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ARTÍCULO

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Received1Sep2014 Accepted6Jan2015 Published16Feb2015 DOI: 10.1038 / ncomms7205

Transparentair fi lterforhigh-ef fi ciencyPM 2,5

captura
1, 1, 1 2 3 4 1 1,5
ChongLiu *, Po-ChunHsu *, Hyun-WookLee , Mengye , GuangyuanZheng , NianLiu , WeiyangLi y YiCui

Particulatematter (PM) pollutionhasraisedseriousconcernsforpublichealth.Although

outdoorindividualprotectioncouldbeachievedbyfacialmasks, indoorairusuallyrelieson

expensiveandenergy- intensiveair- fi lteringdevices.Here, weintroduceatransparentair filtro

forindoorairprotectionthroughwindowsthatusesnaturalpassiveventilationtoeffectively

protecttheindoorairquality.BycontrollingthesurfacechemistrytoenablestrongPM

adhesionandalsothemicrostructureoftheair fi lterstoincreasethecapturepossibilities, que

achievetransparent, highair fl owandhighlyeffectiveair fi ltersof B90% transparencywith

495,00% removalofPM 2,5 underextremehazardousair-qualityconditions (PM 2.5 masa


?3
concentración 4250mgm ) .A fi eldtestinBeijingshowsthatthepolyacrylonitriletrans-

parentair fi lterhasthebestPM 2,5 removalef fi ciencyof98.69% athightransmittanceof

B77% duringhazeoccurrence.

1 2
DepartmentofMaterialsScienceandEngineering, Universidad Stanford, Stanford, California94305, EE.UU.. DepartmentofCivilandEnvironmental
3
Ingeniería, Universidad Stanford, Stanford, California94305, EE.UU.. DepartmentofChemicalEngineering, Universidad Stanford, Stanford, California94305,
4 5
EE.UU.. DepartmentofChemistry, Universidad Stanford, Stanford, California94305, EE.UU.. StanfordInstituteforMaterialsandEnergySciences, SLACNational
AcceleratorLaboratory, 2575SandHillRoad, MenloPark, California94025, EE.UU. * Theseauthorscontributedequallytothiswork.Correspondencean. D

requestsformaterialsshouldbeaddressedtoY.C. (E-mail: yicui@stanford.edu).

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ARTÍCULO NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205

P articulatematter (PM) pollutioninairaffectspeople'sliving


qualitytremendously, anditposesaserioushealththreatto
particlesaredifferentbecauseoftheirchemicalcompositions,
morphologiesandmechanicalproperties
15
.Somerigidinorganic
thepublicaswellasin fl uencingvisibility directand PMparticlesaremainlycapturedbyinterceptionandimpaction
1-7
indirectradiativeforcing, clima, andecosystems .PMisa le conviene ltersurface.SomesoftPMcontainingalotofcarbon
complexmixtureofextremelysmal particlesandliquid compoundsorwatersuchasthosefromcombustionexhaust
1,8
gotitas de .Onthebasisoftheparticlesize, PMiscategorized woulddeformon que ltersurfacesandrequirestrongerbinding
byPM 2,5 andPM 10 , whichrefertoparticlesizesbelow2.5and duringtheprocessofattachingtothe que lter.Itisimportantto
10 mm, respectively.PM 2,5 pollutionisparticularlyharmfulsince studythesurfacepropertiesoftheair que lterstoenhancePM
itcanpenetratehumanbronchiandlungsowingtothesmall particlecapture.However, inexistingair que ltertechnology, no
9
tama~no de las partıculas aumentos
.Hence, a largo termexposuretoPM 2,5 muchworkhasbeenperformedtostudythepropertiesof que ltro
10-14 15
morbidityandmortality .recently, therehavebeenserious materials.Therearetwotypesofair que ltersincommonuse .One
PMpollutionproblemsindevelopingcountrieswithalarge isaporousmembrane se filtro, whichissimilartoawater que la filtración
manufacturingindustrysuchasChina.Figure1a, bshowsimages se filtro (showninFig.1c) .Thistypeofair que lterismadebycreating
ofalocationinBeijingduringclearandhazydays, respectivamente. poresonsolidsubstrate, anditusuallyhasverysmallporesizeto
Duringhazydays, thevisibilitydecreasedgreatlyandtheair fi lteroutPMwithlargersizesandtheporosityofthistypeof filtro
.
qualitywaspoorbecauseofextremelyhighlevelsofPM 2.5
islow ( o30%). Por lo tanto, la fi ltrationef fi ciencyishigh, aunque

Measurestakenbythepublicduringhazydaysaremostly thepressuredropislarge.Anothertypeofair fi lterisa fi brousair


focusedonoutdoorindividualprotection, suchasusingmask filtro, whichcapturesPMparticlesbythecombinationofthick
15
filtros, whichareoftenbulkyandresistanttoair flujo .Inindoor physicalbarriersandadhesion (showninFig.1d) .Thistypeof
espacios protectionisonlyavailableinmoderncommercial fi lterusuallyhasporosities 470% andismadeofmanylayersof
buildingsthrough fi lteringinventilationsystemsorcentralair gruesa fi bresofdiversediametersfromseveralmicronstotensof
acondicionado; residentialhousingseldomhas fi ltrationprotection microns.Toobtainahighef fi ciencia, thistypeof fi lterisusually
fromPM.Moreover, alltheseactiveairexchangesbymechanical thick.Thede fi ciencyofthesecondtypeof fi lteristhebulkiness,
ventilationconsumeenormousamountsofenergybecauseofthe nontransparencyandthecompromisebetweenair fl owand filtro
16
massiveuseofpumpingsystems .Whenpeoplestayindoors e fi ciencia.

