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ContentslistsavailableatScienceDirect

Computational

Biology

and

Chemistry

j ou rn a l h o m epa ge :w w w . e l s e v i e r . c o m / l o c a t e / c o m p b i o l c h e m

Research

Article

Development

of

a

sugar-binding

residue

prediction

system

from

protein

sequences

using

support

vector

machine

Masaki

Banno

a

,

Yusuke

Komiyama

b

,

Wei

Cao

a

,

Yuya

Oku

a

,

Kokoro

Ueki

a

,

Kazuya

Sumikoshi

a

,

Shugo

Nakamura

a

,

Tohru

Terada

a

,

Kentaro

Shimizu

a,∗

aGraduateSchoolofAgriculturalandLifeSciences,TheUniversityofTokyo,1-1-1Yayoi,Bunkyo-Ward,Tokyo113-8657,Japan

bDigitalContentandMediaSciencesResearchDivision,NationalInstituteofInformatics,2-1-2Hitotsubashi,Chiyoda-Ward,Tokyo101-8430,Japan

a

r

t

i

c

l

e

i

n

f

o

Articlehistory:

Received8March2016

Receivedinrevisedform5October2016 Accepted23October2016

Availableonline9November2016

Keywords:

Supportvectormachine Sugar-bindingproteins Sugar-bindingresidueprediction Carbohydrate

Machinelearning

a

b

s

t

r

a

c

t

Severalmethodshavebeenproposedforprotein–sugarbindingsitepredictionusingmachinelearning algorithms.However,theyarenoteffectivetolearnvariouspropertiesofbindingsiteresiduescaused byvariousinteractionsbetweenproteinsandsugars.Inthisstudy,weclassifiedsugarsintoacidicand nonacidicsugarsandshowedthattheirbindingsiteshavedifferentaminoacidoccurrencefrequencies.By usingthisresult,wedevelopedsugar-bindingresiduepredictorsdedicatedtothetwoclassesofsugars:an acidsugarbindingpredictorandanonacidicsugarbindingpredictor.Wealsodevelopedacombination predictorwhichcombinestheresultsofthetwopredictors.Weshowedthatwhenasugarisknown tobeanacidicsugar,theacidicsugarbindingpredictorachievesthebestperformance,andshowed thatwhenasugarisknowntobeanonacidicsugarorisnotknowntobeeitherofthetwoclasses,the combinationpredictorachievesthebestperformance.Ourmethodusesonlyaminoacidsequencesfor prediction.Supportvectormachinewasusedasamachinelearningalgorithmandtheposition-specific scoringmatrixcreatedbytheposition-specificiterativebasiclocalalignmentsearchtoolwasusedas thefeaturevector.Weevaluatedtheperformanceofthepredictorsusingfive-foldcross-validation.We havelaunchedoursystem,asanopensourcefreewaretoolontheGitHubrepository(https://doi.org/10. 5281/zenodo.61513).

©2016TheAuthors.PublishedbyElsevierLtd.ThisisanopenaccessarticleundertheCCBY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction

Interactionsbetweensugarchainsandproteinsplayessential rolesinbiologicalprocessessuchasintercellularcommunication, immunity,and cellularrecognition.The methodstoempirically analyzesuchinteractionsincludehemagglutinationassays,which areemployedin thediscoveryof novellectins.In recent years, methods utilizing glycan arrays have been developed as high-throughputsolutions,enablingresearcherstoobtaindataoninvitro

interactionsbetweenmultiplesugarchainsand proteins(Porter etal.,2010;Blixtetal.,2004;Gabiusetal.,2011).Nevertheless,the bioinformatics-basedpredictionapproachescanfurtherreducethe timeandeffortinvolvedinpredictingsuchinteractions,providing valuablecluesforexperimentalwork.Conventionalmethodsare usefulin determiningprotein–sugarchaininteractions or iden-tifyingsugarchainrecognitionsequences.However,theycannot

∗Correspondingauthor.

E-mailaddress:[email protected](K.Shimizu).

provideinformation onthebindingresiduesin proteins. Meth-odssuchasX-raycrystallographyandnuclearmagneticresonance haveprimarilybeenusedtoidentifythesebindingresidues. How-ever,suchtechniquesposenumerouschallengesbecausetheyare generallycost-andlabor-intensive,Moreover,thehighmotilityof sugarchainsrendersthedeterminationoftheirtertiarystructures difficult(DeMarcoandWoods,2008).Aspartialsolutionstosuch challenges,bioinformatics-basedtechniqueshavebeenattracting attention.

