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Paper-basedAnalytical DevicesforChemical Analysisand Diagnostics Editedby
WilliamR.deAraujo
DepartmentofAnalyticalChemistry,InstituteofChemistry,State UniversityofCampinas—UNICAMP,Campinas,Brazil
ThiagoR.L.C.Paixa ˜ o
DepartamentofFundamentalChemistry,InstituteofChemistry, UniversityofSaoPaulo,SaoPaulo,Brazil
Elsevier
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Listofcontributors HugoA ´ guas i3N/CENIMAT,DepartmentofMaterialsScience,FacultyofScience andTechnology,UniversidadeNOVAdeLisboaandCEMOP/UNINOVA, CampusdeCaparica,Caparica,Portugal
WaleedAlahmad ChemicalApproachesforFoodApplicationsResearchGroup, FacultyofScience,ChulalongkornUniversity,Bangkok,Thailand;Departmentof Chemistry,FacultyofScience,ChulalongkornUniversity,Bangkok,Thailand
WilsonA.Ameku DepartamentodeQuı´micaFundamental,InstitutodeQuı´mica, UniversidadedeSa ˜ oPaulo,Sa ˜ oPaulo,Brazil
MarylynSetsukoArai Sa ˜ oCarlosInstituteofPhysics,UniversityofSa ˜ oPaulo,Sa ˜ o Carlos,Brazil
IanaV.S.Arantes DepartamentodeQuı´micaFundamental,InstitutodeQuı´mica, UniversidadedeSa ˜ oPaulo,Sa ˜ oPaulo,Brazil
VanessaN.Ataide DepartamentodeQuı´micaFundamental,InstitutodeQuı´mica, UniversidadedeSa ˜ oPaulo,Sa ˜ oPaulo,Brazil
EmanuelCarrilho Sa ˜ oCarlosInstituteofChemistry,UniversityofSa ˜ oPaulo,Sa ˜ o Carlos,Brazil;NationalInstituteofScienceandTechnologyinBioanalytics, INCTBio,Campinas,Brazil
CyroL.S.Chagas InstitutodeQuı´mica,UniversidadedeBrası´lia,Brası´lia,Brazil
Chao-MinCheng InstituteofBiomedicalEngineering,NationalTsingHua University,Hsinchu,Taiwan
WendellK.T.Coltro InstitutodeQuı´mica,UniversidadeFederaldeGoia ´ s,Goia ˆ nia, Brazil;InstitutoNacionaldeCie ˆ nciaeTecnologiadeBioanalı´tica(INCTBio), Campinas,Brazil
BrunoCosta-Silva ChampalimaudResearch,ChampalimaudCentreforthe Unknown,Lisbon,Portugal
WilliamR.deAraujo PortableChemicalSensorsLab,DepartmentofAnalytical Chemistry,InstituteofChemistry,StateUniversityofCampinas—UNICAMP, Campinas,Brazil
VanessaN.deAtaide DepartamentodeQuı´micaFundamental,InstitutodeQuı´mica, UniversidadedeSaoPaulo,SaoPaulo,Brazil
AndreaSimoneStucchideCamargo SaoCarlosInstituteofPhysics,Universityof SaoPaulo,SaoCarlos,Brazil
ElviraFortunato i3N/CENIMAT,DepartmentofMaterialsScience,Facultyof ScienceandTechnology,UniversidadeNOVAdeLisboaandCEMOP/ UNINOVA,CampusdeCaparica,Caparica,Portugal
CarlosD.Garcia DepartmentofChemistry,ClemsonUniversity,Clemson,SC, UnitedStates
PauloT.Garcia InstituteofExactSciences,FacultyofChemistry,Federal UniversityofSouthandSoutheastofPara ´ (UNIFESSPA),Maraba ´ ,Brazil
JulianaL.M.Gongoni DepartamentodeQuı´micaFundamental,Institutode Quı´mica,UniversidadedeSa ˜ oPaulo,Sa ˜ oPaulo,Brazil
ErinM.Gross CreightonUniversityDepartmentofChemistryandBiochemistry, Omaha,NE,UnitedStates
Ba ´ rbaraG.S.Guinati InstitutodeQuı´mica,UniversidadeFederaldeGoia ´ s, Goia ˆ nia,Brazil
SamayaKallepalli CreightonUniversityDepartmentofChemistryand Biochemistry,Omaha,NE,UnitedStates
TakashiKaneta DepartmentofChemistry,GraduateSchoolofNaturalScienceand Technology,OkayamaUniversity,Okayama,Japan
AnaCarolinaMarques i3N/CENIMAT,DepartmentofMaterialsScience,Faculty ofScienceandTechnology,UniversidadeNOVAdeLisboaandCEMOP/ UNINOVA,CampusdeCaparica,Caparica,Portugal;ChampalimaudResearch, ChampalimaudCentrefortheUnknown,Lisbon,Portugal;BioMark@UC, DepartmentofChemicalEngineering,FacultyofScienceandTechnology, CoimbraUniversity,Coimbra,Portugal
RodrigoMartins i3N/CENIMAT,DepartmentofMaterialsScience,Facultyof ScienceandTechnology,UniversidadeNOVAdeLisboaandCEMOP/ UNINOVA,CampusdeCaparica,Caparica,Portugal
