcorrosionresistanceofbuildings,heatexchangers,renewable energysystems(solar,OTEC,etc.),transport,shipbuildingandsoonisconcerned.
Ihavefrequentlysharedmyexperienceofaluminiumcorrosionatnumerousconferencesandin severalbrochurespublishedbyPechiney:“AluminiumandtheSea,”“AluminiumintheAutomotive Industry,”“AluminiuminIndustrialVehicles,”and“AluminiumSemi-finishedProducts.”
Followingarequestofthepublisher,Elsevier,Iresumedthereeditingofthefirstversionof Corrosion ofAluminium publishedin2004,whichwasthetranslationof Corrosiondel’Aluminium publishedin FrenchbyDunodin1999.
Inthisnewedition,Ihavereviewedandincorporatedtheknowledgeacquiredrecentlybymany laboratoriesthathavepublishedonthesubjectofaluminiumcorrosionanditsmetallurgicalaspects. In20years,newinvestigativemethodshavealsomadeitpossibletoexplainmanyofthephenomena involvedinstructuralcorrosion.
Asaresult,thisneweditionof CorrosionofAluminium,whilemaintainingitspracticalorientation tomeettheneedsofaluminiumusers,givesalargeplacetotheresultsofthehigh-qualityscientific publicationsofthemanyresearchersdedicatedtothestudyofaluminiumcorrosion.1
Likethepreviousversion,thisneweditionaimsatawidereadershiprangingfromaluminium userstoacademia.Bothwillfindusefulinformationonaluminiumcorrosionbasedonthestateof knowledgeacquireduptothetimeofwritingthisnewedition.
Iwouldliketothankallthosewhohavegivenmetheirprecioussupportinthewritingofthisbook:
➢ DrLionelPeguet,corrosionandsurfaceR&Dengineer,CTECConstelliumTechnologyCentre, Voreppe,France
➢ Jean-SylvestreSafrany,researchengineer,SurfaceTreatments,CTECConstelliumTechnology Centre,Voreppe,France
➢ Franc¸oiseSaillard,informationspecialist,CTECConstelliumTechnologyCentre,Voreppe,France
➢ DamienFe ´ ron,CEASaclay,France,presidentoftheEuropeanCorrosionFederation
➢ BrunoSavelli,CEASaclay,France,DirectiondelaRechercheFondamentale,Servicede Valorisationdel’Information
1Over2000publicationsonaluminiumcorrosionpublishedfromthebeginningofthe20thcenturyuptothepresentdayhave beencitedinthisbook.
➢ PhilippeMarcus,directorofresearchattheCentreNationaldeRecherchesScientifique(CNRS), ChimieParisTech
➢ MichelJannier,expertinaluminiumsurfacetreatmentprocesses
➢ MichelPinc¸on,expertinaluminiumsurfacetreatmentprocesses
➢ MichelGarat,aluminiumfoundryconsultant,formerPechineyR&Dmanager
➢ HassinaFounas,executiveassistantoftheFrenchAnti-CorrosionCentre(CEFRACOR),Paris
IwouldliketothankHughDunlopforagreeingtotranslatemytextintoEnglish.IchoseHugh becauseofhisexperienceandknowledgeofaluminiumsurfacephenomenaandsurfacetreatments, havingbeenanengineerandgroupleaderintheConstelliumCTECVoreppeResearchCentre (formerlyPechiney & Alcan)for27yearsandhimselftheauthorofmanypublications.
IwouldalsoliketoexpressmythankstoGeoffScamans,chiefscientificofficeratInnoval Technology(Banbury,UK)forhisexpertreviewofseveralchapters,particularlythoserelatingto thedifferenttypesofaluminiumcorrosion.Iamverygratefulforhisknowledgeableinput.
IwouldliketoexpressmygratitudeonceagaintoAndre ´ Guilhaudis(1918 2008),whowas Pechiney’scorrosionexpertfrom1945to1980.HewelcomedmetothePechineyResearchCentre inChambe ´ ryin1957andsharedwithmehispassionforaluminiumandhisexperienceincorrosion.