Dockingsimulationisa predictionmethodforsugar-binding residues based on their tertiary structures. To implement this method, many protein–ligand docking programs (Morris et al., 2009;Jonesetal.,1995,1997;Biesiadaetal.,2011;Forlietal.,2016; Grinteretal.,2014)andmolecularsimulationsareoftenemployed. In a previousstudyinvolvingsugar chain-bindingresidues,the heparin-binding residueshavebeen predictedinan interleukin onthebasisofitsproteinstructure(DeMarcoandWoods,2008). Thecandidateresidueswerenarroweddownviarepeateddocking withheparinmonosaccharidesanddisaccharides.Then,the hep-arinhexasaccharidesweredockedtotheremainingcandidatesto http://dx.doi.org/10.1016/j.compbiolchem.2016.10.009

1476-9271/©2016TheAuthors.PublishedbyElsevierLtd.ThisisanopenaccessarticleundertheCCBY-NC-NDlicense(http://creativecommons.org/licenses/by-nc-nd/4. 0/).

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predicttheheparin-bindingresiduesintheinterleukin. Another study has used machine learning to predict glucose-binding residues fromtertiary structure of proteins. It has employed a learning model with a support vector machine (SVM), which usedthe occurrencerates of atomsappearing in theproximity ofglucose-bindingresiduesasthefeaturevalues(McDonaldand Thornton,1994).Tsaietal.(2012)developedasugar-bindingsite predictionmethodbasedonthree-dimensionalprobabilitydensity maps,representingthedistributionsof36non-covalent interact-ingatomtypesaroundproteinsurfaces.Themethodreportedby Zhaoetal.(2014)usesastructuralalignmentprogram,SPalignand bindingaffinityscores,accordingtoaknowledge-basedpotential. Allofthesemethodsrelyonthetertiarystructureofthetarget proteinforthepredictionofthebindingresidues,thusrequiringthe determinationoftheproteinstructure.Theaminoacidsequenceof aproteinismucheasiertoobtainthanitstertiarystructure.Thus,it ispreferableforthehigh-throughputexperimentssuchas genome-wideandglycanarraysanalyses.

Some attempts have been made to build software applica-tionscapableof learningsuchfeaturessothat theycanpredict sugar-binding residues only from amino acid sequences. Malik etal.havedevelopedamachinelearning-basedmethodusing neu-ralnetworks.Theyhaveconstructedapredictionprogramusing theposition-specificscoringmatrices(PSSMs) derivedfromthe residue frequencyand multiplealignments of40 sugar-binding proteinsand18galactose-bindingproteinsasthefeaturevalues. Theperformanceoftheprogramhasbeenevaluatedby leave-one-outcross-validation(CV)(MalikandAhmad,2007).Theirresults showthatthepredictionprogramperformsmoreeffectivelywhen appliedtoadatasetofgalactose-bindingproteinsthanthatwhen learningusingtoallsugar-bindingproteins.Nassifetal.(2009)also developedaglucose-bindingsitepredictionmethod.Thismethod usesspatialfeaturesofbindingpocketsandaminoacidand chem-icalfeaturessuchascharge,polarity,mobility,andhydrophobicity asdeterminantfeaturesof abindingsite. Recently,a mannose-bindingsitepredictionprogramhasbeendeveloped;itusesthe compositionprofileofpatternsassequencefeatures(Agarwaletal., 2011).

Inthispresentstudy,weattemptedahigh-performance pre-dictionbygroupingthesugar-bindingproteinsdependingonthe characteristicsoftheirbindingresiduesanddesigningapredictor dedicatedtoeachgroup.Weanalyzedthecharacteristicsofthe bindingresiduesbyclusteringthesugarsaccordingtotheresidue compositionatthebindingsites,andtherebyclassifiedthe sug-arsintodifferentclasses.Individualpredictorsforeachsugarclass madethelearningofthepropensitiesofthebindingresiduesmore effective. This,in turn, resulted in improvedprediction perfor-manceofthepredictor.Furthermore,ourmethodusesonlythe aminoacidsequencesforprediction.SVMwasemployedbecause itisoneoftherepresentativetechniquesfortheclassificationof thedataintotwocategorieswithhighgeneralizationability.SVM takesasinputPSSMsaroundatargetresidueasfeaturevalues.It canimprovethepredictioncapabilityfurtherbyextensive incor-porationofthenatureofhomologousproteinscoupledwithsugar class-specificlearning.