withoutsuf fi cientairexchange, indoorairqualityisalsoofgreat Existingtechnologywouldnotmeettherequirementsofa


preocupación 17 .Itwouldbeidealifpassiveairexchange-thatis, transparenthigh-ef ciencyPM fi fi lter.Herewedemonstratea
2,5
naturalventilation-throughwindowscouldbeusedforindoor novelpolymernano fi fi bra ltertechnology, whichhasattractive
ltration.Owingtothelargesurfaceareaofmostwindows fi aire, aire attributesofhigh fi lteringef fi ciencia, goodopticaltransparency,
exchangeisveryef fi cient.Protectionatwindowsrequirestheair lowresistancetoair fl owandlightweightasshowninFig.1e.We
fi lterstonotonlypossessahighPM-captureabilitybutalsoa foundthatwhenthesurfacechemistryoftheair fi lteris
highopticaltransparencyfornaturallightingfromthesunand optimizedtomatchthatofPMparticles, thatthesingle fi bra
vista-viewingatthesametime.Hereweintroducetheconceptof captureabilitybecomesmuchmorethantheexisting fibrosa
atransparentair fi lterforindoorair-qualityprotectionatthe fi lters.Therefore, thematerialuseintheair fi ltercanbereduced
windowforthe fi rsttime. signi fi cantlytoatransparentleveltoenablebothtransparencyto
ThePM 2,5 pollutionparticlesinairhavecomplicated sunlightandsuf fi cientair fl ow.Inaddition, cuandoel fi bra
, SO 2?
compositionsincludinginorganicmatter (suchasSiO 2 4 diameterisdecreasedtothenanometrescale, withthesame
?
Andno 3 ) Andorganicmatter (comoel, organiccarbonand packingdensity, theparticle-capturepossibilityisincreasedalot
elementalcarbon) fromdiversesourcesincludingsoildust, becauseoflargesurfacearea, whichalsoensureseffectivePM
vehicularemission, coalcombustion, secondaryaerosols, indus- capturewithamuchthinnerair fi lter.Thistransparent fi ltercan
1,18-21
trialemissionandbiomassburning .ThebehaviourofPM beappliedtoalltypesofsituationsincludingpersonalmasking

Flujo de aire
del flujo de aire de aire de flujo
Fuerte h?
superficie

de adherencia

pequeña abertura
200 nm
de exclusión por tamaño
gruesa
Micron tamaño

poroso filtro de aire de membrana comerciales filtrante fibrosa de aire del filtro de aire transparente

Figura 1 | Particulatematterpollutionandcomparisonamongdifferentair filtros. (a) PhotographofarandomplaceinBeijingduringasunnyday.


(b) PhotographofthesameplaceinBeijingduringahazydaywithhazardousPM 2,5 nivel. (c) Schematicsofporousair fi ltercapturingPMparticlesbysize
exclusión. ( d) Schematicsofbulky fi brousair fi ltercapturingPMparticlesbythickphysicalbarrierandadhesion. ( e) Schematicsoftransparentair
fi ltersthatcapturePMparticlesbystrongsurfaceadhesionandallowingahighlightandairpenetration.

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NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205 ARTÍCULO

andbuildingwindows.Bycontrollingthesurfacechemistryand thewindowscreenasasupportingandadheringsubstrate, theair


filtros microstructureoftheair fi, wereporttransparentultrathin fi lterismechanicallyrobust.Nano fi breswithdifferentsurface
fi ltersof B90% transparencywith eliminación 495,00%, de B60% propertiesaremadebychangingthefunctionalgroupsonthe
transparencywith 499,00% removaland B30% de transparencia polymersidechainsandalsobycoatingdifferentmaterialsusing
con 499,97% removalofPM 2,5 particlesunderextreme asputteringmethod.Thechosenpolymersareavailableinlarge
hazardousair-qualitycondition. quantityandatlowcost includingpolyacrylonitrile (PAN),
polivinilpirrolidona (PVP), poliestireno (PS), alcohol polivinílico
(PVA) andpolypropylene (PP) .Thecoatingmaterialsarecopper
Resultado andcarbon.PP, copperandcarbonareallcommonlyused
15 .
Transparentair fi ltersurfacescreening .Para fi ndthemost materialsincommercial fi filtros brousorporousmembraneair fi
effectivematerialfortransparentair fi filtros, differentpolymers Themolecularmodelsandformulaeofthedifferentpolymersare
andpolymerswithothercoatingswereinvestigatedforPM showninFig.2b.Thepolarityandhydrophobicityaredifferent
capture.Electrospinningwasusedtomakepolymernano fibrosa betweeneachpolymerandthedipolemomentsare3.6,2.3,0.7,
filtros de aire (showninFig.2a) .Electrospinninghasgreatadvantages 1.2and0.6DfortherepeatingunitsofPAN, PVP, PS, PVAand
inmakinguniform fibrosa fi ltersfromdiversepolymersolutions PP, respectivamente.
22-25 Inthisstudy, thePMisgeneratedbyburningincense.The
withcontrollabledimensions Thisversatilitymakes
?1
electrospinninganidealtooltoproduceatransparentnano fi bre burningincensecontainsPMabove45mgg quemado, yel
26,27 exhaustsmokecontainsavarietyofpollutantgases, incluyendo
red .Duringelectrospinning, ahighvoltageisappliedto
thetipofasyringecontainingapolymersolution; theresulting CO, CO 2 , NO 2
, SO 2 andalsovolatileorganiccompounds, comola
electricalforcepullsthepolymersolutionintoanano fi Breand benceno, tolueno, xilenos, aldehydesandpolycyclicaromatic
28
depositsthe fi breonagroundedcollector whichinthis hidrocarburos .Thiscomplexairexhaustisamodelsystem
experimentwasacommercialmetal-coatedwindowscreen containingmanyofthecomponentspresentinpollutedair
mesh.Owingtotheelectrical fi elddistribution, theelectrospun duringhazydays.Ascanningelectronmicroscope (SEM) se
polymernano fi breslieacrossthemeshholesandformnetwork fi rstusedtocharacterizedifferent fibrosa fi ltersbeforeandafter

