MINERALOGYANDSURFACEPROPERTIESOFTHECLAYFRACTION

AFFECTING SOILBEHAVIOURANDMANAGEMENT

RobertBrinkman

Department ofSoilScienceandGeology

P.O.Box37,6700AAWageningen,TheNetherlands

Abstract
Themineralcompositionoftheclayfractionisdiscussed intermsof
crystalstructureandofchemicalandphysicalpropertiesrelatedto
mineralogy.Themaintransformationprocessesaffectingtheclayfractionand
theconditionsinwhichtheyoccurarebrieflydescribed.Examplesaregiven
ofrelationsbetweenlandscapeposition,dominanttransformationprocessand
claymineralogy.Differencesbetweensurfacesofclaysandtheirbulk
compositionmayarisenaturally,asexternalconditionschange,andbythe
actionofman.Althoughitisgenerally impracticaltoattemptchangesin
compositionoftheclayfraction,somechangesinsurfacepropertiesare
feasible.Thesemaymaskoralleviateundesirablecharacteristics oftheclay
fractionasawhole.
 MINERALOGY AND SURFACEPROPERTIES OFTHE CLAY FRACTION

AFFECTING SOILBEHAVIOUR AND MANAGEMENT

Changing the fertility of a soil isa relatively simple,although

temporary,measure. It ismore difficult to change the physical orhydro-
logical characteristics of a soil, although cultivationmeasures,drainage ani
irrigation or mulching can bring about desired changes fora season ora
longer period.
The clay mineral composition of a soil generally cannot be changed by
economic means within ahuman lifetime.The user of the land has to live with
themineralogy of the clay fraction.
In rare cases,rapid changes may occur in the clay fraction of soils.For
example, there are indications that halloysite,a crystalline clay mineral,
may be formed inanamorphous clay fraction within a fewyears once the soil
dries out periodically. Such instances can be found in young volcanic
materials when an original rainforest iscut and replaced by arablecrops.

In 1934,Edelman hypothesized that the clay fraction of soils could

consist ofmixed gels containing Si,Aland bases,aswell as crystalline
layer silicates of different kinds,and that these could be formed from
weathering products of theprimary minerals inthe coarser fractions.He also
postulated ••.hatthe crystalline clays could consist of complicated mixed
crystals: both inthe sense ofmixed layer structures and inthe sense of
solid solutions containing a range ofmajor and trace constituents.
This balanced and modern viewwas incontrast toothers,who neglected
 -3-

structureconsiderationsorcontentsofbases,andconsidered theclay
fractiontoconsistofaninorganic,colloidal,hypotheticalsoilacid
(termed,e.g.,pyrophyllicacidbecauseofitssimilarityincompositionto
pyrophyllite).

Weshallneedtoconsiderthecrystallinenatureofthebulkoftheclay
fractioninmanysoils,thepresenceofamorphousorx-rayamorphousmaterial
whichmaydeterminethesurfacepropertiesoftheclayfractions,andthe
importantandrapidchangesthatmayoccurinthesurfaceoftheclay
fraction,evenwhilethebulkofthematerialmayremainsubstantially
unchanged incompositionorstructure.
ThereferencesinthispaperincludeseveralchaptersofabookwhichI
stillconsidertobethebestsinglesourceofinformationonthe/clay
fractionofsoils,alsofornon-claymineralogists:DixonandWeed (eds),
1977.

MINERALCOMPOSITIONOFTHECLAYFRACTION
Thepropertiesofasoilaredetermined toalargeextentbythe
proportionandthenatureoftheclayfraction.Inmostsoils,thisconsists
of
- layersilicates(claymineralsinthestrictsense);
- othercrystallinemineralssuchasquartz,anatase,orpalygorskite(a
magnesium-aluminium silicatewithafibrousstructure),whichwillnotbe
discussedhere;
- ironand,insomecases,aluminiumoxidesandhydroxides,whichmaybe
crystallineoramorphous;
- amorphousorparacrystallinealuminosilicates(allophane,imogolite);
- organiccompoundsassociatedwiththemineralpartoftheclayfractions.
SomepropertiesofthemineralmaterialsaresummarizedinTable 1and
furtherdiscussedbelow.
Mostsoilsinplainscontainanassemblageofclayminerals,whileupland
soilstendtohaveasimplerclaymineralogy.Inbothcases,oneorafewclay
mineralsmaydominatethesoilproperties.
Forpracticalpurposes,twobroadgroupsofclaymineralsmaybe
distinguished:agroupwithpermanentcharge,whichhaveamoderateorhigh
cationexchangecapacity (cec)atallpHvaluesofinterest,andagroupwith
pH-dependentcharge.
Claymineralswithpermanentcharge
Theclaymineralswithpermanentchargehave layersconsistingoftwo
tetrahedralsheetsenclosing anoctahedralsheet:mainlysilicaandmainly
aluminiumormagnesiumoxide,respectively.SubstitutionofAlorFe(HI)for
Siinthetetrahedralsheets,orofMg,KorFe(II)forAlintheoctahedral
sheetcausesthepermanentchargeofthemineral.Theswellingclayminerals
orsmectitessuchasmontmorillonite,beidellite,nontroniteareexamplesof
thisgroup.
Theexchangeablecationsthatcompensatethepermanentchargeare
electrostatically bound totheclaysurfaces;partofthem,aluminiumin
particular,closelyattached tothesurface,theremainderinadiffuselayer,
ratherliketheatmosphereovertheearth'ssurface.Inthenearbypartsof
thislayerthereareveryfewanions,becauseofelectrostatic repulsion,and
thewatermoleculesneartotheclay surfacearefirmlyoriented bythe
electricfield:notfree,likeinwater.Thediffuselayeristhinwherethe
exchangeablecationsarelargelytrivalent(AI)anddivalent (Ca,Mg), and
wherethesoilsolutionisconcentrated. Withincreasingdilution,oran
increasingproportionofmonovalentcations(Na),thediffuselayerbecomes
thicker.
Suchclayscancontainmuchwaterintheirdiffuselayersthatis
unavailabletoplants.InthesmectiteclaysoilsoftheSudanGezira,for
example,moisturedepletionbyplantsstopsatabout25masspercent,while
soilsaturationisatabout36masspercent(Farbrother,1970).Whilewater
canbetransported throughthediffuselayers,albeitslowly,saltscannot
becauseoftheexclusionofanionsfromthem (Smilesand Bond,1984).This
causesalowefficiency ofsaltremovalfromsalineheavyclaysoils:salt
concentrations inthedrainagewaterarelowerthaninthesoilsolution.