Letı´ciaF.Mendes DepartamentodeQuı´micaFundamental,InstitutodeQuı´mica, UniversidadedeSaoPaulo,SaoPaulo,Brazil
NikaeleS.Moreira InstitutodeQuı´mica,UniversidadeFederaldeGoia ´ s,Goia ˆ nia, Brazil
ThiagoR.L.C.Paixa ˜ o DepartmentofFundamentalChemistry,Instituteof Chemistry,UniversityofSaoPaulo,SaoPaulo,Brazil;NationalInstituteof BioanaliticalScienceandTechnology,Campinas,Brazil
MariaGoretiSales BioMark@UC,DepartmentofChemicalEngineering,Facultyof ScienceandTechnology,CoimbraUniversity,Coimbra,Portugal;BioMark@ISEP, SchoolofEngineering,PolytechnicInstitutePorto,Porto,Portugal;CEB–Centreof BiologicalEngineering,UniversityofMinho,Braga,Portugal
Ching-FenShen DepartmentofPediatrics,NationalChengKungUniversity Hospital,CollegeofMedicine,NationalChengKungUniversity,Tainan,Taiwan
HabdiasA.Silva-Neto InstitutodeQuı´mica,UniversidadeFederaldeGoia ´ s, Goia ˆ nia,Brazil
Listofcontributors xv
LucasR.Sousa InstitutodeQuı´mica,UniversidadeFederaldeGoia ´ s,Goia ˆ nia, Brazil
Yao-HungTsai InstituteofBiomedicalEngineering,NationalTsingHuaUniversity, Hsinchu,Taiwan
PakornVaranusupakul ChemicalApproachesforFoodApplicationsResearch Group,FacultyofScience,ChulalongkornUniversity,Bangkok,Thailand; DepartmentofChemistry,FacultyofScience,ChulalongkornUniversity, Bangkok,Thailand
TingYang InstituteofBiomedicalEngineering,NationalTsingHuaUniversity, Hsinchu,Taiwan
1.Introductionremarksforpaper-basedanalytical devicesandtimeline 1
WilliamR.deAraujoandThiagoR.L.C.Paixao
2.Chemistryofpaper—properties,modification
3.Paper-basedseparationdevices
CyroL.S.Chagas,NikaeleS.Moreira,B
3.3Paper-baseddevicesforchromatographicseparations
3.3.1Electrochemicaldetection49
3.3.2Colorimetricdetection52
3.3.3Chemiluminescencedetection53
4.Colorimetricpaper-basedanalyticaldevices
HabdiasA.Silva-Neto,LucasR.SousaandWendellK.T.Coltro
4.1Introduction
4.2Physicalaspectsofcolorimetricdetection
4.3Colorimetricreactionmethodology
4.4Detectionandreadoutsystem
4.4.1Officescanner69
4.4.2Smartphone69 4.4.3Visualdetection71
4.4.4Comparisonofimagedigitalizationmethods71 4.5Conclusionsandperspectives
5.Electrochemicalpaper-basedanalyticaldevices
IanaV.S.Arantes,JulianaL.M.Gongoni,Let´ıciaF.Mendes, VanessaN.deAtaide,WilsonA.Ameku,PauloT.Garcia, WilliamR.deAraujoandThiagoR.L.C.Paixa ˜ o
5.1Introduction 81
5.2Principlesoftheelectrochemicalmeasurementsusing electrochemicalpaper-basedanalyticaldevices 82
5.3Paperstandardizationandareadefinition 84
5.3.1Patterningnonconductivematerialsonthepapersurface85
5.3.2Electrodesfabricationbyconductivepatterningtracks onpaper86
5.4Thefabricationprocessesofelectrochemicalpaper-based analyticaldevicesandtheirapplications 88
5.4.1Screen-printingandstencilprinting88
5.4.2Digitalprintingandprinterfabricationprocesswithout theuseofmasks90
5.4.3Photolithographyandsputtering94
5.4.4Drop-casting96
5.4.5Pencil-drawing98
5.4.6Graphiteleadsandwirematerialsaselectrodesonpaper102
5.4.7Filtration103
5.4.8Pyrolysisprocess105
5.4.9Laser-scribing105
5.5Conclusionsandperspectives 106 Acknowledgments 107 References 107
6.Surface-enhancedRamanscatteringpaper-based analyticaldevices 117
AnaCarolinaMarques,HugoA ´ guas,RodrigoMartins, BrunoCosta-Silva,MariaGoretiSalesandElviraFortunato
6.1Introduction 117
6.1.1Ramanspectroscopy:ahistoricalperspective117
6.1.2TheoreticalfundamentalsofRamanspectroscopyand SERS118
6.2Ramanenhancementnanostructuresontopapersubstrates: characteristicsandfabricationmethods 121
6.2.1Gold-basednanostructures122