2. Materialsandmethods

2.1. Searchforsugar-bindingproteinsintheproteindatabank database

Wetargetedthesugarsthatfrequentlyoccurinvivo,namely aldosesandketoses,andtheirderivativesinwhichthehydroxy group is oxidized or substitutedwith a methyl group,sulfonic group,phosphategroup,acetylgroup,aminegroup,oracetylamide group.Fig.1illustratestheprocedureforconstructingthedataset usedforprediction.

Withsugar-bindingresiduesdefinedastheresidueswithin4 ˚A ofthesugarmolecule.Weperformedanexhaustivesearchof pro-teindatabank(PDB)forproteinswithatleastonesugar-binding residues.Thisstudyfocusedonnoncovalentinteractionsbetween sugarsandproteinsandnotonglycosylationsitesatwhichsugars arecovalentlybondedwithproteins.Therefore,theresidueswithin the1.5 ˚Adistancefromasugarmolecule,aswellastheresidues adjacenttoacovalentlybonded sugarmolecule, wereexcluded fromthesearch.

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Sugarsareoftencovalentlyattachednotonlytoproteinsbut alsotoothertypesofcompounds.AlthoughPDBcontainsdataon variousglycolipidsformedbybindingbetweensugarsandlipids, thesewerealsoexcluded.Herelipidsweredefinedascompounds registeredintheLipidMaps(Sudetal.,2007),adatabaseoflipid substances. Furthermore,saccharides that are used as cryopro-tectants,surfactants,andadditivestofacilitatecrystallization(Shi etal.,1997)wereexcludedbecausetheydonotengageininvivo

interactionswithsugars.

2.2. Clusteringofsugar-bindingresidues

Thebasicapproachofourstudywastoimprovetheprediction accuracybyclassifyingthesugarsintogroupsanddesigningthe predictorsdedicated toeachgroup.To obtainaneffective clas-sification,wefirstperformedclusteranalysisonthebasisofthe occurrencefrequencyofresiduesatthesugar-bindingsites.Inthe PDBdatabase,wetargetedsugarsboundtotheproteinswith100 ormoreresidues.Thegroupaveragemethodwasemployedasthe clusteringprocedure.

2.3. Eliminationofredundancy

Toreducetheredundancyofthesequences,theproteinswith asequencesimilarityof30%oraboveintherangeexceeding50% alignmentcoveragewerealsoexcludedusingBLASTClust(Altschul etal.,1997).Asaresultofthisprocess,369sugar-bindingproteins, 136acidicsugar-bindingproteins,and270nonacidicsugar-binding proteinswereselected.(37proteinshadbothacidicandnonacidic sugar-bindingresidues).

2.4. Predictionmethodforinteractingresidues

Onthebasisoftheproteinsequenceinformation,weperformed asearchonhomologoussequencesusingtheposition-specific iter-ativebasiclocalalignmentsearchtool(PSI-BLAST)(Altschuletal., 1997)inthenonredundantdatabaseofNCBI,therebycollecting homologoussequences.InthisPSI-BLASTsearch,numberof itera-tionswastwo,andtheE-valuethresholdofsequenceselectionfor profilecreationwas0.001.

Wedevelopedasystempredictingthesugar-bindingresidues ofproteinsonthebasisoftheiraminoacidsequences,using sup-portvector machine(SVM)(Cortesand Vapnik, 1995).An SVM learnsapredictivemodelfromthetrainingdatausingtheprinciple ofmarginmaximization.Itowesitshighgeneralization capabil-itytothislearningapproach.Topredicttheinteractingresidues,a PSSMofsugar-bindingsitesandtheirsequence-neighborresidues isconstructedbasedonthemultiplealignmentofthesugar-binding proteins.Weextractedwconsecutivecolumnvectors (correspond-ingtowconsecutiveresiduesinsequences)fromPSSMandused themas(20×w)-dimensionalfeaturevectorsinSVM.Usingthese featurevalues,SVMpredictedwhetherthecentralresidueswere thesugar-bindingresidues.Thevalueofwisdeterminedbythe parameteroptimizationproceduredescribedinSection2.5.

SVM wasgiven thedata of the sugar-binding residues as a positivedatasetfromTableS1forlearning.Weusedthedataofall theresiduesthatwere5–25residuesawayfromthesugar-binding sitesintheproteinsasanegativedatasetratherthanrandomly selectedproteinresidues.Thereweretworeasonsforusingthis negative dataset. One was to discriminate between the sugar-binding residues from nonsugar-binding residues in a protein. Theotherreasonwasthat,sincetheadjacentresiduestendedto havesomewhat similarfeaturevalues, giving residuesadjacent to binding residues as the negative examples might teach the machinetoimposepenaltiesonthefeaturevaluesresemblingthe

positiveexamples.Fortheevaluationofthepredictorperformance, allresiduesintheproteinsequenceswereusedasthetestset.