Thisisnottheonlyreasonforrelatively lowefficienciesofsalt
removalfromclayswithahighcationexchangecapacity.Mostswellingclay
soilsarestructured,havingpedssurroundedbycracksowingtoshrinkage;
manyalsohavetubularporesthatareduetobioticactivity.AsBoumaandco-
workershaveshowninseveralstudies(referencesinBouma,1984),partofthe
irrigationwaterapplied onastructured clayey soilflowsthroughthelarge
voidsandisdrainedwithoutremovingmorethanasmallfractionofthesalt
withinthepeds:aprocesscalled short-circuiting.Ifsolubleplantnutrients
areappliedtothesoilsurfaceinsuchasystem,partofthesewouldalsobe
 -5-

removedbelowtherootingzonebyrainorirrigationwatershort-circuited
throughlargevoids,becauseofinsufficientcontactwiththecationexchange
siteswithinthestructuralelements.
Thesalt-sievingeffectcanbeminimized,butnotentirelyavoided,by
keepingthesaltconcentrationhighforaslongaspossibleandincreasingthe
proportionofdi-andtrivalentcations.Short-circuitingcanbeminimizedor
eliminated byloweringtheratesofwatermovementthroughthesoiltoavoid
saturation,e.g.bylowratesofirrigationwaterapplicationorbypuddling
thesurfacehorizon.

Swellingclaysoilsmaybecomevirtually imperviousbywatersaturation,
forexampleunderwetland rice,orbyexcessiveorfrequentirrigation.
Shrinkagebydryinggenerally restoresthestructureofthesurfacehorizon
andthehydraulicconductivityofthesubsoilhorizonsthroughtheformation
ofanintersectingsystemofcracks.Thisisusefulfordrylandcropsafter
wetland rice,forexample.
Insoilswithhighshrink-swellratios,bulkdensityisprobablynot
limitingforrootpenetration(Jones,1983),incontrasttoothersoils.
Onslopesinwater-saturatedconditions,soilscontainingmainlysmectite
aresubjecttoslowcreepofthesurfacematerialorsuddendeepslumping
alongarotationalplane(IstokandHarward, 1982).
Theswellingclaymineralshaveamoderateproportionofsubstituted
atoms,hencearelatively lowchargedensity.Forthatreason,the
exchangeablecationsareboundonlymoderatelystrongly,spreadoutina
diffuselayer.Eachlayeroftheclaystructurecontributestothecation
exchangecapacityandtotheswellingcharacteristics.

Otherclaymineralswithasimilarstructurehavemuchhigherproportions
ofsubstitution,henceahighchargedensity:illiteandvermiculite.
Thesebindcertaincationswithenoughenergytofixthembetweenadjacent
layersinnon-exchangeable form.ParticularlyionssuchasK,whichfitneatly
inholesintheclaystruture,servetoprodigearigidstackofclaylayers.
Onlytheoutersurfacesand,toavaryingextent,inperfectlyfittinglayers
withinthestackedstructure,thencontributetocationexchange,andthese
claymineralsswellandshrinkmuchlessthanthesmectites.Ontheonehand,
theseclaymineralscontainmuchKwithintheirstructure,andthisbecomes
availabletoplants,butslowly,duringweathering.Ontheotherhand,parts
 -6-

oftheclaystructurethataredepletedofKcanveryreadily fixfertilizerK
(Douglas,1977,p.285-287;Borchardt,1977,p.314)whenthisispresentin
temporarilyhighconcentration.Sincetheammonium ionisphysicallyvery
similartopotassium,NH, canalsobefixed byvermiculiteorK-depleted
illite(IRRI, 1983),butsomewhatlessstrongly.
Oneoftheswellingclayminerals,beidellite,hasastructure inwhich
NH^ fitsparticularlywell.Soilscontainingbeidellitefixammoniumvery
strongly,aswellasK(Bajwa,1981a).

ClaymineralswithpH-dependentcharge
Theclaymineralswithvariablechargehavelayersconsistingof
alternating tetrahedralsilicaandoctahedralaluminiumhydroxidesheets,with
verylittlesubstitutioncharge.Themainexamplesarekaoliniteand
halloysite.Kaolinitenormallyoccursashexagon-shaped orrounded flakes,of
theorderof 1urnindiameter,muchcoarserthantheswellingclayminerals.
Halloysiteoccursintwovariants:ahydrated formcontainingwaterlayers
betweentheclaylayersandadehydrated form,similarto,butlesswell
ordered thenkaolinite.Halloysiteoftenoccursascurvedorrolledplates
(tubular)orasglobularaggregates,muchfinerthanmostkaolinites.