6.2.2Silver-basednanostructures133
6.2.3Goldandsilvercompositesnanostructures143
6.3Applicationsofpaperandcellulose-basedSERSdevices 146
6.3.1Healthapplications:diagnosticandtherapeutics146
6.3.2Environmentalapplications:food,dairyproducts, beveragesandwatersafety150
6.3.3Otherapplications154
6.4Concludingremarksandperspectives 155
6.5Acknowledgements
7.Chemiluminescencepaper-basedanalyticaldevices 169 WaleedAlahmad,PakornVaranusupakulandTakashiKaneta
7.1Introduction 169
7.2Designandfabricationtechniquesforchemiluminescencemicrofluidicpaper-basedanalyticaldevices 169
7.3DetectionofchemiluminescenceSignalsonmicrofluidic paper-basedanalyticaldevices 170
7.3.1Commercialluminescenceanalyzers170
7.3.2Miniaturizedphotomultiplier173
7.3.3Charge-coupleddevicesanddigitalcameras175
7.3.4Smartphones176
7.3.5Othertoolsandinstruments176
Contents
7.4Conclusion
8.Fluorescentpaper-basedanalyticaldevices 183
MarylynSetsukoArai,AndreaSimoneStucchideCamargoand EmanuelCarrilho
8.1Introduction 183
8.2Fluorescentmaterials 184
8.2.1Organicdyes185
8.2.2Metalnanoclusters185
8.2.3Carbondots186
8.2.4Quantumdots187
8.2.5Upconversionnanoparticles188
8.3Fluorescentresponse 189
8.3.1Brightness-basedresponse189
8.3.2Color-basedresponse196
8.4Conclusions 204 References 205
9.Electrochemiluminescencepaper-basedanalytical devices 213
ErinM.GrossandSamayaKallepalli
9.1Background 213
9.1.1Electrochemiluminescence213
9.1.2Paperdevicesandelectrochemiluminescence214
9.2Paper-devicefabricationmethods 216
9.2.1Papertypes218
9.2.2Fabricationofhydrophobicbarriers219
9.3Fabricationofelectrodesontopaper 220
9.3.1Screenprinting220
9.3.2Bipolarelectrodes222
9.3.3Hybriddevices231
9.4Electrochemiluminescencesensingstrategies 231
9.4.1Electrochemiluminescenceimmunoassays231
9.4.2Aptamer-basedelectrochemiluminescenceassays233
9.4.3Signalamplification235
9.5Potentialcontrolanddetection:worktowardportable devices 235
9.5.1Potentialcontrol235
9.5.2Detection235
9.6Integrateddevices 236
9.7Conclusionsandfuturedirections 237 Acknowledgments 238 References 238
10.Paper-basedimmunoassaysformobilehealthcare: strategies,challenges,andfutureapplications 245 Yao-HungTsai,TingYang,Ching-FenShenandChao-MinCheng
10.1Clinicalvalueofpaper-basedimmunoassays
10.2Thestrategiesofpaper-basedimmunoassayformobile healthcare
10.3Thechallengesofpaper-basedimmunoassayapproaches formobilehealthcare
10.4Futureapplicationsofpaper-basedimmunoassaysfor mobilehealthcare
11.Conclusions,challenges,andnextsteps
IanaV.S.Arantes,Let´ıciaF.Mendes,VanessaN.Ataide, WilliamR.deAraujoandThiagoR.L.C.Paixa ˜ o
11.1Introduction
11.1.1Challengesinfluidtransport260
11.1.2Challengesofcolorimetricdetection263
11.1.3Challengesofelectrochemicalpaper-baseddevices266
Dedication ThiagoR.L.C.Paixa ˜ odedicatesthisbooktohiswifeand son,whohaveinspired,encouraged,andhelpedhimin everythinghehasdone.Additionally,hewouldliketothank allthefundingagenciesthatsupportedhisresearchgroup (FAPESP,CNPq,INCTBio,andCAPES)andhisstudentsand collaboratorswhohavecontributedwithinspirationand knowlegde.Additionally,healsowouldliketothankthe InstituteofChemistryoftheUniversityofSa ˜ oPaulo.
WilliamRdeAraujodedicatesthisbooktohisparents, CleinaandAntonio,andtothememoryofhisgrandparents, AssisandMaria,whogavealltheirsupportandlove. Additionally,heisgratefultohisstudentsandcollaborators whohavecontributedwithinspiringworksandknowledge. HealsowouldliketothanktheInstituteofChemistryofthe StateUniversityofCampinasandtheBrazilianfunding agencies(FAPESP,CNPq,andCAPES)thatsupportedhis researchgroup.