forair fi ltration.Thiselectrospinningmethodisscalableandwith filtración TheimagesareshowninFig.2c, d.Theas-hechos

pantalla de la ventana con el metal recubrimiento

N O OH

n n n n n

V (3,6 D) (2,3 D) (0,7 D) (1,2 D) (0,6 D)

PAN PVP PS PVA PP

PAN antes de PVP antes de PS antes de PVA antes de PP antes de

PAN después de PVP después de PS Después de PVA después de PP después de

PM 2,5
PM
10-2.5
1,0

0,8

0,6

0,4

0,2
la eficiencia de eliminación de

0,0

PS PP
PANPVP PVA
Carbon
Copper

Figure2 | PerformanceofPM 2,5 capturebytransparentair lterswithdifferentsurfaces fi. (a) Schematicsshowingthefabricationoftransparentair filtro


byelectrospinning. ( b) MolecularmodelandformulaofdifferentpolymersincludingPAN, PVP, PS, PVAandPPwithcalculateddipolemomentsofthe
repeatingunitsofeachpolymer. ( c) SEMimagesofPAN, PVP, PS, PVAandPPtransparent fi ltersbefore filtración. ( d) SEMimagesofPAN, PVP, PS, PVA
andPPtransparent fi ltersafter fi ltrationshowingthePMattachment.Scalebarsin c, d, 5 mm. ( e ) Removalef fi ciencycomparisonbetweenPAN, PVP, PS,
PVA, PPcarbonandcoppertransparent fi lterswithsame fi brediameterof B200nmandsametransmittanceof B70% .Errorbarrepresentsthestandard
deviationofthreereplicatemeasurements. ( F) Demonstrationofusingtransparent fi ltertoshutoffPMfromtheoutdoor (rightbottle) fromenteringthe
cubierta medio ambiente (leftbottle).

3
NATURECOMMUNICATIONS | 6: 6205 | DOI: 10.1038 / ncomms7205 | www.nature.com/naturecommunications

y 2015MacmillanPublishersLimited.Allrightsreserved.
ARTÍCULO NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205

nano fi bre fi ltersofdifferentpolymershadsimilarmorphology captureef fi cienciesofdifferentpolymernano fibrosa fi lterswere


con fi bresizes B200nmandsimilarpackingdensity.SincePP assessedatdifferenttransmittancelevels, andtheresultsare
brescannotbemadebyelectrospinning fi, wepeeledthemoff showninFig.3b, c.Byincreasingthethicknessofthe fibroso de filtro,
fromcommercialmasktoatransmittanceof70% .ThePPthus thePM 2,5 fi captureef cienciesofPAN, PVPandPVA filtros
hasadifferentmorphology, con fi bresofmuchlargerdiameter aumentó (showninFig.3b, c) ltro .ForthePAN fi, excelentes
ascomparedwiththeelectrospunnano fi bres.TheSEMimagesof captureef fi ciencieswereachievedforavarietyofopticaltrans-
diferente fi ltersafterthe fi ltrationtestshowthatthenumberand mittancelevels: 495,00% removalat B90% transmittanceand
sizeofPMparticlescoatedonthePAN fi lterwerebothlarger 499,00% removalat B60% transmittanceforPM 2,5
captura.

thanthatofotherpolymers.ThesmokePMformedacoating Removalef fi cienciescategorizedbyparticlessizeareshownin


layerstronglywrappedaroundeachnano fi breinsteadofonly SupplementaryFig.4usingPANtransparent fi lterwithdifferent
attachingtothesurfaceofthenano fi bresasinthecaseof transmittance.A 495,00% ef fi ciencyofPM 2,5 capturebyPVP
inorganicPM (showninSupplementaryFig 1) sobreEl andPVA fi lterswasachievedatlowertransmittanceof B60and
commercialPPair filtros, thePMparticlescapturedcanhardly B30%, respectively.However, forPS fi bresusedinmanycom-
BeSeen. mercial fi filtros, increasingthe fi lterthicknessdoesnotimprovethe
Thequanti fi EDPM 2,5 andPM 10-2.5
removalbydifferent fibrosa PM 2,5 captureef fi ciencybymuch.Theremovalef fi ciencyof
fi ltersisshowninFig.2e.All fibrosa fi ltersareatthesame PM partículas (figura 3c) areallhigherthanthatofPM entodos
10-2.5 2,5

transmitancia ( B70%). Fromtheef fi ciencycomparison, SIIT fourpolymerair fi ltersandmostofthecasestheremovalef fi-