We constructed three types of predictors using three types oftrainingdatasets,asugar-binding residuepredictorusingthe sugar-binding proteins, a acidic sugar-binding residue predic-tor using the acidic sugar-binding proteins, and a nonacidic sugar-bindingresiduepredictorusingthenonacidicsugar-binding proteins.Besides,weconstructedacombinationpredictorby com-biningtheacidicandnonacidicsugar-bindingresiduepredictors. WhiletheSVM-basedpredictoroutputsdecisionvaluesas discrim-inantfunctionvalues,thecombinationpredictoriscomposedof thelinearcombinationofdiscriminantfunctionsoutputbythetwo predictiondevices.Weconstructednewpredictorsusingthelinear combinationofpredictiondevicesforacidicandnonacidicsugars asexpressedinthefollowingequation:

fnew (x)=p×facid (x)+q×fnonacid (x) (1)

For each data x, facid (x) and fnonacid (x) represent a

discrimi-nantfunctionoftheacidicandnonacidicsugar-bindingpredictors, respectively. A new discriminant function fnew was defined by

weighingthesefunctionswiththeparameterspandq.The dis-criminantfunctionfisdefinedas

f(x)=sgn

l

i=1 ˛iyiK(xi,x)+b

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suchthatyi=f(xi)givenNdatasamplesandlisthenumberof

train-ingrecords,yi∈{−1,+1}isthelabelassociatedwiththetraining

data,bisaconstant,xiisthesupportvectors,andKisthekernel

functionusedtotransformthedatapoints.

2.5. Evaluationmethod

To ensurean unbiasedparameter selection, we employed a nestedCVmethod.ThenestedCVcanguaranteeunbiased evalu-ationofgeneralizationcapabilitiesbyselectingmodelparameters inacross-validatingmanner.InthenestedCV,thedatasetwasfirst dividedintoksubsets,withoneusedasthetestsetandthe oth-ersasthetrainingset,asisthecasewithCV.Inthistrainingset, theparametersweredeterminedsothatthepredictorperformance tobeevaluatedbyCVwouldbemaximized.Thus,we obtained theoptimalvalues oftheparameters basedonthegridsearch:

w=5,C=−3and=−10.(Candareparametersforanonlinear SVMwithaGaussianradialbasisfunctionkernel.)Forthe param-etersofthediscriminantfunctioninEq.(1),wefixedthevalueof parameterpas1andobtainedtheoptimalvalue0.96of param-eterqbasedonthegridsearch.Usingtheselectedparameters,we constructedthepredictorsthroughthelearningoftheentire train-ingset.Thecompletedmodelwasthensubjectedtoperformance evaluationonthebasisofthepredictionofthetestset.This proce-durewasrepeateduntilallsubsetswereusedastestsets,andthe resultswereaveragedtoevaluatethepredictorperformance. 3. Results

3.1. Characteristicsoftheinteractingsites

3.1.1. Clusteringofsugarsaccordingtothecompositionofthe residuesinthebindingsites

Fig.2Aportraysatreediagramshowingtheresultsof hierar-chicalclustering.Thesugarswereroughlydividedintotwogroups: withandwithouttheacidicfunctionalgroup.

Althoughthesugarswithanacidicfunctionalgrouphave var-ious functions,their common feature is a basic residue at the binding site. Sialic acid, for example, is a generic termfor the

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Fig.2.Hierarchicalclusteringbyresidueoccurrencefrequencyofsugar-bindingresidues.(A)Hierarchicalclusteringbasedonthegroupaveragemethod.(B)Examplesof acidicsugars.(C)Examplesofnonacidicsugars.

neuraminicacid(i.e.,monosaccharideformedbyaldose condensa-tionofpyruvicacidandd-mannosamine)derivativeswithamino

or hydroxyl substituents. The sialic acids play important roles incellularrecognition.Theproteinsthatbindsialicacidinclude sialicacid-bindingimmunoglobulin-typelectins(Siglecs),a sub-setoftheI-typelectins.Arginineisacrucialfortherecognition ofsialicacidbySiglecs(Crockeretal.,2007).Glycosaminoglycans arepolysaccharidechainsconsistingof disaccharideunitsofan uronicacid(monosaccharidewithacarboxylgroup)andanamino sugar(monosaccharidewithanaminogroup),andmanysulfuric acidmoleculesarecovalentlyattachedtotheirhydroxylgroupsvia esterbonds.Thesurfaceofaglycosaminoglycanhasastrong neg-ativecharge,andarginine,lysine,andoccasionallyhistidineform ionicbondsatthebindingresidues(GandhiandMancera,2008). Incontrast,theCH/interactionsbetweentheCHgroupand aro-maticringarecrucialincommoninteractionsbetweensugarsand proteins(Gabiusetal.,2011).