Preface Paper-basedAnalyticalDevicesforChemicalAnalysisandDiagnostics have beenahottopicintheliteraturesince2007,enablingthefabricationoflowcostdevicestogetherwithawell-knownsubstratewithexcitingpossibilities forpoint-of-careandpoint-of-needapplicationswithoutexpensiveinstrumentation.Hence,thisbookprovidesareviewofthescientificandtechnologicalprogressofpaper-baseddevicescombiningdifferentdetection techniquesonthepaperplatformandfuturetrendsinthefieldof portablepaper-basedsensorsforchemicalanalysisanddiagnostics.The detectiontechniquesfocusoncolorimetric,electrochemical,surfaceenhancedRamanspectroscopy,chemiluminescence,fluorescence,electrochemiluminescence,andimmunoassays.Collectively,thisbookfocusesonthe analyticalmethodsofeachdevice,highlightssometipsandchallengesin thisresearchfield,showsaplethoraofcleverapproachesandstrategiesto developaccessible,accurate,andconvenientportableanalyticaldevices,and providesapracticalframeworkforanyresearchertousethemwhilelearning howtousenewones.Additionally,thechemistryofpaperaimingatits uniquepropertiesandmodificationstrategiesfor(bio)analyticalchemistry applicationsispresented.
Wewanttothankallthecontributingauthorsfortheirenthusiasmand participationinpreparingthisbook.WealsowouldliketoexpressourgratitudetotheeditorialandproductionstaffofElsevier,inparticular,Lena Sparks,forherassistanceinbringingthisbooktoprintandpublication.
Chapter1 Introductionremarksfor paper-basedanalyticaldevices andtimeline WilliamR.deAraujo1 andThiagoR.L.C.Paixa ˜ o2,3 1PortableChemicalSensorsLab,DepartmentofAnalyticalChemistry,InstituteofChemistry, StateUniversityofCampinas—UNICAMP,Campinas,Brazil, 2DepartmentofFundamental Chemistry,InstituteofChemistry,UniversityofSaoPaulo,SaoPaulo,Brazil, 3NationalInstitute ofBioanaliticalScienceandTechnology,Campinas,Brazil
1.1Introduction Asinglepieceofpaperhasnowbeencallingattentionfromacademic researchgroupsandindustryinthelast13yearsmorethanintheprevious centuriestodevelopanalyticaldevicesforpoint-of-needapplications.From thepastto2007,differentrandomcontributionsfromtheacademicliterature hadattemptedtohighlightthepotentialityofpaperasasubstrateforanalyticalpurposes,aschromatographicandelectrophoreticseparations,andin rapidspottests.However,onlyin2007,thispoint-of-viewstartedtochange toputpaperas“new”-oldmaterialforthedevelopmentofanalyticaldevices, asshownbythenumberofarticlesandcitationsreportedin Fig.1.1.Inaddition,itisessentialtohighlighthowthisdevelopmentspreadglobally, Fig.1.2,showingtheengagementofdifferentresearchgroupsaroundthe worldinthedevelopmentofpaperdevicestobeappliedtodecreasecostsof real-timeanalyticaltestsforvariouson-siteapplications.
Fig.1.3 highlightssomerecentapplicationsofpaper-basedanalytical devices(PADs)inthemainfieldsofanalyticalchemistry.Notethatthesignificantcontributionswereappliedinhealthcare/clinicalandenvironmental areasduetotheextraordinaryappealfornewpoint-of-caretesting(POCT) devicesandthecontinuousneedforportablesensorstocheckthequalityof oursurroundings(air,water,andsoil),respectively.Itisworthmentioning thattheareasoffoodqualityandforensicshaveattractedsignificantattentionand,inthenearfuture,willbenefitfromthepaper-basedsensor technology.
2 Paper-BasedAnalyticalDevicesforChemicalAnalysisandDiagnostics
FIGURE1.1 NumberofarticlespublishedandcitationovertheyearextractedfromtheWeb ofScienceusingthefollowingkeywords:“paperpatterned,”“microfluidicpaper-based,”“paperbasedanalytical,”“electrochemicalpaper-based,”“colorimetricpaper-based,”“paper-basedanalyticaldevices,”“sensingpaper,”“papersubstrate,”or“paperasaplatform.”
FIGURE1.2 Worldmapshowsthenumberoftotalarticlerecordsduringthesameperiodof thedatareportedin Fig.1.1 andusingthesame Fig.1.1 keywords.Datawereextractedfromthe WebofScience.
Theuseofpapermaterialforchemicalanalysisreferstoseveraleras.Maybe thefirstknownaccountwasassociatedwithPlinystudiesin23BCE,wherea test“paper”methodfordetectingthepresenceofferroussulfateadulterationin verdigriswasdescribed.Papyrusstripsdippedinanextractfromgallnuts
FIGURE1.3 NumberofarticlespublishedusingPADsindifferentareasofanalyticalchemistryinthesameperiodof Fig.1.1.DataextractedfromtheWebofScienceusingthefollowing keywords:“paper-baseddevicesandclinical”or“paper-baseddevicesandhealthcare,”“paperbaseddevicesandenvironmental,”“paper-baseddevicesandfood,”and“paper-baseddevices andforensics.”
blackensimmediatelyinthepresenceoftheironadulterant [1,2].Nowadays, manykindsofpapermaterialsareavailable,varyingincomposition,morphology,fiberalignment,porosity,etc.,andthesedifferencesprovidespecialperformances.Theseaspectscanimprovetheperformanceofpaper-basedsensors,like theirmicrofluidicspropertiesorcapabilitytoimmobilize(bio)compounds. Recently,filterandchromatographicpapersarethesignificantsubstrates employedinthedevelopmentofmicrofluidicdevicesduetotheirsuperiorwickingability [3];however,differentphysicaland/orchemicalcharacteristicsmay berequiredbiosensors,othercategoriesofpaperhavebeenexploreddepending onthetargetapplication.Nitrocellulosemembraneshavebeenusedduetotheir chemicalfunctionalgroupsthatenablethequicklycovalentimmobilizationof biomolecules [3].
