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L(0Frl Imvhias^O CENTRALE LANDBOUWCATALOGUS 0000 0030 4317 L(0frl imvhias^O ADSORPTION OF POLYLYSINES AT SOLID-LIQUID INTERFACES BIBLIOTHEEK LANDBOUWHOGESCHOOL WAGENINGEN [Sfl/^ll Joi^ Promotor:dr .J .Lyklema ,hoogleraa ri nd efysisch ee nkolloïdchemi e ^o2?o\} W STELLINGEN 1. Bumbullis et al. en Wolfes en Schügerl noemen de bulk-viscositeit die zij berekenen m.b.v. gegevens verkregen uit transversale ca­ pillaire golf- en oppervlaktespanningsmetingen aan viscoelastische oppervlakken ten onrechte de oppervlakte-viscositeit. Bumbullis, W. , Kalischewski, K en Schügerl, K. (1981). Foam behaviour of bio­ logical media. VII. Surface viscosity and viscoelasticity. Eur. J. Appl. Micro­ biol. Biotechnol. H, 110-115. Wolfes, H. en Schügerl, K. (1983). Foam behavior of biological media. VIII. Surface properties. Eur. J. Appl. Microbiol. Biotechnol. _T7, 371-375. 2. De Voeght en Joos missen een essentieel punt in het gedrag van de capillaire golven op het vloeistofoppervlak van natriumlaurylsul- faat/1-tetradecanol oplossingen door niet op te merken dat in dit geval de modulatie van de amplitude van de golven met de afstand wezenlijk verschilt met de amplitudemodulatie die bij water t.g.v. reflecties optreedt. Voeght, F. de en Joos, P. (1983). Waves at the air/liquid interface of a sur­ factant solution with a high surface shear viscosity. J. Colloid Interface Sei. 95, 142-147. 3. Bij een lage en constante geadsorbeerde hoeveelheid vindt t.g.v. de ladingstegenstelling tussen adsorbaat en adsorbens in poly-L- lysine, geadsorbeerd aan polystyreen (latex), geen ladingsgeïndu- ceerde helix-kluwen overgang plaats. Bij hogere adsorpties is zo'n overgang echter wel mogelijk. Dit proefschrift, hoofdstuk 6. 4. De analyse van de Surface-Enhanced Raman Spectra (SERS) van pipe- ridine van Sanchez et al. zou vollediger zijn geweest als zij er ook de invloed van de bezettingsgraad van het adsorbaat bij hadden betrokken. Sanchez, L.A., Birke, R.L. en Lombardi, J.R. (1984). Surface-Enhanced Raman scattering of piperidine. The effect of electrode potential on intensity. J. Phys. Chem. 88, 1762-1766. BIBLIOTHEEK DKR LANDBOUWHOGESCHOOL WAGENINGEN 5. Bij de presentatie van polyelectrolytadsorptiegegevens, waarbij de geadsorbeerde hoeveelheid is uitgedrukt als hoeveelheid massa, dient het duidelijk te zijn of het tegenion wel of niet hierin is inbegrepen. 6. Het onderscheid dat Lok et al. maken tussen reversibel en irrever­ sibel geadsorbeerd runder plasma-albumine is niet zinvol omdat zij de aggregatietoestand van het eiwit niet hebben vastgesteld. Lok, B.K., Cheng, Y-L. en Robertson, CR. (1983). Protein adsorption on cross- linked polydimethylsiloxane using total internal reflection fluorescence. J. Colloid Interface Sei. <n, 104-116. 1. De grafieken van Y /w versus m die Kvastek en Horvat gebruiken om de Warburg coëfficiënt uit te rekenen, geven alleen de door hen verwachte rechte te zien omdat ze het (wel gemeten) hoogfrequente deel ervan weglaten. Kvastek, K. en Horvat, V. (1981). Kinetic study of the Ag/AgI electrode by com­ plex impedance dispersion analysis. J. Electroanal. Chera. 130, 67-79. 