Thesaccharidesweredividedintotwoclassesdependingonthe primarymodeoftheirinteractionswithaligand,thatis,ionic inter-actionornonionicinteraction.Thispropertywasreflectedbythe differencesinaminoacidcontentofthebindingproteins.Takethis intoaccount,weconstructedtheindividualbindingresidue pre-dictorsforsugarswithandwithoutanacidicfunctionalgroupand analyzedthedifferencesintheirproperties.Fig.2BandCshow someexamplesoftheclassifiedmonosaccharides,Andalso,Table1 describesthedetailedinformationof40sugarsinFig.2.

3.1.2. Residueoccurrencefrequencyofsugar-bindingsites

Wecalculatedtheoccurrenceprobabilityforeachtypeofamino acidinsugar-bindingsitesandinthewholesequencesofthe sugar-bindingproteins(Fig.3).

Fig. 3A shows the base-2 logarithm of the odds ratios of sugar-bindingresiduestoalltheproteinresiduescalculatedfor allthesugar-bindingproteins,acidicsugar-bindingproteins,and nonacidicsugar-bindingproteins.

Ineverycluster,polararomaticaminoacidssuchastryptophan, tyrosine,andhistidineaswellasarginineplayedimportantroles.In theacidicsugarcluster,argininehadaparticularlyhighoddsratio, andpolarresiduessuchaslysine,glycine,andserinedisplayed com-parativelyhigherratiosthanthatinthenonacidicsugarcluster.In contrast,theoddsratiooftryptophanwasparticularlyhighinthe nonacidicsugarcluster,andtheoddsratiosofpolarresidueswith anamide,suchasglutamineandasparagine,werehigherthanin theacidicsugarcluster.

It is well established that sugar affects a CH/ interaction withanaromaticringwhilebindingtoaprotein.Thisprobably explainswhythearomaticresiduesaccountedforalarge propor-tionofaminoacidsinthebindingsites.Whileacidicsugarsinteract stronglywithbasicresiduessuchasarginineandlysine,their inter-actionwithacidicresiduessuchasasparagineandglutamineare weaker.

Fig. 3B presents the base-2 logarithm of the odds ratiosof sugar-bindingresiduestotheproteinsurfaceresiduescalculated

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Fig.3. Logoddsratiosofoccurrenceofsugarchain-bindingresidues,theaminoacidsarelistedinorderfromthelowestKyte–Doolittlehydropathyindexscore.Subfigure (C)representstheoccurrenceratiosofresiduesthatformedahydrogenbondwiththeproteinsidechain.Theoccurrenceratiosofresiduesthatformedahydrogenbond withthemainchainareplotted(main-chain)ontheright-handsside.(A)Logoddsratiosofsugarchain-bindingresiduesamongallaminoacidresidues.(B)Logoddsratios ofsugarchain-bindingresiduesamongthesurfaceresidues.(C)Logoddsratiosofsugarchain-bindingresiduesamonghydrogenbondacceptors.

forallthesugar-bindingproteins,acidicsugar-bindingproteins, andnonacidicsugar-bindingproteins.Incomparisonwiththecase ofallresidues,theproportionofhydrophobicresidueswashigh, whereastheoccurrenceratioofpolarresidueswaslow.This ten-dencywasparticularlyprominentforphenylalanineandcysteine inthenonacidiccluster.

Phenylalanineisa nonpolararomaticamino acid, andit can affectintoaCH/interactionwithsugar.Therelativescarcityof phenylalanineresidues exposed on thesurface suggeststhat a largeproportionofthesemoleculeswerefunctioningasbinding residues.

Cysteine stabilizes the protein folding by forming disulfide bonds. In OS-9 (PDB: 3AIH), a human-derived P-type lectin, the cysteine residues in the binding sites are strongly con-served among the proteins with the same domain. Although disulfidebondsarenot directlyinvolvedinsugar-binding, their formation might contribute to the establishment of binding domains (Satoh et al., 2010). Cysteine also forms coordinate bonds with metallic ligands. In the glucose 1-dehydrogenase (PDB: 2CDB), cysteine is involved in the catalytic reaction by forming a coordinate bond with a Zn2+ ion (Milburn et al., 2006).