495,00% ef fi ciencystandard Todavía
shownthatthePANhasthehighestremovalofbothPM 2,5 y cienciesmeetthe PAN
PM 10-2.5 followedbyPVP, PVA, PS, PP, copperandcarbon.The showedthebestcaptureabilitythanotherpolymer fi lterswith
highlightedzone (95-100%) inFig.2emarksthestandardfora similartransmittance.
alto ef fi ciencia ficción lterandofthosetested, onlythetransparent Besidescaptureef fi ciencia, keepingahighair fl owisanother
PAN fi ltermeetsthisrequirement.Theremovalef fi cienciesare importantparametertoassesstheperformanceofanair fi lter.All
calculatedbycomparingthePMparticlenumberconcentration aire fl owtestswerebasedonPANair fi lterthatshowedthebest
withandwithoutair fi lters.ThesizedistributionofsourcePM performanceinPMcapture.InFig.3d, theairpenetration
wasshowninSupplementaryFig.2.Theresultsshowedthatthe throughPANtransparentair fi lterswasdemonstratedbywind
?1
polymercaptureef fi cienciesincreasewithincreasingdipole generatedbyafanatavelocityof3ms .APANtransparent
momentofthepolymer-repeatingunits suggestingthata aire fi lterwithtransmittanceof B90% wasplacedinfrontofa
dipoleorinduced-dipolo-dipoleforcecangreatlyenhancethe bundleofpapertasselshangingonastick.Whenwindwas
bindingofPMtothepolymersurface, andpolymerswithhigher blowingfromthefan, thepapertasselswereblownupwiththe
dipolemomentwouldhavebetterremovalef fi cienciesofPM Panair fi ltersinfrontofit whichdemonstratedgreat
particles.Withthesame fi ltertransmittance (packingdensity), penetrationofairthroughthetransparent fi lter.Quantitative
PANtransparent fi ltershowedthehighestremovalofbothPM 2.5 analysisoftheairpenetrationwascarriedoutbyinvestigatingthe
(98,11 ± 1,41%) andPM 10-2.5
(99,31 ± 0,08%) andonlyPAN pressuredrop ( DP) ofthetransparentPAN fi lterwithdifferent
transparente fi lterquali fi fi edthehigh-ef ciencystandardof 495% levelsoftransmittance.Figure3eshowstheschematicofthe
removal.ThismeansthatthesurfacepropertyofPANismuch pressuredropmeasurement.Thepressuredifferenceacrossthe
betterthanthatofPVP, PS, PVA, PP, carbonormetalsurface; aire fi lterwasmeasured.ItisshowninTable1thatataface
?1
Por lo tanto, itcanensureahighersingle fi brecaptureability.Inorganic velocityof0.21ms , thepressuredropsof85% and75%
PM 2,5 andPM 10-2.5 alsoshowedthatPANair fi lterwasmost transmittanceair fi ltersareonly133and206Pa, respectivamente.
effectiveincapturingPMparticles.ThesoftPMwithlarger Thispressuredropisonly o0.2% ofatmospherepressure, que
amountsofcarbonandwatercontenttendstobemoredif fi Cultto isnegligible.Theselevelsofpressuredroparesimilartothatofa
capturethanrigidinorganicPM, sincethecaptureef fi cienciesof blankwindowscreenwithoutnano fibras (131Pa) El DP

fibrosa fi ltersmadefromthesamematerialarelowerinsoftPM increaseswiththeincreasein fi lterthicknessorthedecreasein


captura (SupplementaryFig.1) .Besidessurfacechemistry, la transmittance.Theoverallperformanceoftheair fi lterconsider-
fi de filtro bredimensionalsoaffectsthePMremovalef fi ciencia ingbothef fi ciencyandpressuredropisassessedbyqualityfactor
signi fi cantlyasshowninSupplementaryFig.3.Asthe fi bre (QF showninTable1andSupplementaryTable1) La
diameterincreasedfrom B200nmto B1mm theremoval fi transparentPAN ltershowedhigherQFthanthefour
ef fi cienciesofPANair fi lterswiththesametransmittanceof70% filtros comerciales (SEMshowninSupplementaryFig.5) de
decreaseddramaticallyfrom98.11 ± 1,41% to48.21 ± 4,19% .A twofoldtoevenordersofmagnitudes.
demonstrationofusingatransparent fi ltertoblockPMpollution
wasshowninFig.2f.Intherightbottle, ahazardouslevelofPM
withPM índice massconcentration Insitu timeevolutionstudyofPMcapture .ThePMcapture
2.5 4300orPM 2,5
?3
4250mgm wasgeneratedandaPANtransparent fi lterwith processandmechanismwasstudiedby insitu opticalmicroscope
B70% transmittancewasplacedbetweenthePMsourceand (OM) andSEMusingaPANnano fibrosa fi lterwitha fi bre
anotherbottle.AsshowninFig.2f, theleftbottlewasstillclear Diameterof B200nm.ThePANnano fibrosa fi lterwasplaced
andthePM 2,5 concentrationwasinagoodlevelmarkedbythe undertheOM.Continuous fl owwithhighconcentrationof
índice (massconcentration ?3
PM 2.5 o15mgm ) .Thisdemon- smokePMwasfedtothe fibrosa fi lter.Thedynamicprocessis
strationshowstheexcellentef fi cacyofthePANtransparent filtro. shownintheSupplementaryMovie1.Figure4ashowsthePAN
fi bre fi lterbeforecapturingPM.InFig.4b-d, thetimesequence
(5,120and600s) ofPMcaptureisshown.Schematicsexplaining
Performanceoftransparentair filtro .Besidescaptureef fi ciencia, thePMcaptureatdifferentstagesareshowninFig.4e-h.Atthe
theothertwoimportantparametersforatransparentair filtro, initialcapturestage (figura 4b, f ), PMwascapturedbythePAN
lighttransmittanceandair flujo, werethenevaluated.Figure3a nano fi bresandboundtightlyonthenano fi bres.Asmoresmoke
showsthephotographsofthePANtransparentair fi lterswith wasfedcontinuouslytothe filtro, morePMparticleswere
transmittanceof B85, B75, B55, B30and B10% .Fortheair attached.TheparticleswereabletomovealongthePANnano-
fi lterswithtransmittanceabove50%, su fi cientlightcanpenetrate fi bresandaggregatetoformlargerparticlesandleftbehindsome
throughandenablelightingfromsunandsight-viewing.ThePM emptyspacesfornewPMparticlestoattach (shownin