8. Bij het onderzoek naar het gebied van afschuifsnelheden waarbij men pseudo-plastische vloeibare levensmiddelen in de mond beoor­ deelt op hun dikvloeibaarheid, gaan Cutler et al. ten onrechte voorbij aan het feit dat de meeste van deze vloeistoffen ook thi- xotroop zijn. Cutler, A.N., Morris, E.R. en Taylor, L.J. (1983). Oral perception of viscosity in fluid foods and model systems. J. Text. Stud. U±, 377-395. 9. Bij het nagaan van het verband tussen de geadsorbeerde hoeveelhe­ den polyacrylzuur en de wandlading van de adsorbentia hematiet en rutiel, houden Gebhardt en Fuerstenau ten onrechte geen rekening met een verschuiving van de wandlading die kan optreden t.g.v. de adsorptie van het polyelectrolyt. Gebhardt, J.E. en Fuerstenau, D.W. (1983). Adsorption of polyacrylic acid at oxide/water interfaces. Colloids and Surfaces 7, 221-231. Dit proefschrift, hoofdstuk 4 en 5. 10.D eschattin gdi eBuscal le nCorne rmake nva nd egemiddeld evolume ­ fractiepolyacrylzuu r aanhe toppervla k vanhu npolystyreendeel - tjes, opbasi sva no.a .protontitratie sva ngeconcentreerd epoly - acrylzuuroplossingen, isinconsisten tme tee nva nd edoo rhe nge ­ maakteveronderstellingen . Buscall,R . en Corner,T . (1982). Polyelectrolyte stabilised latices.Par t2 : Characterisation and colloidal behaviour.Colloid s and Surfaces5 ,333-351 . Ditproefschrift ,hoofdstu k6 . 11. Integenstellin g totd eresultate nbeschreve ni ndi tproefschrif t vinden Furusawa et al. geennoemenswaardig e invloedva nd ezout - concentratie op de adsorptie van poly-L-lysine aanpolystyree n (latex)bi jp H4 .Waarschijnlij k isdi the tgevol gva n demeet ­ proceduredi ez etoepassen . Furusawa, K., Kanesaka,M . en Yamashita, S. (1984). Adsorption behavior of poly-L-lysine and its conformation at the latex-water interface. J. Colloid Interface Sei.99 ,341-348 . Ditproefschrift ,hoofdstu k4 . 12. Intheoretisch epublicatie swaari nd eresultate nva ncomputerbere ­ keningenwezenlij kzij nvoo rd etheorie ,dien td ebeschrijvin gva n debijbehorend eprogramma' sminsten sgelijkwaardi gt ezij naa ndi e welkegangbaa r isbi jd eparagraa fmateriale ne nmethode ni nexpe ­ rimenteleverhandelingen . 13.Ee n grotere integratieva nbelei dm.b.t .waterkwalitei te nwater ­ kwantiteitda nn ui nNederlan dgebruikelij k is,ka nleide nto tee n groteredoelmatighei dva nhe twaterbeheer . 14.D e consumptie van zoutjes bijhe ttelevisiekijke nka ntoeneme n doord eaanwezighei dva nondertitels . B.C.Bonekam p Adsorptiono fpolylysine sa tsolid-ligui dinterface s Wageningen,1 2septembe r198 4 B.C.Bonekam p ADSORPTIONO FPOLYLYSINE S ATSOLID-LIQUI D INTERFACES Proefschrift terverkrijgin gva nd egraa dva n doctori nd elandbouwwetenschappen , opgeza gva nd erecto rmagnificus , dr.C.C .Oosterlee , inhe topenbaa rt everdedige n opwoensda g1 2septembe r198 4 desnamiddag st evie ruu ri nd eaul a vand eLandbouwhogeschoo l teWageninge n Voor mijn ouders Voor Margo, Stijn en Bart ABSTRACT Bonekamp,B.C . (1984)Adsorptio n ofpolylysine s atsolid-liqui d interfaces.Doctora l thesis,Agricultura l University, Wageningen. 