Thealuminiumattheedgeofthesheetsispositivelycharged,particu-
arlyatlowpH,whichproducesasmallanionexchangecapacity.Whereasions
suchaschlorideornitrateareinfactexchangeableonsuchsites,phosphate
andsilicaareboundtightly,andremainfixed (Muljadietal, 1966;summary
inDixon1977,p.388).Kaolinitesgenerallyhavearelativelycoarseparticle
size,andinthatcasetheamountoffixationissmall.Fine-grained
kaolinitesaswellashalloysites,whichareextremelyfine-grainedwithlarge
edgeareas,canfixlargeamountsofappliedphosphate(Bajwa,1981b).
Theseclaymineralshaveaverylowcec,increasingwithpHby
dissociationofOHgroups.Theyshowvirtuallynoswellingorshrinkagewith
changesinwatercontent.Soilsdominated bykaoliniteorhalloysitegenerally
havenooronlyweakpedstructure.Forsuchsoils,Jones(1983)estimates
thatrootpenetrationisimpededaboveacriticalbulkdensity,
(1.2+0.005xsand 'A)
Soilsonsteepslopeshavingaclayfractionwithsmallwaterholding
capacity,forexamplemainlykaoliniteordehydratedhalloysite,arenot
subjecttocreeporslumping,butmayformdebrisavalanchesinverywet
conditionswherebeddingplanesoftherockrunparalleltotheslope(Istok
 -7-

andHarvard,1982).
Oncesoilsdominatedbykaoliniteorhalloysitehavebecomedensebyland
clearingactivities,byrainimpact,orbywheelorbullocktrafficorplough
pressureduringcultivation,theydonotregaintheirstructureandhydraulic
conductivitybywettinganddryingliketheswellingclaysoils,butneedto
berestoredbybiologicalormechanicalmeans.Thiscanbedonebystimulation
ofwormactivitythroughmulching.Initialrippingorcultivatortreatmentmay
beuseful,butonly ifthesoilisdryormoist.Thesameproblemoccurswhere
suchsoilsarepuddledforawetlandcropandsubsequentlyusedforadryland
crop.Proceduresforsafemanagementofsuchsoilsaregiven,e.g.,by
Vierhout (1983).

Aluminium-interlayeredmaterials

Incertainsoilscontainingclaymineralswithpermanentcharge,the
interlayerspacesoftheseclaymineralsareblockedbysheetsofpartly
neutralizedaluminium ions.Thesesheets,incompleteandgenerallypoorly
3+
ordered,consistofringstructuressuchasAlg(OH),e .Theyarenot
exchangeable,neutraliseaconsiderablepartofthecec,andrestrictthe
swelling thatcantakeplace.Fairlycompletealuminiuminterlayersthus
convertclayswithpermanentchargeintomaterialssimilartokaolinite.

Evenmoderateproportionsofaluminiuminterlayeringhaveagreateffect
onstabilityofclaysagainstdispersion,asexperimentallyverifiedby
MuranyiandBruggenwert (1984).Atlowsaltconcentrations,anilliteclay
soilmaterialdispersedandcollapsedintoavirtually impermeablemassat
exchangeablesodiumpercentages(ESP)about30andabove,whereasthepartly
aluminium-interlayeredmaterialremainedpermeableatallESPvaluestested,
upto80percent."
Thismayberelevantforthereclamationofsodic,orsaline-sodicsoils.
Acidformedafterapplicationofsulfuroroffinelygroundpyriteasinparts
ofIndia,orwasteacidfromchemicalindustries,asusedlocallyinthe
U.S.S.R,presumablydissolvesomealuminiumfromclaymineralsbesidesCafrom
limethatmaybepresent.Thiswouldproducealuminiuminterlayersbesides
dissolvedcalciumsulfate,bothaidingreclamation.

Oxidesandhydroxidesofiron(III)andaluminium

Soilscontaininglow-activityclays(claysfractionswithalowcec)
oftencontaingibbsite(Al(OH)o)besideskaolinite,generallyasdiscrete
clay-sized particles.Thismaterialaggravatesthemanagementproblemsofsuch
soils,because itscecaswellasmoisture-holding capacityareessentially
zero,andbecauseappliedphosphateisfixedmoreseverely bygibbsite thanby
kaolinite.

Iron(III)oxides,too,mayoccurintheclayfractionasdiscrete,
crystallineparticlesofgoethiteorhematite.-Thesetwogenerallyhavea
relatively lowspecificsurfaceandhavesimilarpropertiesasgibbsite,at
leastinwelldrainedsoils.
Ironoxidesorhydroxidescanalsoformgenerallydiscontinuouscoatings
onkaoliniteanotherclayminerals.Theseareoftenamorphous,haveavery
highspecificsurface,anddrasticallymodify thechargecharacteristicsand
thephysicalpropertiesofsuchsoils.Thecationexchangecapacity isvery
low.Phosphatefixationissevereandremainssevereexceptafterverylarge
phosphateapplications.Thestructurestability ismuchhigherthanthatof
kaoliniticsoilswithlowproportionsofironoxides:infiltrationrates
remainhighevenafterrainfallimpactandtheporescollapselessreadilyby
traffic.