4
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NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205 ARTÍCULO

, T-85 T-75 T-55 T-30 T-10

1,0 1,0

0.8 0,8

0,6 0.6

0,4 0.4
PM 2,5 PM
10-2.5
PAN
0,2 de eliminación 0,2 PAN de
eficiencia de la eficiencia de eliminación
PVP PVP
PS PS
0,0 PVA 0,0 PVA

0,0 0,2 0,4 0,6 0.8 1. 0. 0. 0.4 0. 0. 1,0

Transmitancia Transmitancia

filtro de aire

del flujo de aire de entrada de aire de flujo de salida

?P
No hay viento de viento en

Figura 3 | Transparencyandair fl owevaluationoftransparentair fi filtros. (a) PhotographsofPANtransparentair fi ltersatdifferenttransparency.


(b) PM 2,5 removalef fi cienciesofPAN, PVP, PS, PVAtransparent ltersatdifferenttransmittances fi. ( c) PM 10-2.5 removalef fi cienciesofPAN, PVP, PSand

PVAtransparent ltersatdifferenttransmittances.Errorbarrepresentsthestandarddeviationofthreereplicatemeasurements fi. ( d) Photographshowing


?1
thatthetransparent fi ltercanenableef fi cientairexchangedemonstratedbyanelectricfanatwindvelocityof3ms . (e) Schematicsshowingtheset-up
filtros forthemeasurementofpressuredropofair.

liketoenlargetheircontactareasandbindtightlytoensurean
Tabla 1 | Performancesummaryoftransparentair fi ltros
excellentcaptureperformance.
comparedwithcommercialair fi ltros.

T DP ?1 )
Muestra (%) E (%) (Pa QF (Pa
PMchemicalcompositionanalysis .Tofurtherexplaintheper-
PAN-8 8 96,1 13 0,024 formancedifferenceofdifferent fibrosa fi ltersincapturingsmoke
PAN-7 7 98,1 20 0,019
PM, thecompositionandsurfacechemistryofsmokePMwas
1 16,9 29
Comercial- 0.00062
investigated.Figure5ashowstheX-rayphotoelectronspectro-
Comercial- 6. 99,5 80 0,0068
scopy (XPS) characterizationofPM.XPSonlydetectedthesur-
E, PMremovalef fi ciencia; DP, pressuredrop; PAN, poliacrilonitrilo; QF, qualityfactor;
faceelementcomposition ( B5nmindepth) ofthesmokePM.It
T, transmitancia.
isshownthattheC1-ssignalcomprisesthreemajorpeaksat
QF¼? Ln (1? E%) / DP.
284.7,285.9and286.6eV, correspondingtoC-C, C-O y
C¼Obonds.TheO1- speakssupporttheresultsofC1-habla
andshowthepresentofC-OandC ¼Oat533.1and531.9eV,
SupplementaryMovie1) .Inaddition, theincomingnewPM respectively.Besidestheseelements, asmallproportionofNis
particlescouldattachdirectlytothePMthatwerealreadyonthe presentonthesurfaceofsmokeparticle, whichisshownatthe
PANnano fi bresandmergedtogether (showninFig.4fand peakof400.8eVofN1s.TheoverallresultsshowthatC, O y
SupplementaryMovie1) .Asthecapturekeptgoingon, thePAN NarethethreeelementspresentonsmokePMsurfaceandtheir
fi lterswere fi lledwithbigaggregatedPMparticles.Thejunction ratiois58.5%, 36,1% and5.4%, respectively.Thefunctional
ofnano fi breshadmorePMaccumulatedandformedspherical groupsareC-C C-O C ¼OandC-Nwitharatioof
particlesinbiggersizes. 4,8: 5,1: 1,3: 1.ThebulkcompositionofsmokePMwascharacter-
SEMwasusedtocharacterizethedetailedinteractionbetween izedbyFouriertransforminfraredspectroscopy (FTIR) yla
PMparticlesandPANnano fibras, andtheimagesareshownin spectraareshowninFig.5b.Themainpeaksareat B3,311,
?1
Fig.4i, j.ThegeneralcapturemechanismofsoftPMparticleis 2,291,1,757,1,643,1,386,1,238,1,118and1,076cm , que
thatafterbeingincontactwiththePANnano fi bra, thePM indicatedtheexistenceofO-H, C-H, C ¼O, C ¼C, C-NandC- O
particlewouldwraparoundthenano fi brestightly (Fig.4i), (lastthreepeaks) functionalgroups.Inaddition, dis- energía
deformand fi nallyreachtoastablesphericalshapeonthe persiveX-rayspectroscopy (EDX) characterizationshowedsame
nano fi bre.ThiswrappedaroundcoatingindicatesthatthePM compositionofC NandOinPMparticles (shownin
particlesfavourthesurfaceofPANnano fi bressothattheywould SupplementaryFig.6) .TheXPS, FTIRandEDXanalysesshow