C.VARGEL
Inge ´ nieurENSEEG 15November2019
Introductoryremarks Itiscustomary,andforconvenience,torefertoaluminium,butwhatismeantinmostcasesare aluminiumalloys.Itshouldberecalledthatunalloyedaluminiumaccountsforjustover10%ofthe world’sannualconsumptionofallaluminiumproducts.
However,forthesakeofsimplicity,Iuse‘aluminium’insteadofthetraditionalexpressions ‘aluminiumanditsalloys’or‘aluminiumandal uminiumalloys’.Itshouldnotbeconcludedthat thecorrosionresistanceofallaluminiumalloys isthesameinanyenvironment!Therearecertainly somesimilarities,buttherearealsoimportantdifferencesbetween2XXXand7XXXseriesalloys andthoseoftheotherfamilies.ThatiswhyIhavemadethisdistinctionwheneverappropriate.
Whenoneormorealloyshavebeenusedforcorrosiontestsinagivenenvironment,itseemed desirabletometomentionthembecausetheywerepartofthetestprotocolchosenbythescientists andcontributedtoitsvalidation.Similarly,itseemsessentialtoindicatethealloyscommonlyused inanapplication.Thesearereferencesthathelptoestablishtheuseandstrengthenthechoiceof prescribersandusers.
ThedesignationofwroughtandcastalloysemployedisthatoftheAluminumAssociation1 [1].To facilitatethereadingofPartsEandFdealingwiththecorrosionresistanceofaluminiuminchemicals, Ihavequoted(between{})theirADRnumber,2 whichistheUnitedNationsfour-digitcodeforthe substanceinquestion.ThedesignationoforganicchemicalslistedinPartsMandNshallpreferablybe thataccordingtotherulesofIUAPCnomenclature.3
Excludedfromthescopeofthisworkarealuminiumpowderproducts,powderandgranuleswhose propertiesandapplicationsarenotrelatedtotheapplicationsofcastproducts,wroughtsemifinished products,rolledproducts,extrudedproductsandsoon.Alsoexcludedaresinteredaluminiumpowder compositesaswellasaluminizedsteel.
Reference
[1]KaufmanJB.Understandingwroughtandcastaluminiumalloysdesignations.[Chapter3],ASM International,p.23 37. https://doi.org/10.1361/iaat2000p023.
1TheAluminumAssociation,1400CrystalDriveSuite,430ArlingtonVA22202. 2ADR,accordfordangerousgoodsbyroad.
3IUAPC,InternationalUnionofPureandAppliedChemistry.
Historicalreviews A.1 Chapteroutline 1.1Chemicallyproducedaluminium........................................................................................................4
1.2Electrochemicallyproducedaluminium..............................................................................................4 References..............................................................................................................................................6
ThechemistLouisGuytondeMorveau(1736 1816),aco-workerofAntoineLaurentLavoisier (1743 1794),coinedtheword‘alumine’foroneofthesulphatescontainedinalum. Alumine is derivedfromtheLatinword alumen,whichissaidtohavebeenusedforpotassiumalum KAl(SO4)2 12H2OduringtheRomanperiod.Aluminiumcompoundswereusedinlargequantitiesin antiquepottery,asdyestuffandasanastringentinmedicine [1].Itisnottheword‘alumine’thathas cometodesignatealuminiumorebuttheword‘bauxite’.Thisisbecausein1821PierreBerthier (1782 1867),aminingengineer,discoveredthattheredsoilofthevillageLes-Baux-de-Provencein Francecontained40 50wt.%ofwhathetermed‘hydratedalumina’ [2].