Insurfacesoilswithhighorganicmattercontents,theassociationof
organicmatterwiththeironoxidescounteractsalltheseeffectstosome
extent.Wetland conditions,too,modify theeffectsofthefinelydistributed
iron(III)hydroxides.Reductionofiron(III)phosphatesincreasesphosphate
availability;reductionofFe(III)oxidestoFe(II)increasescecdirectlyas
wellasbytheassociated riseinpH.

Amorphousaluminosilicates
Amorphousaluminosilicatesandrelatedmaterialswhichonlyhaveshort-
rangeorderincludeallophaneandimogolite.Theseoccurinmanyyoung
volcanicsoils.Suchsoilshaveveryhighmoistureretentionandphosphate
fixationandalowtoveryhighpH-dependentcec.Theymanycontainveryhigh
proportionsoforganicmatter,presumably protectedagainstrapidmicrobial
decompositionbytheassociationwithlargeamountsofaluminium.
Thesesoilsarequitestableagainstrainimpactandnoterodible,but
mayfailunderload.Failure,mayoccurintheformoflandslides,slumpsor
creep(WarkentinandMaeda,1980).Soilscontainingamorphousclay
constituentsandhydratedhalloysitemayturnliquid,andslow-moving
earthflowoverconsiderabledepthmayoccurfrequently,evenwhereoverall
 -9-

slopesarenotverysteep(IstokandHarvard,1982).

Allthetypesoffailurementioned forsoilswithdifferentclay
mineralogiesoccurinwater-saturatedcondition.Preventioninalandscape
withwetlandterraceswouldhavetodependondrainageatthebottomofthe
terracewallsand,wherepossible,oncarefulconstructionoftheterraces
withthemostslowlypermeablematerialinthesurfacelayer.Thesetechniques
havebeenraisedtothelevelofafineartbytheIfugaosofcentralLuzon,
Philippines(MoormannandvanBreemen,1978,p.89-90;vanBreemenetal.
1970, p.39-73).

ORIGINSOFTHECLAYFRACTION;TRANSFORMATIONPROCESSES
Theclayfractioninsoilsmaybetransportedanddeposited,together
withotherfractionsofthesediment;itmaybeinheritedfromasedimentary
rockthathasphysicallyweathered;oritmayhavebeenformedbyweathering
ofmineralsincoarserfractions,ortransformedfromotherclayminerals.

Onyounglandsurfaces,suchasrecentalluvialplainsorslopeswitha
moderateorhighrateoferosion,thenatureoftheclayfractionislargely
determinedbytheoriginalmaterial.Sincemanysedimentshavearatherwide
sourcearea,theirclayfractionsoftenareamixtureof,e.g.,illite,
montmorilloniteorvermiculitewithorwithout somealuminiuminterlayering,
kaoliniteandsomeclay-sizedquartz.Suchmixturestendtoberatherconstant
withinanalluvialplainbutmayvaryfromoneriverplainorestuaryto
another.

Onolderlandsurfaces,forexampleonriverorcoastalterracesorin
uplandareaswithlittleerosion,weatheringandclaytransformationbecome
moreimportant.Afewmajorclaytransformationprocesses,actingonavariety
oforiginalmaterials,canexplainthedifferentclaymineralogiesthatmay
occur.Theseprocesses,discussedatsomelengthinBrinkman(1982),are
summarizedbelow.Theyarethefollowingfive,inorderofdecreasingareal
importance.
-Hydrolysisbywatercontainingcarbondioxide,whichremovessilicaaswell
asbasiccations.
-Cheluviation,whichdissolvesandremovesespeciallyaluminiumandironby
chelatingorganicacids.
 -10-

- Ferrolysis,acyclicprocessofclaytransformationanddissolutionunder
theinfluenceofalternating reductionandoxidationofiron,whichlowers
thececbyaluminium interlayering.
- Dissolutionbystrongmineralacids,whichattacksallclayminerals,
producingacidaluminium saltsandamorphoussilica.
- Claytransformationunderneutraltostronglyalkalineconditions (reverse
weathering),whichmaygiverisetomineralssuchasmontmorillonite,orin
extremecasespalygorskiteoranalcime.

Hydrolysisbywatercontainingcarbondioxide
Hydrolysisbywatercontaining CO?,alsocalleddesilication,sometimes
referred toas"weathering"without furtherspecification,isadominant
processofclayformationandtransformationparticularly inthehumid
tropics,butalsoinpartofthetemperatezone.
WaterinequilibriumwithatmosphericCC>2hasapHofabout5.6,thesane
asuncontaminated rainwater.Whenexcessrainwaterpassesthroughasoil,
claymineralsbegintodissolvecongruently (proportionately)untilthe
solubilityproductofgibbsite,Al(0H)o,isreached.Thishappensalreadyat
_Q

anAlconcentrationoftheorderof 10 mol/1atpHvaluesabout5.5 to6.