Othernonlaboratory-basedpapersubstrateshavebeenusedforthefabricationofinexpensivePADs,suchastheuseofglossypaper [4],officepaper [5],towelpaper [6],andpaperboard [7].Thesetypesofpaper,ingeneral, providelowerwettabilityandhigherphysicalstability.However,theyare lesspurepresentingfillersinyourcomposition,whosecompoundscould interfereinthebioassaysor,insomecases,enhancethemeasuredproperties [7].Inaddition,thechemistryofpapersurfaceisveryvast,andseveral approachestochangefunctionalgroupstoenhancechemicalinteractions, microfluidics,andotherpropertiesofpapersensinghavebeenreported.A deepdiscussionaboutthemainstrategiesandtypesofpaperwillbepresentedinChapter2,ChemistryofPaper—Properties,Modification Strategies,andUsesinBioanalyticalChemistry.
Sincetheinventionofthepaper,anditsfabricationprocess,byChinese CaiLunin105CE [8],itsmainadvantagewastostorageacknowledgment fromgenerationtogenerationwithoutusingoldsubstrateslikewritingin stoneandanimalskins.Tounderstandthisnewsearchforthedevelopment ofanalyticaldevicesusingpaper,thisbookisproposed.Wewillstartabrief historicalaspectdiscussionofthisdevelopment,aimingatanalyticaldevices.
Sinceitsinvention,theideawastotransferhistoryfromonecivilization toanother,keepmemoriesalive,addink,ordyes,topaper.Theuseofanalyticaldeviceswasbasedonthissameidea.Thepapermatrixstoreschemicalreagents,asthedyestorageduringthewritingprocess,toperform chemicalreactionstoqualifyorquantifychemicalspecies.Thisfeaturewas probablynotthoughtofbyitsinventor.Thiscapabilitytostoragechemical compoundsisbasedonthepaperproduction,whichcamefromadilute aqueoussuspensionofcellulosefibersthat,throughdifferentprocesseslike sievedrain,press,anddryprocess,yieldasheetresultedbyrandomlyinterwovenfibersorientation [9],areservoirforchemicalcompounds.Inaddition,this3Dstructureobtainedwillbeessentialtoresultinthespontaneous capillarytransportofsolutioninsidethat,whichisessentialforthemicrofluidicsdevelopment [10].
Historically,thelitmuspaper(mixtureofdyesextractedfromlichens absorbedontofiltercellulosepaper)isprobablythefirstanalyticaltestfound foracidityandbasicityofdifferentsolutionsasafastpoint-of-needexperiment becausethechemicalcompound(dyes)storedinthecellulosepaperchanges thecolorinthepresenceofprotonwithoutthenecessityofchemicalequipment formeasurement.ItsinventionwasattributedtoIrishchemistRobertBoylein the17thcentury,anditisstillinusenowadays [11].Atthispoint,thefirst essentialcharacteristicofpapercouldbenoted,theabsorbency,thecapability tostorechemicalreagentsinsidethepapermatrix,andthedisposabilityofthe devicebecausethepaperstripcouldbeusedforasingletime.
Intentionallyornot,theintroductionofpapersubstratesolvedanessentialtrade-offinthesensorareaandiswell-exploredbypaper-basedresearchersnowadays.Oneoftherequirementsfordevelopingthesensoristhatthe proposeddeviceneedstoberobust.However,robustnessrequiresweak interactionsonly,whichimplieslowsensitivityandlowchemicalspecificity. Thedisposabilitycharacteristicsofthepaper-basedsensors,andconsidering thereproducibilityofthefabricationprocess,allowedustoprobeawide rangeofchemicalinteractionandreaction,includingstrongsensor-analyte bindingbecausethedevicewillnotbeusedmorethanonce.Norequirement willneedtoperformachemicalorphysicaltreatmenttousethedevicefora secondtime.Anothercriticalaspectofthelitmuspaperisrelatedtothe visualreporter.Theproposedanalyticaldeviceconvertschemicalinteraction responsestoanopticaloutput,whichisessentialforlow-costspreadofthe paper-basedsensorsandappealsforthedevelopmentofdiagnosticforthe developingworld [12]. 4 Paper-BasedAnalyticalDevicesforChemicalAnalysisandDiagnostics
Introductionremarksforpaper-basedanalyticaldevices Chapter|1 5
Afterthisfirstfoundpaper-basedtest,in1850,aurineteststripwasproposedbyMaumene ´ ,whichusesabrown-blackcolorformationforacolorimetricreactionbetweensugarinurineandtheproposedreagent [9,13,14].In anothermanuscript [15],theauthorusedthepreviousurineteststripreportingthatdeviceshaveessentialadvantagesformedicalapplicationsdueto theirsimplicityandon-siteapplicabilitycomparedtosolution-basedassays.