Subsequently,in1861FrenchchemistHenriSainte-ClaireDevillenamedtheore‘bauxite’.In fact,bauxitecompositionsvarydependingonthesourceoforebuttheyusuallycontainaluminium hydroxidessuchasgibbsiteAl(OH)3,boehmite g-AlO(OH)anddiaspore a-AlO(OH),therestbeing composedessentiallyofironoxidesandhydroxides,mainlyhaematite, a-Fe2O3 andgoethite FeO(OH)(thesourceofitsredcolour),andthealuminosilicateclaymineralkaolinite,Al2Si2O5(OH)4. EventhoughitisthemostabundantmetalintheEarth’scrust(83,000ppm)andthethirdmost abundantelementafteroxygenandsilicon,aluminiumdidnotbecomeanindustrialmetalbeforethe endofthe19thcentury.Aluminaisoneofthemoststableofalloxides,withanenthalpyofformation, DG,of 1,582kJ$mol 1 (theenthalpyofironoxideis 1,015kJ$mol 1).Itishenceverydifficultto reducealumina.
ThediscoveryofmetallicaluminiumisattributedtoSirHumphreyDavy(1778 1829).He referredtoitusingtheterm‘aluminium’in1809.Byelectrolysisofmoltenaluminiumsalts,he obtainedanalloyofaluminiumwithiron,becausehehadusedanironcathode [3].ThechemistHans ChristianOersted(1777 1851)andlaterFriedrichWo ¨ hler(1800 1882)chosetoreducealuminium chloridewithpotassium.Thechloridehadbeenpreparedbychlorinationofbauxiteinthepresenceof carbon.ItwasWo ¨ hlerwho,in1827,succeededinproducingasufficientlypuremetaltodetermine someofitsproperties,mostnotablyitslowdensity.
CorrosionofAluminium. https://doi.org/10.1016/B978-0-08-099925-8.00001-6
Therewereinitiallytworoutesfortheindustrialproductionofaluminium:
•Byachemicalmethod(1856 1889);
•Followedbytheelectrochemicalprocessinventedin1886andstillinusetoday.
1.1Chemicallyproducedaluminium In1854,HenriSainte-ClaireDeville(1817 1881)improvedWo ¨ hler’sprocess.Hereplacedpotassium withsodiumfortworeasons:thereductionof1molofAluses3molofsodium,totalling60g,instead of3molofpotassiumamountingto117g.Atthattime,sodiumwaslessexpensivethanpotassium.He alsoreplacedaluminiumchloride,whichisrathervolatile,withasodiumaluminiumchloride.
ThefirstplantwascreatedinParis,in1856,inthe‘LaGlacie ` re’area,butsoonitwasshutdown:
‘ThesmallplantofLaGlacie`re,locatedinaninnersuburbofParis,amidsthousesandmarket gardens,releasingintotheatmospheresmokeladenwithsodaandchlorine,wasforcedtoceaseits aluminiumproductionafternumerouscomplaints’ [4].
Inthespringof1857,Sainte-ClaireDevillemovedtheplanttoNanterre(nearParis),farawayfrom residentialareas.In1859,productionreached500kg.Thatsameyear,whenLouisLeChatelierhad patentedareductionprocessofaluminawithsodiumcarbonate,aplantwasbuiltinSalindres,closeto Ale ` sintheGardFrenchdepartment,notfarfromthebauxitesupplyandthesaltfieldsofLaCamargue. TheproductioninSalindreshadvariedfrom505kg,whentheplantwasstartedin1860,to2,959kgin 1880,whenthisprocesswasdiscontinued.
Thefirstkilogramsofaluminium,producedin1856,weresoldslightlymoreexpensivethansilver, around300francs,equivalenttoUS$3,200in2016.Duringthedecade1880 1889,themetal producedinSalindreswassoldforbetween60and70francsperkilo,theequivalentofUS$750 800 in2016.Aluminium,whichSainte-ClaireDevillelikedtocomparetosilver,wasmainlyusedfor silverwareandjewellery.CharlesCristofle(1805 1863),thecelebratedParisiansilversmith,produced castartworkmadeofaluminiumalloyedwith2%wt.copper.In1858,thesonofNapoleonIIIwas offeredarattlemadeofaluminium.