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Table1

NamesofsugarsusedinclusteringanalysisinFig.2.

Ligandid Ligandname

BG6 Beta-d-Glucose-6-phosphate

PRP Alpha-phosphoribosylpyrophosphoricacid ADA Alpha-d-galactopyranuronicacid IDS 2-O-sulfo-alpha-l-idopyranuronicacid SGN N,O6-disulfo-glucosamine G1P Alpha-d-glucose-1-phosphate 16G N-acetyl-d-glucosamine-6-phosphate G6P Alpha-d-glucose-6-phosphate R1P Ribose-1-phosphate F6P Fructose-6-phosphate FBP Beta-fructose-1,6-diphosphate

GCU d-Glucuronicacid

SIA O-sialicacid

BDP Beta-d-glucopyranuronicacid KDO 3-Deoxy-d-manno-oct-2-ulosonicacid M6P Alpha-d-mannose-6-phosphate NAA N-acetyl-d-allosamine RAM Alpha-l-rhamnose ARA Alpha-l-arabinose NAG N-acetyl-d-glucosamine NDG 2-(Acetylamino)-2-deoxy-A-d-glucopyranose BMA Beta-d-mannose XYP Beta-d-xylopyranose XYS Xylopyranose AHR Alpha-l-arabinofuranose FUL Beta-l-fucose GCS d-Glucosamine SGC 4-Deoxy-4-thio-beta-d-glucopyranose GDL 2-Acetamido-2-deoxy-d-glucono-1,5-lactone RIP Ribose(pyranoseform)

A2G N-Acetyl-2-deoxy-2-amino-galactose MAN Alpha-d-mannose RIB Ribose FUC Alpha-l-fucose FRU Fructose GLC Alpha-d-glucose GLA Alphad-galactose NGA N-Acetyl-d-galactosamine BGC Beta-d-glucose

GAL Beta-d-galactose

Fig.3C shows the base-2logarithm of theodds ratio ofthe proteinsidechainsbeingthebindinglociofthehydrogenbond acceptorsforthesugar-bindingproteins,acidicsugar-binding pro-teins,andnonacidicsugar-bindingproteins.Asimilaranalysiswith hydrogenbondacceptorsrevealedthatthenumberwasverysmall, andallthehydrogenbondswereformedinthemainproteinchains. IncomparisonwithFig.3B,thedifferencebetweenthetwo clus-terswasnotable;serine,lysine,andarginineaccountedforlarger proportionsintheacidicsugarcluster,whereastryptophan, his-tidine,asparagine,andglutamineweremorepredominantinthe nonacidicsugarcluster.

Theseresultsindicatedthataminoacidssuchaslysine,arginine, andserineformhydrogenbondswithacidicsugars.Incontrast, hydrogenbondswithasparagine,glutamine,andpolararomatic residueswerelesslikelytooccurintheacidicsugar-binding pro-teinsthanintheproteinsbindingthenonacidicsugars.

3.2. Performanceofsugar-bindingresiduepredictors

Weevaluatedthreepredictors,thesugar-bindingresidue pre-dictor, acidic sugar-binding site predictor, and the nonacidic sugar-bindingsitepredictorwiththedividedtestingdatasetusing five-foldCV,andwhereintheparameterswereoptimizedtogive thebestpredictionperformanceforeachsugarcluster.

3.2.1. Performanceevaluationofsugar-bindingresiduepredictors

We evaluated the performance of each predictor using all residuesof sugar-binding proteins asthe test set.Table 2 lists

Table2

Performanceoffoursugar-bindingresiduepredictorsforsugar-bindingproteins.

SVMsugarpredictors Sens.a(%) Spec.b(%) AUC MCC

Allsugarsc 34.1 92.3 0.754 0.178 Acidicsugarsd 30.1 93.9 0.738 0.169 Nonacidicsugarse 38.5 90.4 0.749 0.169 Combinationsugarsf 31.6 94.1 0.760 0.185 aSensitivity. bSpecificity.

c Sugar-bindingresiduepredictor. dAcidicsugar-bindingresiduepredictor. eNonacidicsugar-bindingresiduepredictor. f Combinationpredictor.