5
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ARTÍCULO NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205

Combinar para PM existente

Asociar al nanofibras

PM funden

Figure4 | Insitu timeevolutionstudyofPMcapturebyPANtransparent filtro. (a-d) Insitu studyofPMcapturebyPANnano brecharacterizedbyOM fi


mostrando ltermorphologiesatdifferenttimesequencesduringacontinuousfeed.Scalebars fi, 20 mm.Thetimescalesfor ( a-d) is0,5,120and600s,
respectivamente. (e-h) SchematicsshowingthemechanismofPMcapturebynano fibrosa fi lteratdifferenttimesequences. ( i) SEMimageshowingthe
detailedmorphologiesofattachedsoftPMthatformedacoatinglayerwrappingaroundthePANnano fi bre.Scalebar, 1 mm. (j) SEMimageshowingthatthe
nano fi brejunctionhasmorePMaggregatedtoformbiggerparticles.Scalebar, 1 mm.

consistentresultsofthesmokecompositionthatcontainsmostly aremostlypresentontheoutersurfaceofPMaccompaniedby
organiccarbonwithfunctionalgroupsofdifferentpolaritiessuch somenonpolarfunctionalgroupsuchasalkanes (shownin
asalkanes, aldehydeandsoon.Thefunctionalgroupsofhigh Fig.5j) .Thisisconsistentwiththeresultthatpolymerair fi filtros
polaridades, suchasC-O, C ¼OandC-N, aremainlydistributed deficiencias withhigherdipolemomentshavehigherPMcaptureef fi.
ontheoutersurfaceoftheparticles.Tofurtherdemonstratethe BecausethepolarfunctionalgroupssuchasC-O, C ¼Oand
functionalgroupdistributionsacrossthePMparticle, transmi- C-NwerepresentattheoutersurfaceofthePMparticles,
sionelectronmicroscopy (TEM) andelectronenergylossspec- polymerswithhigherdipolemomentcanhavestrongerdipole-
troscopy (EELS) areusedtocharacterizethesmokePMcaptured dipoleandinduced-dipoleintermolecularforcessothatthePM
onPAN fi bre.Figure5cshowsthemorphologiesofPMattached captureef fi ciencyishigher.
tothePAN fi bres.ThePMparticleshaveastickyamorphous
carbono-likemorphologywiththecorescontainingsomecon-
densedsolids, whiletheoutersurfacescontaininglightorganic PANtransparentair fi lterlong-termperformance .Thelong-
matters.EELSwasusedtomeasuretheenergylossacrossthePM termperformanceofthetransparent fi lterwasevaluatedusinga
attachedtoPAN fi bra (Fig.5d, e) andbarePAN fi bra (Fig.5d, f). PAN fi lterwithatransmittanceof B75% undertheconditionof
TheresultshowsthatatthePMparticle, thechemicalcontents hazardouslevelequivalenttothePM 2.5
índice 4300andamild
changewithposition.Byscanningthebeamfromoneendofthe windcondition ( o1milesperhour) .Theperformanceisshown
PMtotheotherend, thepeaksoftheCKedge (284eV), thenk inFig.6a.After100h, thePAN fi lterstillmaintainedahigh
borde (401eV) andtheOKedge (532eV) fueron fi rstshownatthe PM 2,5 andPM 10-2.5 removalef fi ciencyof95-100% and100%,
outersurfaceofthePM (showninFig.5g) .Asthebeammovedto respectivamente, andthepressuredroponlyincreasedslightlyfrom
thecentreofthePM, theNKedgeandOKedgesignals B2toB5Pa TheSEMimagesinFig 6b, cshowedthe
diminishedandonlytheCsignalwaspresent (showninFig.5h). morphologiesofPANnano fibrosa fi lterafter100-htest.ThePM
Atlast, asthepositionmovedtotheoutersurfaceagain, thenk particlescapturedwereaggregatedandformeddomainsofvery
borde (401eV) andOKedge (532eV) peaksshowedupagain.As largeparticlesof20 -50 mm.NodetachmentofPMwasnoticed
control, theEELSsignalofthePAN fi breshowedthesamesignal afterusingcleanairtoblowthroughtheusedPAN fi lterby
allacrossthewhole fi brewithCKedge (284eV) andNKedge measuringthemassloss (within0.006% oferrorbar) .Aseparate
(401eV), whichmatchesthechemicalcompositionofthePAN PMadsorptiontesthasshownthatthePANtransparent filtro
polímero (showninFig.5i) .Thisindicatesagainthatthepolar achievedacaptureofPMpollutants10timesofthemasstothe
functionalgroupsthatcontainOandN (C-O, C ¼OandC-N) fi lter'sself-weight.This10 ? capabilityimpliesthatthelifetime

6
NATURECOMMUNICATIONS | 6: 6205 | DOI: 10.1038 / ncomms7205 | www.nature.com/naturecommunications

y 2015MacmillanPublishersLimited.Allrightsreserved.
NATURECOMMUNICATIONS | DOI: 10.1038 / ncomms7205 ARTÍCULO

C1 O 1s

C-C

C-O
C-O

Intensidad (au) C = O Intensidad (au)


C=O

296 29228828428 540536532528524


la energía de unión (eV) energía de enlace (eV)

f
N 1s Composición (%) e

CON
58. 36. 5.4

C-N Proporción

Intensidad (au) C-CC-OC = OC = N


4. 5. 1. 1

408 404 400 396 392


energía de enlace (eV)

