A Step-by-Step Process-Induced Unidirectional Oriented Water Wire in the Nanotube - Jin et al. - 2021 - Unknown

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pubs.acs.org/JPCLLetterAStep-by-StepProcess-InducedUnidirectionalOrientedWaterWireintheNanotubeLeJin,DepengZhang,YuZhu,XinruiYang,YiGao,andZhigangWang*CiteThis:J.Phys.Chem.Lett.2021,12,350−354ReadOnlineACCESSMetrics&MoreArticleRecommendations*sıSupportingInformationABSTRACT:Theorientationofwatermoleculesisakeyrequirementforthefasttransportofwaterinnanotubes.Ithasbeenacceptedthattheflipofthewaterchainfollowsaconcertedmechanism,whichhasledtotheviewthatbidirectionalwaterfluxinnanotubescanbetransformedintounidirectionaltransportwhentheorientationofwatermoleculesismaintainedinlongnanotubesundertheexternalfield.InthisLetter,onthebasisofmoleculardynamicssimulationsandfirst-principlescalculations,weconfirmedthattheflipofthewaterchainisastep-by-stepprocess,whichisdifferentfromtheperceivedconcertedmechanism.Furtheranalysisindicatedthatwithoutanexternalfield,itneededmorethan20watermoleculestomaintaintheunidirectionalsingle-filewaterflowinacarbonnanotubeatadurationtimeofseconds.Consideringthatthethicknessofthecellmembrane(normally5−10nm)islargerthanthelengththresholdoftheunidirectionalwaterwire,thisstudysuggestedthatitmaynotrequiretheexternalfieldtomaintaintheunidirectionalflowinthewaterchannelatthemacroscopictimescale.heorientationofconfinedwatermoleculesiscrucialforunidirectionalwaterflowwasmuchshorterthanpreviouslyT1−3thefasttransportofwaterinchannels.Sincetheperceived.Moreimportant,consideringthatthethicknessofdiscoveryofwaterfluxinthincarbonnanotubesin2001,cellmembrane(normally5−10nm)waslargerthanthelengthextensivestudieshavebeendevotedtoextraordinarywaterthresholdoftheunidirectionalwaterwire,itispossiblethatbehaviorsinconfinedspacesfortheirpotentialapplicationsinspontaneouswaterflowmayexistinthewaterchannelatthe1,4−10theartificialwaterchannelanddesalination.Usingmacroscopictimescale.carbonnanotubesasthedistinctmodelsystems,manyfactorsTostudytheflippingprocessofawaterchainunderhavebeenidentifiedthatinfluencewatertransportinsmallconfinement,wefirstperformedmoleculardynamics(MD)channels,suchasthedefectofwaterwiresandthediameterofsimulationsusingonetosevenH2Omoleculesin(6,6)CNT.11−13nanotubes.Atpresent,itiswellacceptedthatwithouttheWeusedtwo,three,andfourH2Omoleculesastheexampleexternalfield,bidirectionalwaterfluxexistsinshortnanotubes(othercasesaregivenintheSupportingInformation).TheDownloadedviaUNIVOFCALIFORNIASANTABARBARAonMay16,2021at11:38:57(UTC).Seehttps://pubs.acs.org/sharingguidelinesforoptionsonhowtolegitimatelysharepublishedarticles.becauseofthefastandconcertedflipoftheorientationofthewatermoleculesintheCNTformedtheone-dimensional(1D)1waterchain.Torealizetheunidirectionalflowforpracticalchain(Figure1a).Weusedtheanglebetweenthedipoleandapplications,anumberofintricatestrategieshavebeentheplaneperpendiculartotheaxisoftheCNTtodetermine14−16proposed,includinganinducedexternalchargeorforce.theorientationofthewatermolecules(Figure1b).Figure1cDespitesignificantprogress,ourfundamentalunderstandingofshowstheevolutionofdipolestrengthwiththesimulationtimetheflipofhydrogenbondsofconfinedwaterisstilllimitedforthewaterchain.Forallthesystems,thedipoleorientationsbecauseofthelackofstudiesattheatomiclevel.flippedfrequently.TheaveragetimebetweentheflippingInthisLetter,bycombiningtheclassicalsimulationsandintervalsofthewaterchainwasabout0.8psfordimer,6.0psfirst-principlescalculations,wedemonstratedthattheflipoffortrimer,21psfortetramer,69psforpentamer,385psforhydrogenbondsforasingle-filewaterchainwithincarbonnanotubeisastep-by-stepprocess.ThepersistenttimeofthedipolealignmentforthewaterchainwasexponentialtotheReceived:November8,2020numberofthewatermolecules.Inparticular,ittookmorethanAccepted:December15,202020watermoleculestomaintaintheorientationofwaterchainPublished:December23,2020atadurationtimeofseconds.Astheunidirectionalorientationofwaterchainwasaprerequisiteforunidirectionalwaterflow,thisstudysuggestedthatthelengthofthechannelfor©2020AmericanChemicalSocietyhttps://dx.doi.org/10.1021/acs.jpclett.0c03340350J.Phys.Chem.Lett.2021,12,350−354

1TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure1.Effectofthenumberofwatermoleculesonpersistenttimeofdipolealignmentforwaterchains.(a)Modelofconfinedwaterchain.(b)Definitionofmoleculardipoleangleinwaterchains.(c)Changeofthedipolemomentwiththetimeintypicaldynamicsprocesses.Thiswaterchainconsistsoftwotosevenwatermolecules.μ0representsthedipolemomentofonewatermolecule.(d)Relationshipbetweenthelifetimeoftheorientationoftheaxialdipolemomentsandthenumberofwatermolecules.Thecoefficientaandtheconstantbare0.64and1.63foroursimulations,respectively.Nisthenumberofwatermolecules.SolidsquarepointsarethedataobtainedbyMDsimulations.Thelineisobtainedbyfittingtheformer.Itcanbeexpressedasthefunctionshowninthefigure.Thedashedpartofthelinerepresentstheextrapolationbasedonthefittedrelationship.103,106,109,1012,and1015representpicosecond(ps),nanosecond(ns),microsecond(μs),millisecond(ms),andsecond(s),respectively.∼denotesmagnitude.Figure2.Snapshotsoftrajectoriesforthetypicalmolecularorientationofwaterchains.(a)Changeofdipoleangleforeachwatermoleculeinthedifferentchain.Differentcolorsindicatethedifferentnumberofwatermolecules.(b)Flippingprocessofwatertetramerchain.(c)Comparisonoftherotationtimeofeachwatermoleculeforthetetramerchain.hexamer,and926psforheptamer.Itwasevidentthatanrelationship,whenthenumberofwatermoleculeswasincreaseinthenumberofwatermoleculesslowedthedipoleextrapolatedto12,16,andmorethan20,thedurationtimeflipsofthewaterchain,andthedurationtimeforeachrequiredtomaintainthedirectionofaxialdipolecouldreachdirectionbecamesignificantlylonger.Todescribethelifetimemicrosecond(μs),millisecond(ms),andsecond(s),ofthedirectionoftheaxialdipole,theaveragedurationtimerespectively.(t)couldbeexpressedusinganexponentialequationfittedasTobetterunderstandtheunderlyingflippingmechanismofLog(t)=a×N+b(asshowninFigure1d).Accordingtothisthewaterchaininthenanotube,snapshotsoftrajectoriesfor351https://dx.doi.org/10.1021/acs.jpclett.0c03340J.Phys.Chem.Lett.2021,12,350−354

2TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterFigure3.Potentialenergysurfaces(PESs)andthereactionratesofflippingprocessesforwaterchainsthatconsistofdimer,trimer,andtetramer.(a−c)PESsofthewaterchains.Thestructuresinthedottedframecorrespondtothetransitionstates(TSs)orintermediates(Ints).(d)Relationshipbetweenthereactionratesandthetemperature.AllvalueswerecalculatedwiththetransitionstatetheorywithEckartTunneling19,20corrections(TST-Eckart)theoryusingtheKiSThelPprogram.Valuesofthesereactionratescorrespondingto300Kalsoaremarked.Theyellow,red,andbluelinesrepresentthereactionratesofdimer,trimer,andtetramerinCNT,respectively.thetypicalorientationofwatermoleculesareshowninFigurefourH2Omoleculesin(6,6)CNTasthemodelsystems,we2.InFigure2a,theanglesfluctuatewithinthedurationtime.analyzedthepotentialenergysurfaces.AsshowninFigure3,WhenthenumberofH2Omoleculesincreased,thefluctuationtheflippingprocessofthewaterchaingeneratedaseriesof11timeofthemoleculesincreased.Thesefluctuationsnormallydefectivestructures,whichweconsideredtobethecorrespondedtotheflipsofthemolecules,whichdidnotintermediatesofthereactionpath.Theformationoftriggereasilytheflipofthewaterchain.Wealsofoundthattheintermediateswasanessentialstepinthewaterchainflippingflipofwatermoleculesdidnotoccursimultaneously(seeinsetprocess.Thisfindingwassignificantlydifferentfrompreviously8,17ofFigure2a).Theflipofthewaterchainwasastep-by-stepconsidereddefectivestructures.processratherthanaconcertedprocessasperceivedinRemarkably,therewasonlyonetransitionstate(TS)andnopreviousliterature.Theflippingprocessofthetetramerchainintermediateforthewaterdimerchain.ForthewatertrimerinFigure2bclearlyshowstheone-by-oneflipofthewaterchain,thereweretwoTSsandoneintermediate.Whenthemoleculefromoneendtotheotherend.Moreover,asshownnumberofwatermoleculeswasfour,thenumberofTSsandinFigure2c,theaveragerotationtimeforendH2Omoleculesintermediatesincreasedtothreeandtwo,respectively.Thetakesonlyfewpicoseconds,butthatforthemiddleH2OnumberofTSsandintermediatesincreasedwithanincreaseinmoleculetookuptotensofpicoseconds.Thisdemonstratedthenumberofwatermolecules.ItisreasonabletoinferthatthatthewatermoleculesatbothendsofthechainrotatedthenumberofTSsandintermediateswouldbeN−1andN−moreeasilythanthatoftheinternalwatermolecules.To2,ifthenumberofwatermoleculeswasN.Thatistosay,whenconfirmtheprocess,thesnapshotsofthetrajectoriesforwaterthenumberofwatermoleculesexceededtwo,theflippingpentamerchainwerealsoanalyzed,whichwasconsistentwithprocesswasaccompaniednotonlybythedipoleflip,thethefeatureofthewatertetramerchain(seeFigureS1forbreakingandgeneratingofH-bonds,andtheconversionof18details).Meanwhile,thedynamicpropertiesofwaterchainindonorandacceptorrolesbetweenmolecules,butalsobythechiralCNTswereanalyzed(FigureS2).Itwasfoundthattheformationanddisappearanceofintermediates.Inaddition,averagetimebetweentheflippingintervalsofwaterchainsnotduringtheflippingprocessesofthewatertetramerchain,theonlydecreaseswiththeincreaseofCNTsdiameter,butalsoislengthsoftheO−HbondsthatdidnotparticipateintherelatedtothechiralityoftheCNT.Further,wealsoexplorebreakingandgeneratingofH-bondswere1.00−1.02Å.theflippingprocessofthe“heavy”-waterchainin(6,6)CNTHowever,thelengthsoftheO−HbondsparticipatedinH-(FigureS4).Thewatermoleculesatbothendsofthechainbondscanreach1.07Å.TheformationofH-bondstretchedrotatedmoreeasilythanthatoftheinternalwatermolecules,thecorrespondingO−Hbond,andthemagnitudeofthewhichisconsistentwiththatofthe“light”-waterchain,andthechangeswere10−2Å.Thisbondpropertyisalsoappliedtotheaveragetimebetweentheflippingintervalsofthe“heavy”-waterdimerandtrimerchain(seeFigureS5fordetails).waterchainislargerthanthatofthe“light”-waterchain,whichInaddition,notethattheenergybarriertobeovercomewasiscausedbythedeuteriumatomhavingoneneutronmorecloselyrelatedtothenumberofwatermolecules.Asshowninthanhydrogenatom.Figure3,forthewatertrimer,theenergybarrierwasaboutTorevealthephysicalflippingmechanismofthewater0.64eV.Thiswasabout0.33eVhigherthanthatofthewaterchain,weperformedfirst-principlescalculations.Usingtwotodimerchain.Forthetetramerwaterchain,itwasatleast0.5eV352https://dx.doi.org/10.1021/acs.jpclett.0c03340J.Phys.Chem.Lett.2021,12,350−354

3TheJournalofPhysicalChemistryLetterspubs.acs.org/JPCLLetterhigherthanthatoftwowatermolecules.Itwasclearthatthemolecules,seeFiguresS6andS7.Thisanalysisshowedthatelongationofthewaterchainrestrainedtherotationofthethedefectivestructureswerethestableintermediates,whichwatermolecules,especiallyforthoseinthemiddleofthewaterretardedthestepwiseflipofthewaterchaininCNTandchain.Weattributedthisresulttotheenhanceddipolepreferredtheretentionoftheoriginalorientationofthemomentswiththeincreasednumberofwatermoleculesdipoles.(Figure1).Inaddition,wealsoobservedthattherotationofInthispaper,ourworkproposedastep-by-stepflippingtheendmoleculetendedtoflipbacktotheinitialstructuremodelofconfinedwaterchains,whichresultedintheabilityofratherthantosimplyinducetherotationofthenextH2Oasingle-filewaterchaintoretainitsoriginalorientationforamolecule(using(H2O)4astheexample),becausethefirstlongtimeinshortCNTs.Weconsideredthedefectiveintermediate(Int1)hadamuchlowerbackwardbarrier(0.15structuresinthewaterchaintobestableintermediatesduringeV)toTScomparedwiththeforwardbarrier(0.42eV)tothetheflippingprocess,whichwerenecessarypathwaysforwatersecondintermediate(Int2).Thisfurtherdemonstratedthatthechainflipratherthanaccidental.Thestepwiseflipofthewaterflipofthewaterchainwasastep-by-stepprocess,whichmeantmoleculesinthesingle-filewaterchaincontradictsthepreviousthatthedifficultyofthewaterchainflippingprocessiscausedpresumptionoftheconcertedmechanism,whichinducedtheprimarilybytheinteractionbetweenwatermolecules.Thisunexpectedmaintenanceoftheunidirectionalorientationofprovidedfavorablesupportforthespontaneoustransportofthewaterchain.Consideringthattheunidirectionalwaterchain.orientationofthewatermoleculesistheprerequisitefortheTofurtherunderstandthedifficultyofwaterchainflipping,unidirectionalwaterflowandthewaterchannelsofthecellwecalculatedthereactionratesfortheflippingprocessesbasedmembranenormallywerelongerthan5nm,ourdiscoveryonthetransitionstatetheorywithEckartTunnelingindicatedthatthetransmembranewaterchannelmight19,20corrections(TST-Eckart).TheequationpresentedformaintainunidirectionalwaterflowatthemacroscopictimetheTST-Eckartisasfollows:scalewithoutanexternalfield.TST/TTSTv()TTv=×χ()()T■COMPUTATIONALMETHODSTSTkTbRTΔn−ΔGTk≠,0()/TWeperformedmoleculardynamicssimulationsatthetemper-wherev()T=σeb,andχ(T)istheh()P0atureof300KusingtheGromacsprogram.21Wesetthetransmissioncoefficient.Figure3dgivestherelationshipensembleandthermostatasNVTandBerendsen,respectively.betweenthereactionratesandthetemperature.ConsideringTheconfinedsystemwasunderperiodicboundaryconditions300Kasanexample,thereactionratesofthewaterchainswithaboxsizeof25Å×25Å×39.352Å.Weemployedaconsistingoftwo,three,andfourwatermoleculesis6.97×107TransferableIntermolecularPotentialwith3Points(TIP3P)s−1,3.03×103s−1,and1.46×101s−1,respectively.Withan22watermodeltoformthewaterchainintheCNT.Theincreaseinthenumberofwatermolecules,thereactionratecarbonatomsofCNTweremodeledasunchargedLennard-decreased,makingitmoredifficulttoflipthewaterchain.JonesparticlestoensureonlythevanderWaalseffectontheFigure4showsthedetailedflippingprocessofwaterwater.Atime-stepof1fswasused,anddatawerecollectedtetramer.ThisexampleshowsthechangeintheH-bondevery1fs.Thetimeforthesimulationwas105nsforeachprocessandthelast100nsofsimulationwerecollectedforanalysis.Forfirst-principlescalculations,wecarriedouttheempirical-dispersion-correctedhybridPerdew−Burke−Ernzerhof(PBE0-D3)methodofdensityfunctionaltheoryusingthe23−25Gaussian09package.Weusedthebasissets6-311+G(d,p)and6-31G(d)forwaterandCNT,respectively.Thediameterandlengthofthearmchairtypesingle-walledFigure4.FlippingprocessforthewatertetramerchaininCNT.(6,6)CNTsimulationwere8.20and20Å,respectively.IncalculationsexceptfortheCNTpreoptimization,wefrozeallorientationduringthewaterchainflips.ThesevenstructuresoftheatomsoftheCNTtoprovidetheconstantconfinementcorrespondedtothesevenextremepointsonthePES.Ineffect.ThewaterchainwasconfinedintheCNTalongthedetail,theinitialorientationsofalloftheH-bondsweretubeaxis,andthesewatermoleculeswereconnectedtoeachupward.Fromreactanttothefirstintermediate,theH-bondofotherbyH-bonds.Fromthedifferentinitialgeometriesofthelowertwowatermoleculeswasbroken.WhentheH-bondconfinedwaterchains,wesearchedthestructuresforextremewasrebuilt,itsorientationmoveddownward.TheH-bondpoints(includingequilibriumandtransitionstate)intheorientationoftheotherthreewatermoleculesdidnotchange,rotationalprocessofwatermoleculesintheCNTandtracedhowever.Fromthefirstintermediatetothesecondthereactionpathwaysoftheflippingprocessofthewaterintermediate,theH-bondbetweenthemiddletwowaterchainsaccordingtointrinsicreactioncoordinate.moleculeswasbrokenandrebuilt,anditsorientationmoveddownward.Forthelowertwowatermolecules,theH-bond■ASSOCIATEDCONTENTorientationremaineddownward.Fromthesecondintermedi-*sıSupportingInformationatetotheproduct,theH-bondbetweentheuppertwowaterTheSupportingInformationisavailablefreeofchargeatmoleculeswasbrokenandrebuilt,anditsorientationmovedhttps://pubs.acs.org/doi/10.1021/acs.jpclett.0c03340.downward.Forthelowerthreewatermolecules,theirH-bondorientationremaineddownward.ThisdemonstratedtheReliabilityofthecomputationalmethods;statisticsoncompleteflippingprocessofthewatertetramerchain.Forwaterchainsincludingthedipolemoments,averagetheflipdetailsoftwowatermoleculesandthreewaterpersistenttimeofdipolealignment,andcomparisonof353https://dx.doi.org/10.1021/acs.jpclett.0c03340J.Phys.Chem.Lett.2021,12,350−354

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