Fig.4. Receiver–operatorcharacteristiccurvesoffoursugar-bindingresidue pre-dictorsforsugar-bindingproteins.(Forinterpretationofthereferencestocolorin thisfigurelegend,thereaderisreferredtothewebversionofthisarticle.)

the sugar-binding site prediction capabilities of each predictor model. Fig. 4 shows the receiver–operator characteristic (ROC) curvesdrawnonthebasisoftheevaluationresults.AnROCcurve is a graphical plot of thefalse positive rate (ratioof nonbind-ingresiduesfalselypredictedaspositive,hereafterreferredtoas FPR)on thex-axis, and thetrue positive rate(ratio of binding residuescorrectlypredictedaspositive,TPR) onthey-axis.The higherthecurveis,thebettertheevaluatedpredictoris.Inthis fig-ure,thecurvesforthecombination(green),nonacidicsugar(red), acidicsugar(blue),andallsugar(orange)showtheresultsforthe combinationpredictor,nonacidicsugar-bindingresiduepredictor, acidicsugarresiduepredictor,andsugar-bindingresiduepredictor, respectively.

As shown in Table 2, the combination model exhibited the largest values for both Matthew’scorrelation coefficient (MCC) scoreandareaundertheROCcurve(AUC).AUCiscalculatedby factoringintheentireROCcurve,andMCCisalocalindexof per-formancedeterminedwhenacertainthresholdisselected.Ascan beseeninFig.4,thismodelwasparticularlyeffectiveinthelow FPRrangeincomparisonwithalltheotherpredictormodels.Given thishighperformanceinthelowFPRrange,thecombinationmodel canberegardedasaneffectivemodelforthepredictionsof sugar-binding.

3.2.2. Performanceevaluationofacidicsugar-bindingresidue

prediction

Table3liststheacidicsugar-bindingresidueprediction capa-bilitiesofeachpredictormodel,andFig.5showstheROCcurves drawnonthebasisoftheevaluationresults.AsshowninTable3, sugar-bindingresiduepredictortrainedwiththedatasetofacidic

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Table3

Performanceof foursugar-bindingresiduepredictors foracidicsugar-binding proteins.

SVMsugarpredictor Sens.a(%) Spec.b(%) AUC MCC

Allsugarsc 30.0 95.1 0.783 0.200 Acidicsugarsd 39.4 93.5 0.787 0.221 Nonacidicsugarse 34.0 92.6 0.752 0.163 Combinationsugarsf 29.7 95.8 0.784 0.193 aSensitivity. b Specificity.

c Sugar-bindingresiduepredictor. d Acidicsugar-bindingresiduepredictor. eNonacidicsugar-bindingresiduepredictor. f Combinationpredictor.

Fig.5.Receiver–operatorcharacteristiccurvesoffoursugar-bindingresidue pre-dictorsforacidicsugar-bindingproteins.

Table4

Performanceoffoursugar-bindingresiduepredictorsfornonacidicsugar-binding proteins.

SVMsugarpredictor Sens.a(%) Spec.b(%) AUC MCC

Allsugarsc 30.0 95.1 0.783 0.200 Acidicsugarsd 39.4 93.5 0.787 0.221 Nonacidicsugarse 34.0 92.6 0.752 0.163 Combinationsugarsf 29.7 95.8 0.784 0.193 aSensitivity. b Specificity.

c Sugar-bindingresiduepredictor. d Acidicsugar-bindingresiduepredictor. eNonacidicsugar-bindingresiduepredictor. f Combinationpredictor.

sugar-bindingproteins(acidicsugardataset)exhibitedthelargest valuesof bothAUCand MCC. Inparticular,in comparisonwith thecombination modeland thesugar-binding model, a signifi-cantdifferencebetweenMCCvalueswasobserved,whereasthere wasnosubstantialdifferencebetweentheAUCs.Althoughthe per-formanceoftheacidicsugarpredictormodelwaslowerthanthe performanceofothermodelsinthehighFPRranges,itwashigher inthelowerFPRranges.OvertheentireROCrange,thisresultedina significantdifferencebetweenMCCsdespitethelackofsubstantial differencebetweenAUCsintheperformanceevaluation.

3.2.3. Performanceevaluationofnonacidicsugar-bindingresidue

prediction

Table 4 lists the nonacidic sugar-binding residue predic-tioncapabilities of each predictormodel, and Fig.6 shows the ROC curves drawn on the basis of the evaluation results. The

Fig.6.Receiver–operatorcharacteristiccurvesoffoursugar-bindingresidue pre-dictorsfornonacidicsugar-bindingproteins.

Table5

Summaryofsugar-bindingresiduepredictions.