Fromthenon,gibbsite isprecipitatedwhileclaymineralscontinueto
dissolveandsilicaisremovedbythepercolatingwater.Thus,gibbsiteis
formedin,e.g.,kaolinitic soilsunderperhumidconditions.
Whereleachingislessrapidandwheretheclayfractioncontains
mineralssuchasmontmorillonite orillite,whichcontainahighproportionof
silicaaswellasbasiccations,continueddissolutioncausesthesilica
concentrationtorisefurther,aboveabout10 mol/1.-AThen,kaoliniteis
stableovergibbsite,sokaolinitemaybeformedfrom,forexample,
montmorillonite orfeldsparsunderhumidconditions.
Inboththesecases,anyironthatisreleasedfromthemineralstructure
isprecipitatedashydroxideorasgoethite(FeOOH)becauseofitsextremely
lowsolubility.
WhereconcentrationsofMgorotherstructuralcationsarerelatively
highduringweathering,montmorillonite orvermiculitemaybetransformedinto
theiraluminium-interlayeredequivalents,becausethesearestableover
kpoliniteandgibbsiteunderetheseconditions.Evenincaseswherekaolinite
isstableoverthealuminium-interlayeredmaterial,thelattermaystillbe
formedasan.intermediate stepinthetransformationsequence.
 -11-

Thestabilityrelationshipsreferred tointhissectionarebasedon
thermodynamics,butcanbevisualizedmostsimplyintermsofsolubility
productsthatdeterminewhetheragivencompounddissolvesorisprecipitated.

Hydrolysisofclaymineralsoroffeldsparsorotherweatherableminerals
incoarserfractionsisaslowprocess,inwhichsilicaisremovedatratesof
about1to10mg/1,andbasiccationsatsimilarorlowerrates.
Wherepotassiumconcentrationsinsolutionarekeptverylowbyplant
uptake,dissolutionofKfromillitemayproceedfasterthandesilicationof
thematerial.Then,illitemaybetransformed intoK-depleted (swelling)
illite,andwithfurtherminorchangesintovermiculiteoraswellingclay
mineralsimilartobeidellite.These,inturn,wouldbesubjecttotheslower
tranformationsdiscussedabove.

Decomposition bystrongacids
Whenpyriteclays,occurringinmanymangroveareas,areoxidizedby
drainage,sulfuricacidisformedbyoxidationofthepyrite.Thisrapidly
dissolvesclayminerals,atpHvaluesbetween2.5and3.5,untilthesilica
concentrationisabout2x10 mol/1(about 120mg/1).Then,amorphoussilica
isprecipitated.
IfMgandKconcentrationsarehighenough,forexampleinsaline
conditions,montmorilloniteandillitemaybestablewithrespectto
kaolinite.Then,thedirectionofclaytransformationisawayfromkaolinite,
incontrasttohydrolysis.
Dissolutionbystrongacidsgivesrisetoaluminiumconcentrations
rangingfrom 1tosomehundredsofmg/1,severalordersofmagnitudehigher
thaninhydrolysisbywaterwithC0 2 ,andtosilicaconcentrationsofabout
100mg/1, about10timeshigher (vanBreemen,1976).Theprocesscantherefore
proceedmuchfasterthanhydrolysisifthereactionproductsareremoved,
e.g.,indrainagewater.
Reactionproductsthatarenotremovedmayformamorphoussilicaand
aluminiuminterlayersinswellingclaymineralsoncethepHhasrisenagainto
about5orhigher.

Cheluviation
Duringcheluviation,organicacidsspecificallydissolvealuminiumandiron,
andremovetheminchelatedform.Thedirectionofclaytransformationis
 -12-

similartothatduringdissolutionbystrongacids.
Cheluviationoccursextensively inhumidclimateswithacoldseason,but
onlylocallyinverypoor,sandymaterialswithpoordrainage inthehumid
tropics.Itisnotdiscussedherebecauseitisofnegligibleimportancein
wetlandordryland riceareas.

Ferrolysis
Claydecompositionandtransformationbyferrolysisrequirestwo
alternating setsofcircumstances.Duringwater-saturated conditionswithsome
leaching,thesoilisreducedandthepHrisesslowlybytheconversionof
2+ becomesexchangeableaswellassoluble.Partofthe
Fe(OH)^intoFe ,which
exchangeablebasiccationsareremovedbyleaching.Watersaturation
alternateswithdryingandoxygenentry.Then,exchangeableFe 2+
isoxidized,
producingFe(OH)^andexchangeablehydrogen.Thisattackstheclaymineralsas
dootherstrongacids,butthealuminiumandothercationsreleased fromthe
claystructurebecomeexchangeable,notsoluble.Thesilicafromtheclaymay
remainasunsupported edgesoftheformerclaystructure.
Duringthenextperiodofwatersaturation,iron(III)hydroxidesare
2+ ofwhichdisplacesexchangeablealuminiumand
againreduced toFe ,part
othercationsintothesoilsolution.Partofthesilicaintheunsupported
edgesisdissolvedaswell.Leachingwatermayremovesomesilica,aswellas
partoftheAlandothercations,togetherwithbicarbonate.
BecausethepHrisesduringreduction,thealuminiumstillpresentis
partlyneutralized,andpolymerizes intoringstructuressuchasAl^(OH)^. 3+

Theseformincompleteoctahedralsheetsintheinterlayerspacesofswelling
clayminerals.Suchaluminium interlayersarenotexchangeable;they
neutralizepartofthececandblockother,originallyexchangeablecationsin
inaccessiblecavitiesoftheincompletelayerstructure.
Ferrolysisthusgivesrisetoaluminium-interlayeredmaterialswithlow
cec, formed fromswellingclaymineralswithoriginallyhighcec,andalsoto
amorphoussilica-thelatterincontrast tohydrolysisbywatercontaining
carbondioxide.Therateofclaytransformationbyferrolyisisprobablyan
orderofmagnitudehigherthanthatofhydrolysisbywaterwithCO-,

