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A:NewToolsandMethodsinExperimentandTheory
OptimizedContinuousApplicationofHyperpolarizedXenontoLiquids
BenjaminNiederländer,PeterBlümler,ThierryBrotin,DagmarVan
Dusschoten,AndreasOffenhäusser,HansJoachimKrause,andWernerHeil
,JustAcceptedManuscript•DOI:.8b09479•PublicationDate(Web):07Nov2018
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Page1of36TheJournalofPhysicalChemistry
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4OptimizedContinuousApplicationof
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7HyperpolarizedXenontoLiquids
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101,412
änder,ümler*,,
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,äusser4,H.-
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,UniversityofMainz,Germany
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,ENSdeLyon,France
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ülichGmbH,IBG-2,Germany
ülichGmbH,ICS-8,Germany
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27Abstract:
28Inrecentyears,NMRwithhyperpolarized(HP)xenoninsidefunctionalizedhoststructures
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30()havebecomeapotentialcandidateforthedirectobservationofmetabolic
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32processes().Acriticalissueforrealapplicationsisthedissolutionofthe
33HP-,wepresentrecentdevelopmentsfor
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35animprovedandcontrolleddissolutionofHP-Xeinliquidsusinghollowfibermembranesand
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38129
-Xecontinuouslyatsmalladjustablepressures
40andinapolarization-
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42HP-gasinaqueousliquids,
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45
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47optimizethesystemparameters,severalphysicalmodelsweredevelopedtodescribethe
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49transportandthelossesofnuclearpolarization.
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51Finally,-Xewas
52dissolvedinanaqueouscryptophane-A-(OCHCOOH)solution,andstableXesignalscould
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54bemeasuredover35min,
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56experimentalconditionsenabledthestudyofchemicalexchangeofxenonbetweencryptophane
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58andwaterenvironmentsevenforatime-consuming2DNMR-
59stabilityoverthemeasurementtimeallowedanexactdeterminationoftheresidencetimeofthe
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Xe-atominsidethecryptophane,±.
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612912
7Xenon-NMRisawell-establishedmethodtocharacterizemicroporoussystems,surfaces
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10explores,however,itswidechemicalshiftrangeofmorethan300ppminNMR(nuclear
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12magneticresonance)spectraallowstodistinguishphysicaladductsandadsorbatesselectively
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,xenondissolvesinmanyliquids,allowingsuchstudiesalsoin
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,itssolubilityinaqueousenvironmentsisratherlow,oftenlimiting
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,suchsensitivityproblems
181296
19canbepartiallyalleviatedbytheuseofso-calledlaser-orhyperpolarized(HP)Xe.
20Hyperpolarized129Xeistypicallyproducedbyspin-exchangeopticalpumping6andexhibitsa
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22spinpolarizationwhichisseveralordersofmagnitudehigherthaninthermalequilibriumat
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24commonmagneticfieldstrengths(5–25T)androomtemperature.
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26Inrecentyears,dissolvedxenonbecameapotentialcandidateformolecularimagingduetoits
27affinitytofunctionalizedhost-molecules(,cucurbiturilsandcryptophanes)
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,cryptophaneswerefunctionalizedbybiotintodetect
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31certainproteinsviathefrequencyshiftoftheHP-XeNMR-signalwheninsidethecryptophane
,
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36liquidcontentinsuchfoams,thegas/liquidinterfacecancauseseverelossinspectralresolution
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,thedissolutionprocess
39hastoberapidandwithoutsignificantdepolarizationoftheHP-
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41overcomebyusinghollow-fibermembranes,asalreadyusedforclinicalblood-oxygenation
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43().Suchmembranesactlikenanoporoussieveswherethegas/liquid
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interfaceisprimarilyprovidedbytheinterplayofsurfacetensionandimmiscibilityofpolymer
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47
48maintaintheseconditions,however,thepressuregradientatthisgas/liquidinterfacemustbe
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50keptlowtoavoideitherliquidingressintothemembranematerialorbubbling.