In1937Yagoda [1] describedseveralachievementsofthattimeregardingthedevelopmentofspottestsonpaperplatformandhighlightsthat“The useofpaperimpregnatedwithsuitablereagentsinestablishingthepresence ofchemicalconstituentsisprobablyoneoftheearliestdevelopmentsinthe artofAnalyticalChemistry”usingthepioneeringFritzFeigl’sdiscovery about"spotanalysis"(spottest) [36].Inaddition,yourpioneeringstudiesto confinethespottestwiththeaidofawater-repellentbarrier(paraffin) embeddedinthefibersofthepaperallowedperformingcolorimetrictestson porousfilterpaperwithoutlossinsensitivityowingtothespreadingofthe spotoveralargesurface.Thispointwasnecessarybecausetheuniformityin theareaandtintofthespotprovidesthecorrelationbetweentheconcentrationofthespecieswiththeintensityofcolorproducedbythedropofsolution.Thiswasthefirststeptoprogressinsemiquantitativeanalysesinstead ofqualitativeresultsgenerallyperformed.
Aninterestinghistoricalpointregardingthepatternofpapersubstrate reportedbyYagoda [1] formicroanalysiswasthedescriptionofmanysubstancessuchaswaxes,resins,andcelluloseesterstostandardwater-repellent zonesonfilterpaper.Highlightingmainlytheuseofparaffinwaxduetoits generalinertnesstochemicalreagentsandtotheeasewithwhichitcanbe embeddedindiversepatternsonthepaper,astheuseofahotmetaltubefor melttheparaffinandtransfertoasheetofpaperinthering-shapedzones (Fig.1.4A) [1].Morethan70yearslater,Carrilhoetal. [16][16] describedthe technologicaladvancesthatallowedtheuseofacommercialscreen-printer controlledbycomputertoprintathinlayerofwaxinanydesireddesignto patternthepaperreproducibly,whichmovesthepaper-basedsensorstoward accuratequantitativeresults(Fig.1.4B).Severalstrategiesbasedonthe Yagodaapproachwerepublishedinthe2000s,likeusingahandheldstamping processtotransferparaffinfromparaffinedpapertoanotherusingapreheated metalstamptofabricatemicrofluidicPADs(µPADs)(Fig.1.4C) [17].
Inlightoftheanalyticalapplications,thecapabilitytoperformphysical andchemicalseparationsofananalyteorgroupofanalytesfromacomplex matrixisessentialforaccuratedeterminations.Regardingthisaspect,the papersubstratecompositionandstructureallowthespontaneoustransportof aqueoussolutionbycapillarityanddifferentialflowrateofthecomponents duetophysicochemicalinteractionswiththecellulosicphase.ThefirstindicationontheuseofpaperinseparationsciencewasgivenbyVon KlobusitzkyandKo ¨ nig [18],whoemployedthisplatformtoisolatesyellow pigmentsfromsnakevenom.Inthe1940sand1950s,paperbegantomake
Continued )
▲
severalcontributionstoseparationsciences,beingexploredasasubstratefor chromatographicandelectrophoreticseparations,mainlyforplantextract analysesandbiochemicalapplicationsthataimedtoseparateaminoacids, peptides,andproteins [19,20].AfurtherdiscussionandmilestonesofpaperbasedseparationdevicescanbefoundinChapter3,Paper-BasedSeparation Devices.
In1957whenitisreportedthefirstpaper-basedbiosensorintheliterature [21] whichusedcolorreportedfromachemicalreactiontodetectglucosetocircumventtheissuereportedby Benedict’stest.Anotherimportant factindevelopingpaper-basedsensorsandmicrofluidicsin1982appeared intheliteratureusinganothercolorimetricvisualreporterandthecapillaritypropertiesofpaperoriginallyintroducedbyMullerandClegg [22].The lateralfloworiginatedbythecapillar itypropertieswasusedtofabricatean assaytoscreenhybridomasbasedonantigen antibodyinteractiononpaper toproduceavisiblecolorchangetothenakedeye [23] .Thesearticles openedthebasisforthepregnancytestkitswidelyusednowadaysand startedimplementingmicrofluidicsresearch.Fromthatto2007,norevolutionarydevelopmentseemedtohave occurredintermsofpaper-based chemicalsensingapproaches,onlysomeessentialindustriesstartedtowork inthedevelopmentofpaper-basedteststripssuchasMerck [24] and others.