Claytransformationunderalkalineconditions
Whereconcentrationsofsilicaandstructuralcationsarerelatively
 -13-

high,mineralsynthesisratherthandissolutioncantakeplace,aprocessalso
referredtoas"reverseweathering".
InalkalineorneutralconditionswithmoderateMgconcentrationsin
solution,montmorillonite isstableoverotherclaymineralssuchaskaolinite
orvermiculite.Montmorillonite isinfactformedinplainsorvalleysin
humidtosemiarid tropicalclimates,insofarastheinflowofmagnesiumand
silicafromadjoininguplandsissufficient.
WhereMgconcentrationsarehigh,asinsomesemiaridandarid
environments,afibrousmineral:palygorskiteisformed.Thiscontainsa
higherproportionofMgthanmontmorillonite.
InstronglyalkalineconditionswithhighNaconcentrationsinsolution,
analcimeisformed,generallyinaclay fractiondominated bymontmorillonite.
BecausetheNainstructureofthismineralistosomeextentexchangeable,
anomalouslyhighexchangeablesodiumpercentagescanbemeasured insuch
soils.

CLAYMINERALOGYANDLANDSCAPEPOSITION

Indifferentclimatezones,differentclaytransformationprocessestend
todominate:desilicationinperhumidclimates,reverseweathering inarid
conditions,orferrolysisonlevelsitesinclimateswithastrongseasonal
alternationbetweenthesetwo.Inmanyclimates,however,soilsoncrestsor
slopesmayhaveaverydifferentclaymineralogy fromthevalleysorplains-
notbecauseofdifferentparentmaterialsbutbecausethesoilhydrologygives
rise'todifferentclaytransformationprocessesoveroftenshortdistances.
Therelationshipsbetweenlandform,hydrology,soilformingprocessesand
claymineralogyofwetlandricesoilsaresummarizedbyMoormannandvan
Breemen(19/8).Someexamples,partextendingintodryland,arediscussed
below.

Kaoliniteandsmectite
Redorbrownkaoliniticsoilsonuplandslopesalternatewithblack
smectiteclaysoilsinvalleysorplainsoverextensiveareasinhumidto
semiaridAfricaandAsia.Theuplandsoils,formedbyhydrolysisbywater
containingcarbondioxide,arestronglytoweaklyacid,withlowormoderate
basesaturation,andhaveaclayfractionwithmainlykaolinite,oftensome
illite,andiron(III)oxides,quartzandfeldspar.Thececoftheclay
 -14-

fractionisuniformly low.Thevalley soilswereformedbyclaytransformation

underneutraloralkalineconditions,withsilicaandbasiccationsleached
fromtheuplands.Thesurfacehorizonsofthesesoilsmayhaveaclayfraction
containing smectite,withkaoliniteandillitetransported fromtheuplands,
andthewithdeeperhorizonshavemainly smectite.Thesmectiticvalleysoils
aregenerallybasesaturated,tend tohaveapHaboutneutralandhaveahigh
cec.
Anearlyexampleofsuchasoilassociationinamountainlandscapeon
Javawasdescribed byMohr(1944,p.168,162);ananalyzedexamplefromWest
AfricaistheShepeteritoposequenceinGreenland (ed),1981;management
aspectsoftheAlfisolsontheuplandsand theVertisolsinthevalleysofthe
Deccanplateauhavebeenstudied,e.b.,byKrantzetal(1977).

Aluminium-interlayered andinterstratifiedminerals
Whereslopesaremoregentlesothatsoilsonthelowerpartsofthe
slopesbecomeperiodicallywater-saturated,Planosols(Albaqualfs),orless
extremesurface-watergleysoils,maybefoundbetweentheuplandandvalley
soils.
Suchsoilsmayhavealuminium-interlayered materialintheclayfraction,
orinterstratifiedminerals:thesehavethesamegeneralstructureassmectite
butshowincompleteswellingbecauseofaluminium interlayeringofpartofthe
material.Theseperiodicallywetsoils,whicharesubjecttoleachingrather
thanaccumulationasinthevalleys,havelowclaycontentsandalowcecof
theclayfractionintheupperhorizons;theyaregenerallymoreacid thanthe
welldrainedsoilsonsteeperorhigherpartsofthelandscape.Ferrolysis
presumablyisthemainprocessthathasformedtheseasonallywetsoilsonthe
gentleslopesandlowrises,betweenhydrolysisontheuplandsandclay
formationunderneutraloralkalineconditionsinthevalleysofdepressions.
TwosuchtoptsequenceshavebeenstudiedbyBocquier (1973).One,
illustrated inFig.1,extendsfromgraniticuplandthroughagentleslope
intoanearly levelplain.Theothertoposequenceappearstobevirtually
flat,butinfacthaselevationdifferencesupto1mandslopesupto1per
cent.Eventhesehavebeenenoughtocausemajorsoilandclaymineral
differencesasdescribedabove.
Instillflatterlandscapes,forexampleintheolderriverplainsand
lowterracelandformsofBangladesh(Brinkman,1977),seasonallywetsoils
withlowclaycontentsinsurfacehorizonsandwithaluminium-interlayered
 -15-

clayfractionscovermostofthelandscape,whileperenniallywet,heavyclay
soilswithoutevidenceofclaydestruction,occurinthedepressions.