Testdataset/bestpredictor Sens.a(%) Spec.b(%) AUC MCC

AllSBPsc/combination 31.6 94.1 0.760 0.185 AcidicSBPsc/acidic 39.4 93.5 0.787 0.221 NonacidicSBPsc/combination 28.7 95.1 0.752 0.178 aSensitivity. bSpecificity. c SBPs:sugar-bindingproteins.

combinationmodelexhibitedthelargestvaluesforbothAUCand MCC.AscanbeseeninFig.6,thismodelwasparticularlyeffective in theFPR range lower than 0.1 in comparison withtheother predictormodels.Intherangeabovethatvalue,thecombination modeland thenonacidic sugar-binding protein-basedpredictor modelwerealmostthemosteffective;thepredictortrainedwith theunclassifieddatasetwaslesseffective.

3.2.4. Summaryofsugar-bindingresiduepredictions

Table5summarizesthepredictionresultsforthethreedatasets usingthethreepredictors.Thecombinationpredictoryieldedthe best performance for thesugar-binding proteins and nonacidic sugar-binding proteins as test datasets. Acidic sugar-binding residuepredictorachievedthebestperformanceforacidic sugar-bindingproteinsasatestdataset.Thiswasprobablybecausethe parametersselected werebiasedtoward alargenumber ofthe nonacidicsugars(accountingforover70%oftheentiredataset), which in turn degraded the prediction capabilities for a small numberofpredictionforacidicsugarbindingresidue.The predic-tiontendencyofboththesugar-bindingresiduepredictorandthe combinationpredictorwassimilartothatofthenonacidic sugar-bindingresiduepredictor.

Inpractice,thecombinationpredictorwouldbethemost use-fulwhen thetargetsugarsareunknown.Ifitwereapparentin advancethatthetargetsugarspossessedanacidicfunctionalgroup, itwouldbepreferabletoemploytheacidicsugar-bindingresidue predictor.

4. Conclusions

Usingclusteranalysis,wefoundthattheaminoacid composi-tionsatthebindingsitesdifferedfortheacidicsugarsandnonacidic sugars.Whileahighproportionofbasicresidueswerefoundinthe bindingsitesfortheacidicsugars,theacidicresiduesglutamine

(8)

andasparaginewererelativelyscarce.However,amongthe bind-ingresiduesforthenonacidicsugars,theproportionsofglutamine, asparagine,andglutamicandasparticacidswerehigh,andthebasic residue,lysine,wasrelativelyscarce.Webelievethatthisdifference wasresponsiblefordividingthesaccharidesintotwoclusters.

Consideringtheseresults,weattemptedtoconstructan indi-vidualpredictorforacidic andnonacidicsugar-bindingresidues andsucceededinimprovingthepredictioncapabilities.The com-bination predictor, incorporating a linear combination of the predictiondevicesforacidicandnonacidic,sugar-binding,showed thebestperformanceinthepredictionofsugar-bindingresidues and nonacidic sugar-binding residues. This result showed the effectivenessof ourmethodof individuallearning accordingto the properties of sugar-binding residues. Our individual learn-ingapproachisparticularlyeffectivewhenthedifferenceinthe sequencefeaturesbetweenthegroupsislarge.Althoughthe perfor-manceofourmethoddoesnotseemtobesufficient,wesuccessfully showed an improvement in performance using the individual learningapproach.

We also developed a method to predict whether a given protein is sugar-binding. We builtthe work-flow system com-biningthepredictorofsugar-bindingproteinandsugar-binding residue, and launched this system onthe Web. The predictors could befound and used on the Galaxy pipeline (Blankenberg etal.,2010)withhighflexibility.Todaywepresentedthis prod-uctasanopensourcefreewaresystemontheGitHubrepository viadocumentobjectidentifierofZenodo(https://doi.org/10.5281/ zenodo.61513). Thus, the predictor performance of the sugar-bindingresiduewasobtainedonthesugar-bindingproteins,highly accuratepredictionscanbeachievedusingthissystem.The sugar-bindingresiduepredictionissolelybasedonaminoacidsequences; itisfastenoughtobeappliedtogenome-widepredictions. Acknowledgments

WewouldliketothankDr.WayneDawsonandthemembers oftheBioinformationEngineeringLaboratoryfortheirsupportand valuablediscussions.ThisworkissupportedbythePlatformfor DrugDiscovery,Informatics,andStructuralLifeSciencefromthe MinistryofEducation, Culture,Sports, Science,andTechnology, Japan.

AppendixA. Supplementarydata

Supplementarydataassociatedwiththisarticlecanbefound, intheonlineversion,athttp://dx.doi.org/10.1016/j.compbiolchem. 2016.10.009.

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