1,0

0,9 Counts Counts

0.8 1,2 0,4


OH
C-O
300 0,8 μ m) μ m)
300 0,2
C=C 500 0,4 500
C-O 700
pérdida de energía (eV) 0 La pérdida de energía (eV)
Transmitancia
CH 700 0
0,7 OC= Posición ( Posición (
, C-N C-O

0,6

Borde CK borde C K borde C K


4,0003,5003,000 2 , 5002,0001,500 1.000

-1 )
Número de onda (cm
N borde K borde N K

Cuenta los recuentos recuentos


C=O O K borde

, C-C

C-H
C-O
C=C
30 50 70 300 500 700 300 500 700
, C-N pérdida de energía (eV pérdida de energía (eV) La pérdida de energía (eV)

Figura5 | SmokePMcompositionanalysis. (a) XPScharacterizationofPMparticleshowingtheC1s, O1sandN1speakanalysisandcompositionratio.


(b) FTIRcharacterizationofPMparticleshowingtheexistingfunctionalgroups (. c) TEMimagesshowingthemorphologiesofPMparticlescapturedon
PAN fi lter.Scalebar, izquierda, 0,5 mm; derecha, 1,5 . mm ( d) TEMimageofthePMparticlecapturedonPANnano fi breusedforEELSanalysis.Scarbar, 1 mm.

(e, f) EELSdataofposition ( e) y ( f.) correspondingtoPMparticleandPAN fi bra ( g-i) ExtractedEELSdataondifferentpositions :( g) surfaceofPM


partículas; (h) bulkofPMparticleand ( i) PAN fi bra (. j) SchematicshowingPMparticlecompositionswithnonpolarfunctionalgroups (C-C, C-HandC ¼C )

insideandpolarfunctionalgroups (C ¼O, C-OandC-N) fuera.

fi ofatransparent lterwiththetransmittanceof B75% era respectively.Inaddition, commercialmaskscommercial-1 y


expectedtobeabove300hunderthehazardousPMlevel (PM fi bras-2withPP comerciales (imagesshowninSupplementary
índice 4300). Fig.5) weretestedforcomparison.Commercial-1showedmuch
lowerPM 2,5 andPM 10-2.5 removalof70.40% and94.66%,
respectivamente Comercial-2showedcomparableremoval
Performanceofthetransparentair fi ltersina fi eldtest .En
ef fi cienciesofPM 2,5 (99,13%) andPM 10-2.5 (99,78%), aunque
ordertostudytheef fi cacyofour fi ltersinarealpollutedair
itisessentiallynottransparent (transmittance6%). Por lo tanto, PAN
medio ambiente, wecarriedouta fi eldteston3July2014inBeijing,
29 filtro showedthebestperformanceasatransparent fi.
China.Onthebasisofarecentstudy , thePM 2,5 inBeijinghas
40,7% oforganicmatters, whichissimilartoourexperimental
condición ThePM 2,5 concentrationonthatdaywasata Performanceunderdifferenthumidityandwindforce .Onthe
hazardouslevelequivalenttoaPM 2.5
índice 4300.Theresults basisoftherealweathersituation, windforceandhumiditywere
areshowninFig.6d, e.PAN fi lterswithtransmittance B77%, alsotakenintoconsiderationandtheresultsareshownin
B54%, B40% achievedPM 2,5 andPM removalef deficiencias SupplementaryFigs7and8.ThePAN fibrosa fi lterwiththe
10-2.5
of98.69% 99,42% 99,88% and99.73% 99,76% 99,92%, transmittanceof B73% wastestedatdifferentwindforce
?1 ?1
respectively.Forcomparison, aPS filtro, whichshowedlower representingcalm (0.21ms ), lightbreeze (3.12ms ), suave
?1 ? 1 ) conditions.The
removalofsmokePM, consistentlyshowedlowerremovalof brisa (5.25ms ) (andfreshwind 10.5ms
PM 2,5 andPM 10-2.5
enla fi eldtest, of76.61%, 73,50 %, 96,76% removalef fi cienciesunderallcaseswere 496,00% andshowed
and95.91%, 95,17%, 99,44% attransmittanceof71%, 61%, 41%, anincreasingtrendofremovalef ciencytowindvelocity fi, que

7
NATURECOMMUNICATIONS | 6: 6205 | DOI: 10.1038 / ncomms7205 | www.nature.com/naturecommunications

y 2015MacmillanPublishersLimited.Allrightsreserved.
ARTICLE NATURECOMMUNICATIONS|DOI:10.1038/ncomms7205

fi transparente lters.Webelievethatourtransparentair fi ltercan


1.0
beusedasastand-alonedeviceorincorporatedwithexisting
0.8 masksorHEPA fi lterstoachieveahealthierindoorliving
medio ambiente.
0.6