Amorphousclayminerals
Inareaswithrecentvolcanicactivity,particularly ontuff,soil
formationisrapidbecauseofthelargeproportionofeasilyweatherable
materialinthesoils.Initially,thesesupporthighsilicaandbasiccation
concentrationsevenduringratherintensiveleaching,andifthepHishighas
well,smectiteisformed.Highrunoffonsteepslopesmaydecreasethe
leachingrate,sothatthisstageisextended.Allophaneisformedrapidly
fromdissolved silicaandpolymericoctahedralAlcompounds,presumablyata
somewhat lowerpHandlowerbasiccationconcentrations thanmontmorillonite.
Afterremovalofmostofthebasiccationsandreadilydissolved silicaby
continued leaching,theirconcentrations inthesoilsolutionbecome solow
thatkaoliniteorhalloysiteisstableovermontmorillonite.Amorphous
aluminosilicatestendtocrystallizeand form imogolite,thenhalloysite,
eventuallykaolinite,withtimeaidedbyperiodicdryingout.

Inawelldrained toposequenceonbasicvolcanicrocksinaperhumid
climate,fromnearthedratero£QuoinHill,Sabah,tothebottomofthe
slope,Eswaranand Sys(1976aand b)showedatrendfrommajorproportionsof
allophaneorrelatedamorphousmaterialintheclayfractiononthesteep
upperslope,graduallydecreasing tozerointheoldest soilsonamoregentle
slopedownhill.Smectitedecreasedfrommajorontheupperslopetonearzero
onthemid-slope;kaoliniteandhalloysiteincreaseddownhillfromminor
proportionstodominant intheoldestsoils.

Avariant ofthistoposequence canbefound fromMountMakiling toLos

Banos,Philippines.ThehighestpartoftheslopehastypicalAndisols,with
probablymainlyamorphousmaterials intheclayfraction.Alahar(aformer
mudflow)ofthesameoriginconstituting theupperpartoftheIRRIfarmhas
soilssimilartothemid-slope soilatQuoinHill,buttheadjacent plainin
whichthelowerpartoftheIRRIfarmislocated,whichcontainsmaterialsof
thesameorigin,has imperfectlydrained swellingclaysoils-presumably the
result ofclaytransformationunderhighconcentrationsofsilicaandbasic
cationsinthedrainagewaterfromtheadjacentupland.
 -16-

SURFACEVERSUSBULKCOMPOSITIONOFCLAYFRACTIONS

Themineralogicalcompositionofclayfractiongenerally istheresultof
long-terraprocessesanddoesnotchangequicklywithachangein
circumstances.However,thesurfacepropertiesofaparticle in-theclay
fractionarenotnecessarily inequilibriumwithitsbulkcomposition.Surface
propertiesaremodifiedrelativelyquicklywhenexternalcircumstanceschange,
andsurfaceratherthanbulkpropertiesaregenerallyofprimary importance
forphysicalchemistry:forthefertility,toxicity,andothermanagement
aspectsofsoils.Herbillon(1981),e.g.,hassummarized thenatureand
propertiesofclayandoxidesurfaces.

Ironoxides
Soilswithkaoliniticclayfractionscontaininglessthanabout12
percentFe^O^generallyhavethepropertiesassociatedwithkaolinite:low,
pH-dependent cec,lowstructurestability,consequenterodibilityandtendency
tobecomedensewhenmechanicallydisturbed bytrafficorrainimpact,
moderatephosphatebufferingcapacityandfixation.
Inkaolinitic soilswithcontentsoffreeironoxidesexceeding12
percentoftheclayfraction,theclay tendstohaveanoxidesurface.Such
soilsthenhaveverylowcec,highstructurestabilityandgenerallysevere
phosphatefixation.Thepercentagequoted isvariable,however,dependingon
thenatureanddistribution oftheoxides.

Insmectitesoils,too,thereisamajordistinctioninstructure
stabilityandinthedegreetowhichagranularorfineblockysurface
structurecanberestoredbydrying.TheChromicVertisols,withrelatively
highcontentsoffreeironoxides,havefavourablepropertiesinthisregard,
whilethePellicVertisolsdonot.Theremaybeothercausativefactorsas
wellbesidesthecontentanddistributionofironoxides.

Othersubstancesorbondingagents
Structuralstabilityinsomesoilsmaybeduetoothersurfacefeatures
oftheclayfractionbesidesorganicmatter,oxidicsurfacesorpolyvalent
exchangeablecations.Besidesfinelydispersed ironoxides,features
identified byButleretal(1976)inAustralia includethepresenceofafine
clayfractionstrongly bondedorcemented intosilt-sizedaggregates,probably
 -17-

mainlyatedgesofclaypacketsratherthanonplanarfaces.Silica
cementationispossiblebuthasnotbeenprovedinthesesoils.Intergrowthof
claymineralcrystalsmayalsobeafactor,aswellasthelargeelectrostatic
interactionbetweenclaylayerswithahighchargedensity.
Kaolinitecorrosionandsubsequentcementationhasalsobeensuggestedas
acauseforanomalouslyhighstructuralstabilityincertainOxisols Coughla.i
etal,1973andHerbillonetal, 1966).

TnclayfractionsofKenyansoilswithamorphousmaterialWielemaker
(1984)foundindicationsthatthececatagivenpHishigherwithevenminor
increasesintheratioofextractableamorphousSitoAlandSitoFe.Healso
modified thechargecharacteristicsexperimentallywithapplicationsof
amorphoussilica.Similaramorphoussilica-ironcompoundswithsomealuminium
coverthesurfacesofcrystallineclaymineralsinclaysoilsoverlargeareas
inQuebecandOntario,Canada.Thesesoilareverystiffinplace,butmay
becomevirtuallyliquidwhenextensivelysheared (McKyesetal, 1974),even
thoughthecontentofamorphousmaterialisonly 10-12percent.