ThenextbreakthroughinPADsdevelopmentwasreportedin2007.It wasresponsiblefortheenhancementofarticlespublished,asshownin Fig.1.1,whentheWhitesidesandcollaboratorsreportedaverycleverway tointroducemicrofluidicpatternsonapaperstructureusingaphotoresistto controlthefluidflowdirection [25],andtheresearchfieldrelatedwiththe µPADswasopenpublishingmorethan1000articlesuntilnow.Inaddition,
FIGURE1.4 (A)Paraffinpatternedspottestsonpaper.(B)Patterninghydrophobicbarriersin paperbywaxprinting.(a)Schematicrepresentationofthebasicsteps [1 3] requiredforwax printing.(b)Digitalimageofatestdesign.Thecentralareaofthedesignwasmagnifiedto showthemoreminorfeatures.(c)ImagesofthetestdesignprintedonWhatmanno.1chromatographypaperusingthesolidinkprinter.Thefrontandbackfacesofthepaperwereimaged usingadesktopscanner.(d)Imagesofthetestdesignafterheatingthepaper.Thedashedwhite linesindicatetheoriginaledgeoftheink.Thewhitebarsintheinsetshighlightthewidthofthe patternatthepositionindicatedbythearrows.(C)Schemeofthefabricationprocessof µPADs basedonstamping.In(1),aparaffinizedfilterpaperisplacedoverthenativefilterpapersurface;in(2),themetalstampisheatedat150 Candbroughtintocontactwiththelayeredpaper pieces;step(3)representsatypical µPADfabricatedbytheproposedmethod. (A)Reprinted adaptedwithpermissionfromH.Yagoda,Applicationsofconfinedspottestsinanalyticalchemistry:preliminarypaper,Ind.Eng.Chem.Anal.Ed.9(2)(1937)79 82.Availablefrom: https:// pubs.acs.org/doi/abs/10.1021/ac50106a012.Copyright2020AmericanChemicalSociety.(B) ReprintedwithpermissionfromE.Carrilho,A.W.Martinez,G.M.Whitesides,Understanding waxprinting:asimplemicropatterningprocessforpaper-basedmicrofluidics,Anal.Chem.81 (16)(2009)7091 7095.Availablefrom: https://pubs.acs.org/doi/10.1021/ac901071p.Copyright 2020AmericanChemicalSociety. http://xlink.rsc.org/?DOI 5 C4RA07112C
8 Paper-BasedAnalyticalDevicesforChemicalAnalysisandDiagnostics
in2009thesamegroupreportedinouropiniontherealarticleresponsible forthepopularizationofthePADsinanalyticalchemistryduetolowcost andcommerciallyavailablewaytocreatethemicrofluidicchannelinthe paperstructureusingwaxprintingtechnologywithoutlaboriousstepsorany additionallaboratory-basedrequirements [16]
Afterward,numerous µPADsusingcolorimetricdetectionstartedtobe fabricated.Thenumberofarticlespublishedinthisfieldbegantoincreaseas reportedagainin Fig.1.1,creatingnowthescientificenvironmentforpaper gainpopularitytobethe“new”materialinanalyticalchemistrytoproduce andcreatenovelcommerciallyavailabledevicesforclinicalapplications,in thefirstmomentduetoitsadvantageablecharacteristicsasoflowcost, availability,equipment-freepumpingofasolution,simplicity,andsuitability indisposabledevicesascomparedovertheothermaterials.
Basedontheadvantagecharacteristicsreportedhere,PADsappearina goodmomentinanalyticalchemistry.Oneoftheresearchlinesinthisanalyticalchemistryfieldistheminiaturizationofthedevicestohavesmall devicesforpoint-of-needapplicationstohelpmedicalexperts. Fig.1.5
FIGURE1.5 Evolutioninanalyticalchemistrytominiaturizetheinstrumentsforacomplete point-of-needapplicationanywhere. Fig.1.1AandB showedanexampleofapaperwearable deviceforsweatmeasurements [29] ReprintedwithpermissionbyCreativeCommons Attribution-NonCommercial3.0UnportedLicenceandpublishedbyTheRoyalSocietyof ChemistryfromQ.Cao,B.Liang,T.Tu,J.Wei,L.Fang,X.Ye,Three-dimensionalpaper-based microfluidicelectrochemicalintegrateddevices(3D-PMED)forwearableelectrochemicalglucosedetection,RSCAdv.9(10)(2019)5674 5681.Availablefrom: http://xlink.rsc.org/? DOI 5 C8RA09157A.Copyright2020TheRoyalSocietyofChemistry.
reportstheevolutionofportabledevicestohaverealandsmall,point-ofneedequipment.Wecrossthefirstboundarywiththefirstglucometer proposedintheliterature [26],movingthediagnosticsforourhome.Itis probablythefirstsuccessfulcommercialcaseofelectrochemicalPOCTsensorsintheindustrypoint-of-needapplication.Thewearableequipmentcame tostay [27].Nowwearemovingtothenextboundaryin Fig.1.5,where paper [28] appearsasonealternativeforthisevaluationandforcharacteristicsdiscussedinthisbook.
Notethatthefirstreportsofusingpaperforchemicaltestswereprimarily usedasasubstrateforcarryingoutpresumptivetests.However,thereiscurrentlyagreatefforttointegratemultipleanalyticalstepsinthesamedevice. Thepaperhasdifferentfunctionswithsamplingsteps,sampletreatment, constituentseparation,andevenmultipledetectionzonesformultiplexed determinations.Thusthereisatrendtowardthedevelopmentoflab-on-apaperdevicestooperatein-fieldanalysistruly.