0.4
Métodos
PM 2.5 Electrohilado. Thesolutionsystemforthepolymersusedinthisworkis6wt%
0.2
Removal efficiency ¼1.5? 10
5
gmol
?1
, Sigma-Aldrich) indimethylformamide (EMD
PM 10–2.5
PAN (MW
6 ?1
0.0 Millipore), 7% en peso de polivinilpirrolidona (MW ¼1.3? 10 gmol , Acros) en
4 ?1 ,
etanol (FisherScienti fi c),% 10 en peso alcohol polivinílico (MW ¼9.5? 10 gmol
0 2 4 6 8 100 5
Sigma-Aldrich) indistilledwaterand6wt% de poliestireno (MW ¼2.8? 10
Time (h) gmol
?1
, Sigma-Aldrich) indimethylformamidetogetherwith0.1wt% ofmyr-
istyltrimethylammoniumbromide (Acros) .Thepolymersolutionwasloadedina
1-mlsyringewitha22-gaugeneedletip, whichisconnectedtoavoltagesupply
(ES30P-5W, GammaHighVoltageResearch) .Thesolutionwaspumpedoutofthe
needletipusingasyringepump (KDScienti fi c) .La fi breglasswiremesh (New
YorkWire) wassputter recubierto (AJAInternational) con B150nmofcopperon
bothsidesandwasgroundedtocollecttheelectrospunnano fi bres.Thewiredia-
meterwas0.011inch, andthemeshsizewas18 ? 16.Theelectrospunnano fi bras
wouldlieacrossthemeshholetoformtheair filtro, similartoprevious
informes 26,27,30 .Theappliedpotential, thepumprate, theelectrospinningduration
andtheneedle-collectordistancewerecarefullyadjustedtocontrolthenano fi bra
diameterandthepackingdensity.
1.0 1.0

0.8 0.8 .
Opticaltransmittancemeasurement Thetransmittancemeasurementuseda

0.6 xenonlamp (69911, Newport) asthelightsource, coupledwithamonochromator


0.6
PM (74125, Newport) tocontrolthewavelength.Aniriswasusedtotrimthebeamsize
PM 2.5 10–2.5
0.4 0.4 a B5mm? 5mmbeforeenteringanintegratingsphere (Newport) fortrans-
PAN PAN
mittancemeasurement.Aphotodetector (70356, Newport) wasinsertedintooneof
0.2 PS 0.2 PS
Commercial-1
Removal efficiency Removal efficiency
Commercial-1 theportsofintegratingsphere.Thephotodiodeisconnectedtolock-inradiometry
Commercial-2 Commercial-2
0.0 0.0 sistema (70100Merlin, Newport) forphotocurrentmeasurement.Thesampleswere

0.0 0.2 0.4 1. 0.4 1.0 placedinfrontoftheintegratingsphere; por lo tanto, bothspeculartransmittanceand


0.60.8 0.00.2 0.60.8
diffusetransmittancewereincluded.Forair fi lterscoatedoncopperwiremesh, una
Transmittanc Transmittance
cleancopperwiremeshwiththesamegeometrywasusedasareference.Forself-
Figure6|PANtransparentfilterlong-termperformanceandfieldtest de pie filtros, ambientairwasusedforreference.Thetransmittancespectrum
wasthenweightedbyAM1.5solarspectrumfrom400to800nmtoobtainthe
(Beijing)performance. (a)Thelong-termPM 2.5 andPM 10–2.5 removal
averagetransmittance.
efficienciesbyPANtransparentfilterof70%transmittanceunder
continuoushazardouslevelofPMpollution.( b,c)SEMshowingthePAN .
PMgenerationandef fi ciencymeasurement Forallperformancetestsunless
transparentairfiltermorphologyafter100-hPMcapturetest.Scalebars,
mentionedotherwise, modelPMparticlesweregeneratedfromincensesmokeby
50and10 mm,respectively.( d,e)ThePM 2.5 andPM 10–2.5 removal burning.ThesmokePMparticleshaveawidesizedistributionfrom o300nmto
efficienciesofPANandPStransparentfilterswithdifferenttransmittance 410mm, withthemajorityofparticlesbeing o1mm.Thein fl owconcentration

comparedwithcommercial-1andcommercial-2mask.Testswere wascontrolledbydilutingthesmokePMbyairtoahazardouspollutionlevel
equivalenttothePM de índice 4300.PMparticlenumberconcentrationwas
2,5
performedinBeijingon3July2014underair-qualityconditionofPM 2.5
detectedwithandwithout fi ltersbyaparticlecounter (CEM) andtheremoval
index 4300.Errorbarrepresentsthestandarddeviationofthreereplicate ef fi ciencywascalculatedbycomparingthenumberconcentrationbeforeandafter
measurements. fi ltration.IntherigidPMcapturetest, dustPMparticleswerefabricatedby
grindingsoilparticlesusingaballmilltosubmicronsizes.Thepressuredropwas
couldbeduetotheincreaseinPMparticlerejection.Thisis measuredbyadifferentialpressuregauge (EM201B, UEitestinstrument) .Unless
15 ?1
consistentwithotherstudies mencionado, thewindvelocityusedintheef ciencytestwas0.21ms fi yla
.ForPMcaptureunderextreme
humiditywas30%.
humidconditions (45% humidityand30% de humedad), theresults
showedthathumidityhelpsPANandPSwiththetransmittance
Caracterización. TheSEMimagesandEDXweretakenbyFEIXL30SirionSEM
de B70% toachievebetterPMcapture, especiallyforPSthat
withanaccelerationvoltageof5kVforimagingand15kVforEDXcollection.The
increasedfrom37.08to95.59% .Thisisbecausetheambient
TEMimagesandEELSdatawerecollectedwithanFEITitanTEMwiththe
watercontentincreasedthecapillaryforcebetweenthePM accelerationvoltageof300kV.TheXPSspectrumwascollectedusingthePHI
particlesandPSnano fi bresduringPMattachment.However, por VersaProbeScanningXPSMicroprobewithanAlK asource.TheFTIRspectrum

PVPandPVA, becauseoftheirsolubilityinwater, underextreme wasmeasuredusingtheBrukerVertex70FTIRspectrometer.

humidconditions, la fi ltersweredamagedsigni fi cantlyresulting


innodetectableremoval.Stillunderhumidcondition, PAN References
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