Rapidchangesinsurfaceproperties
Themostrapidchangesinsurfacepropertiesandphysicalchemistryof
soilsarebroughtaboutbyalternatingreductionandoxidation.Theprocesses
occurringduringsoilreductionhavebeenextensivelydealtwithby
Ponnamperuma (1972).
Duringreduction,iron(III)oxidesareconvertedintosolubleand
2+
exchangeableFe ,withaconcurrent riseinpH.Inneutralsoilswith
smectiteorverraiculiteintheclayfraction,thismaygiverisetosynthesis
ofmaterialswithastructuresimilartosmectiteandcontainingFe(II)inthe
octahedralsheet.Wheresuchsoilsremainperenniallywet,zinctendstobe
fixedinaformunavailable towetlandrice:Isuspectbecauseitcanbebuilt
intotheoctahedralpositionsofthesynthesizedmaterial.Uponreoxidation,
thezincbecomesavailableagain,whichsuggeststhatthematerialisonly
stableinreducedconditions-presumablybecauseofitshighFe(II)content.
Inacidsoils,particularly thosewithakaoliniticclaymineralogy,
solubleFe 2+
concentrationstendtorisetohighlevelsbecauseofthelowcec
andbecauseconditionsareunfavourableforprecipitationofiron(II)oxides
orcarbonatesorsynthesisofsilicates.Then,theirontoxicitysyndromemay
2+
beobserved inwetlandrice,dependingontheFe concentrationinrelation
 -18-

totheconcentrationsofnutrientcationsandphosphateavailability.
2+ into
Whenareduced soilisoxidizedagain,theFe isconverted
Fe(OH)3.Theoriginalironoxidesarethusdistributed inadifferentway,and
withagenerallyhigherspecificsurfaceandactivity.Inhigh-activityclay
soils,thismayincreasethestabilityofastructureestablishedbefore
inundation,asinfloodfallowingofsugarcanelandintheGuyanacoastal
plain,orofastructureestablished justbeforeoxidation,asinland
preparationforwheatafterriceintheJangtzedelta,China.Inlow-activity
claysoils,theeffectsofalternate reductionandoxidationarelessclearly
beneficial,inpartbecausetheremovalbyleachingofnutrientcationstends
tobeaccelerated inperiodically reducedconditions.

Insoilswithhighamountsofactiveironoraluminium,forexamplewith
amorphous,halloysiticoroxidicclay fractions,phosphatefixationissevere
andcecmaybeloworvery low.Phosphateorsilicaonthesurfaceofsuch
materialsdrasticallychangestheirproperties.Althoughveryhighphosphate
applicationstodecreaseoreliminatephosphatefixationmaynotbeexonomic
inmostcases,theyareeffectiveand rapid.Theuseofsilicaorfinely
groundsilicatesmaybemoreeconomic.This,too,tendstolowertheamount
andseverityofphosphatefixationandraisesthececatagivenpH.
Substancesthatcouldbetriedincludewollastonite(Casilicate),usedasa
silicafertilizerinsomewetland riceareas,orground feldspar,orbasic
slag,containingphosphateandsilicate.
Inpractice,CasilicateapplicationsonaGibbsihumoxinHawaiigave
disappointing results,butthehighPfixingcapacity inOxisolswasreduced
bylong-term irrigationwithwatercontaining 30mgSiperliter(Fox,19S0).
Thisresulted inatriplingofwater-solubleSifrom 1.6to5.3mg/1,increase
inpoorlycrystallinesoilSifrom730to1360mg/kg,andadropinPsorption
(at0.2mg/1solutionconcentration)from235to100mg/kg,allcomparedwith
thesoilthatreceived low-Siirrigationwater.
ExperimentsbyJepsonetal(1976)indicatethatsilicareactswitha
gibbsite(AKOH)^)surfaceinquantities fromlessthanamonolayeratpH4to
morethanthatatpH9,withanincreaseincationexchangecapacityand
decreasesinanionexchangecapacityandAlsolubilityatagivenpH.
Thesedifferentfindingscanprobably besummarized intheestimatethat
silicationofoxidicsurfacesisfeasible,butthattheprocessworksmuch
moreslowly insoilsthaninlaboratory situationsbecauseofimperfectmixing
 -19-

andslowdiffusionofsilicatotheoxidicsurfaces-probablyoverseveral
cropseasons.
 -20-

1
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 -24-

Table 1.Somechemicalandphysicalpropertiesofsoilswithclayfractions
dominated bydifferentmaterials.

Properties

Dominant cec Kor phosphate swell- physical

materialin NH, fixation shrink stability
clayfraction fixation ratio
oronsurface

vermiculite v.high high mod. mod.

beidellite high high high mod.

montmorillonite, high high mod.

nontronite

illite mod. low mod. mod.

kaolinite, low* high low

halloysite

allophane, v.high* v.high mod./ mod.**

imogolite low

Fe,Aloxides v.low* high/ high

andhydroxides v.high

Al-interlayered low* high mod./- mod.

clays

* pH-dependent
-notsignificant
**highagainstrainfallorwatererosion;allophanesoilslowunderload