Thesmartphonetechnologyhasasignificantcontributiontothisresearch fieldbecausethesedevicesallowcouplingseveraldetectorstobeusedon PADsdirectlyatthepoint-of-need,enhancingtheuser-friendlyofthe portablechemicaltestsandallowingthecommunicationbywirelesstotransferinreal-timetheresultstotheuseroramanagercenter.Animportant pointwastheuseofthecameraofthesmartphonesalliedtoseveralappsto extractcolorpatternsfromimagesofchemicaltests.Thisapproachallows conductingquantitativeanalysesandminimizingpossiblemistakesduethe dubiousnaked-eyecolorinterpretation.Hence,asalreadydescribed, Chapter2,ChemistryofPaper—Properties,ModificationStrategies,and UsesinBioanalyticalChemistry,willstarttodiscussthepaperchemistryto understanditsparticularcharacteristic,whichturnsthisoldmaterialasthe “new”platformforanalyticaldevicesandtheuniqueattributesforseparationssciences(Chapter3:Paper-BasedSeparationDevices).Afterthat,differentdetectorswerecoupledtothePADsafterthecolorimetric(Chapter4: ColorimetricPaper-BasedAnalyticalDevices)onetoenhancethesensitivity, selectivityorexpandtherangeofsensinganalytes.Otherstandarddetection methodssuchaselectrochemical,surface-enhancedRamanscattering,chemiluminescence,fluorescence,electrochemiluminescence,andusingimmunoassayswillbediscussedfromChapters5 10,reportingdifferentwaysto producethesedevices.
AbriefrecenttimelineoftheevolutionofPADsforquantitativeanalysis after2007isdisplayedin Fig.1.6,whereitishighlightedthedifferentdetectionmethodsoccurrencecoupledtoportablepapersensors.However,itis essentialtoemphasizethatitsqualitativeuseisolderthanthisproposed timelinereportedin Fig.1.6,aspreviouslymentionedinthischapter.
Finally,thefinalchapterofthisbooksummarizesthemainachievements anddrawbacksfoundinthisfantasticresearchfield,highlightingthetremendouschallengesforthecontinuousprogressofthisarea.
FIGURE1.6 TimelineofPADsafter2007usingdifferentdetectors,orseparationtechniques, coupledtothePADs:(A)colorimetric [25],(B)electrochemical [30],(C)fluorescent [31],(D) (Continued )
Introductionremarksforpaper-basedanalyticaldevices Chapter|1 11
▲ chemiluminescence [32],(E)paper-basedseparationdevice [33],(F)electrogeneratedchemiluminescencedetection [34],(G)Surface-enhancedRamanspectroscopypaper-baseddevice. (A) ReprintedwithpermissionfromA.W.Martinez,S.T.Phillips,M.J.Butte,G.M.Whitesides, Patternedpaperasaplatformforinexpensive,low-volume,portablebioassays,Angew.Chem. Int.Ed.46(8)(2007)1318 1320.Availablefrom: http://doi.wiley.com/10.1002/anie.200603817
CopyrightJohnWileyandSons.(B)ReprintedwithpermissionfromW.Dungchai,O. Chailapakul,C.S.Henry,Electrochemicaldetectionforpaper-basedmicrofluidics.Anal.Chem. 81(14)(2009)5821 5826.Availablefrom: https://pubs.acs.org/doi/10.1021/ac9007573
Copyright2020AmericanChemicalSociety.(C)ReprintedwithpermissionfromM.M.Ali,S.D. Aguirre,Y.Xu,C.D.M.Filipe,R.Pelton,Y.Li,DetectionofDNAusingbioactivepaperstrips. Chem.Commun.(43)(2009)6640.Availablefrom: http://xlink.rsc.org/?DOI 5 b911559e
Copyright2020TheRoyalSocietyofChemistry.(D)ReprintedwithpermissionfromJ.Yu,L. Ge,J.Huang,S.Wang,S.Ge,Microfluidicpaper-basedchemiluminescencebiosensorforsimultaneousdeterminationofglucoseanduricacid.Lab.Chip11(7)(2011)1286.Availablefrom: http://xlink.rsc.org/?DOI 5 c0lc00524j.Copyright2020TheRoyalSocietyofChemistry.(E) ReprintedwithpermissionfromR.F.Carvalhal,M.Sima˜oKfouri,M.H.deOliveiraPiazetta,A. L.Gobbi,L.T.Kubota,Electrochemicaldetectioninapaper-basedseparationdevice.Anal. Chem.82(3)(2010)1162 1165.Availablefrom: https://pubs.acs.org/doi/10.1021/ac902647r
Copyright2020AmericanChemicalSociety.(F)ReprintedwithpermissionfromJ.L.Delaney, C.F.Hogan,J.Tian,W.Shen,Electrogeneratedchemiluminescencedetectioninpaper-based microfluidicsensors,Anal.Chem.83(4)(2011)1300 1306.Availablefrom: https://pubs.acs. org/doi/10.1021/ac102392t.Copyright2020AmericanChemicalSociety. http://xlink.rsc.org/? DOI 5 C2AN36116G
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