ö
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53toenrichbloodinmicewithHP-
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55theimplementationofthisconceptisthedissolutionoftheHP-gasinbio-liquids.
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57Inthiswork,wepresentadeviceforfast,efficient,polarization-sustainingandcontinuous
58dissolutionofhyperpolarized129-Xenoninliquidsviahollow-
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60focuswasgiventothepossibilitytoaddbuffergasestotheHP-Xeandtocontinuousapplication
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,wheretheperformance
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82D-NMRexperimentsonHP-
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10duetothefieldgradientsviatheHP-gastransferbetweendifferentmagneticfieldsisdiscussed
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12inAppendixA.
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22Beforetheessentialnewfeaturesofthesetuparedescribedindetail,aschematicoverviewof
23129
25inahome-builtpolarizerbyspin-exchangeopticalpumping(,adetaileddescriptionis
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27foundin11).TypicalvaluesforHP-
28129
29withpolarizationlevelsofabout20%using92%isotopicallyenrichedXe-gas(NUKEM
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31IsotopesGmbH,Alzenau,Germany).Asystemofglass-valves(,KontesHI-VAC,DWK
32LifeSciencesLLC,Rockwood,USA)thenallowsadmixingofbuffergases(
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34expansionorrelaxationsuppression11)andalsoconnectsaturbopumpforevacuation.
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36Operatingthecompressorunit()insuctionmodethenallowssubsequentfillingthe
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compressor’svolumewithseveralgases(hereHP-XeandHe).Thisgasmixtureisthen
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39continuouslypressedintothemembraneunit(,membranes:CelgardX30-240,3M
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41DeutschlandGmbH,Wuppertal,Germany)withawell-controlledoverpressureintheorderof
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.
44Thedissolutionanddetectionpartoftheexperimentwasdesignedinaverycompactwayand
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46includedtheNMR-excitation/detectioncircuittoreducethedistancebetweengasdissolution
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,thelatterpartwasplacedinsidethehomogeneouspartofanNMR
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-
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51spectrometer(,KEA2100MHz,MAGRITEK,Aachen,Germany).
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,a
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55home-builtpermanentmagnet-system(B0=)
56homogeneityandfieldstrengthofthismagnetwasinsufficientforspectroscopyexperiments,
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58whichwerethereforedoneataspecialsplit-coilsuperconductingmagnetatthe
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60ForschungszentrumJülich(B0=).
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3AllglassandmetalpartsthatareincontactwiththeHP-gaswerecarefullycleanedbya
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5universaldetergentsolution(MucasolfromMERZHYGIENEGmbH,Frankfurt,Germany),
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7rinsedseveraltimeswithwaterandbakedoutinavacuumovenat150°
8treatedidenticallybutbakedoutattemperaturesofabout100°C.
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:Schematicdrawingofthesetupseparatedintosixfunctionalunits:a)pressureunittocontrol
35thecompressorb)compressor(twotypesareusedofwhichonlytheTedlarbagcompressor
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37isshown)c)polarizertogenerateHP-Xe11whichismanuallytransportedtod)(dashed
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39arrow).d)Evacuationandgasmixingstage,e)NMRspectrometer,f)membraneunitto
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42textfordetails.
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Whiledialysismembranes12areswollenpolymerswhicharesemipermeabletoseparate
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50moleculesfromaliquidcarrier,oxygenationmembranessimplyincreasetheinterfacebetween
-sizescaffoldto
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53reducetheindividualinterfacesperpore().Theporesizesshouldbeaslarge
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55aspossibletoachievefastgasexchangebutsmallenoughtomechanicallystabilizethe
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,theessentialparametertoavoidliquid-leakageintothegas-part
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5range20-40barsandhencefourordersofmagnitudehigherthantheoppositeleakageofgas
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7(bubbles)
8clotting(causingembolism),thepressuredifferenceonsuchmembranesshouldnotexceed15
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-pressureonthegassideisrealizedbyaspecial
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12compressor,whichisdescribedinthefollowingsection.
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14About40ofsuchhollow-fibermembranes(outerdiameter244µm,wallthick