1.2Electrochemicallyproducedaluminium In1871,Ze ´ nobeGramme(1826 1901)inventedthefirstrevolvingmachinecalleda‘dynamo’.The useofpowerfulsourcesofdirectcurrentmadeitpossibletoenvisionproductionmethodsbasedon electrolysis.Sainte-ClaireDevillehadtriedunsuccessfullytoelectrolysemoltenaluminiumchloride. ThemanufacturingprocessofaluminiumbyelectrolysisofmoltenaluminawasdevelopedinFrance byPaulLouisToussaintHe ´ roult(1863 1914),whofiledapatenton23April1886,andintheUnited StatesbyCharlesMartinHall(1863 1914),whofiledhispatenton9July1886.Bothhadsucceeded indissolvingalumina(meltingpoint2030 C)incryolite3NaF AlF3,whichmeltsat977 C,withthe industrialmeltcontainingabout2 3wt.%alumina.
In1887,Bayerfiledapatentforamethodtoextractaluminafrombauxitebasedontheattackof bauxitebyhotcausticsoda.He ´ roultwenttoNeuhausen,Switzerla nd,inordertosetuphisprocess. Theyearafter,hereturnedtoFranceandin1888createdtheFrogesplantnearGrenobleinFrance wheretheproductionwas1,100kgin1889.SeveralplantsweresetupinFrance,Switzerland, andtheUnitedStates.Sixthousandmetrictonswereproducedin1900,andthesalespriceof
TableA.1.1Worldproductionofprimaryaluminium
19006 191044 1920125 1930270 1940780 19501,500230 19604,450790 197010,5002,230 198015,4004,670 199019,5008,470 200024,65012,700 201042,30020,200 201557,70025,000 201659,900 201763,400
FrompublishedrecordsoftheWorldAluminium InternationalAluminiumInstitute.
aluminiumstabilizedataroundUS$3.30perkilogr am.Thiswasthestartoftheindustrialadventure ofaluminium.Theworldproductionofso-calle dprimaryaluminiumamountedto6,000tonnes in1900(see TableA.1.1 )andhassteadilyincreased(see Fig.A.1.1),especiallysince1950.More recentlytherehasbeenafurthersharpincreaseassociatedwiththedevelopmentofChinese production(<5,000kTin2000to >30,000kTby2015).
FIGUREA.1.1 Worldproductionofprimaryaluminium.
Itisworthnotingthat,duetoitsinherentresistancetocorrosionandmorerecentlythroughthe developmentofaluminiumrecycling,75%oftotalworldaluminiumproduction(w750MT)isstillin productiveuse(eversince1888).
References
[1]Dictionnairehistoriquedelalanguefranc¸aisesousladirectiond’AlainRey.Paris:EditionsRobert;1994. p.55.
[2]BerthierP.Analysedel’aluminehydrate ´ edesBauxdeProvence.AnnalesdesMines1829;5(2):531 4.
[3]PascalP.Nouveautraite ´ deChimiemine ´ rale.e ´ diteurs,Paris:MassonetCie;1960.
[4]Saint-ClairDevilleH.Del’aluminium.Sesproprie ´ te ´ s,safabrication,etsesapplications.Paris:MalletBachelier,Imprimeur-Libraire;1859.p.8.
CHAPTER Physicalpropertiesof aluminium A.2 Theprincipalphysicalpropertiesofunalloyedaluminiumarelistedin TableA.2.1
TableA.2.1Propertiesofunalloyedaluminium
Longitudinalelasticmodulus,EMPa69,000
Poisson’sratio, n 0.33
aThisisthegenerallyacceptedvalueforthedensityofmetalbetween99.65%and99.99%pure.At700 C,thedensityof moltenmetalof99.996%purityis2,357kg.m 3 CorrosionofAluminium. https://doi.org/10.1016/B978-0-08-099925-8.00002-8
Thereflectivityofbareandanodizedaluminiumdependsbothonthesurfaceaspectandonthe wavelength(Fig.A.2.1).Reflectivityincreaseswithpurity:withbrightmetalanodizedtoanoxide thicknessof5 mm,reflectivityincreasesfrom75%onmetalwithapurityof99.6%to85%reflectivity fora99.99%puremetal(Fig.A.2.2).
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