208p , 80 figs,5 tables .Englis han d Dutchsummarie s Adsorption properties ofth epolyelectrolyte s poly-L-lysine (PL-L)an dpoly-DL-lysin e (PL-DL)o n hydrophobic (polystyrene latex, silver iodide)an dhydrophili c (silica) negatively charged solidparticle swer e studied. Adsorbed amounts asa functio no f concentration,ioni c strength,surfac echarge , PL chain length and chain charge density weredetermined .Th eadsorptio no fP Lo n negatively charged polystyrene latex and silica was alsomonitore d conductometri- callyan dpotentiometrically . Further flocculation and coagulationmeasurement swer e performed. Information about the secondary structureo fadsorbe d PL-Lwa s obtained fromproto n titrations ofPL- Lan d PL-DLadsorbe d atpolystyren eparticles . The stereoregularity and secondary chain structureo fP Ldoe sno t influenceth e adsorbed amount.A t lowconstan tadsorbe d amount,ther e isn o coilt oheli xtransi ­ tion in adsorbed PL-L,becaus e ofth echarg econtras tan dhydrophobi c interactions between PL and the surface.Onl y when the adsorbed amount is high ateac hpH ,a transition takesplac ean d adsorbed PL-Lca nb epartl yhelical . At lowp Han d lowioni c strength theadsorbe dpolyelectrolyte s showa rathe r flat conformation and there is no pronounced effecto fth ehydrophobicit yo fth eadsor ­ bent. All negative surface groups form ionpair swit ha n -NH,grou p ofPL ,bu tth e reverse is notth ecase .Th eadsorptio no fth ebasi cpolyaminoacid s increases(i.e . loopsan d tails start todevelop )i fth ep H isincrease d or ifth eioni c strengthi s raised. With the hydrophobic adsorbents theelectrolyt e effectpersist s upt over y high concentrations. Inth ecas eo fth ehydrophili c silica no increase above0.0 1M salt was observed, because here hydrophobic interactions are absent. The ionic strengthan dp Hdependenc e ofth eadsorptio no nhydrophobi c substrates are insatis ­ factorily agreementwit h theoreticalpredictions . Free descriptors:Adsorption ,binding ,solid-liqui d interface,polycation-polyanio n complex,polyelectrolyte ,charge dmacromolecule ,charge dpolyaminoacid ,poly-L-lysine , poly-DL-lysine, PLL,PLDL ,polystyren e latex, silica,conformation ,conformationa l transition,helix-coi l transition,secondar y structure,proto ntitration ,conductiv ­ ity,flocculation ,coagulation . CONTENTS page 1 INTRODUCTION 1 1.1 Generalbackgroun d 1 1.2 Aimso fthi swor k 3 1.3 Systemsuse dan doutlin eo fthi sstud y 3 1.4 References 5 2 ADSORPTIONO FPOLYAMINOACID SWIT HIONIZABL ESID EGROUP S 7 2.1 Introduction 7 2.2 Polyaminoacidsa tinterface s 8 2.3 Polyelectrolyte adsorption 10 2.4 References 13 3 MATERIALS 15 3.1 Polylysinean drelate dpolyaminoacid s 15 3.1.1 Synthesisan dstructur e 15 3.1.2 Solutionpropertie so fP L 16 3.2 Polystyrene latex 20 3.2.1 Preparation 20 3.2.2 Characterizationo fP Slate x 21 3.2.3 Thepolystyrene-wate r interface 28 3.3 Silicaan dBorosilicat eglas s 29 3.3.1 Preparationan dspecifi csurfac eare ao fsilic a 29 3.3.2 Borosilicateglas spurificatio nan dspecifi c 30 surfaceare a 3.3.3 Determinationo fth esurfac echarg edensit yb y 32 conductometrico rPotentiometri eproto n titrations 3.3.4 Someothe rrelevan tpropertie so fth esilica - 34 wateran dglass-wate rinterfac e 3.4 SilverIodid ean dPolyoxymethylen ecrystal s 37 3.5 Summary 37 3.6 References 38 Page ADSORPTIONO FTH EHIGHL YCHARGE DPOLYELECTROLYT EPOLYLYSIN E '4 1 ONDIFFEREN TSUBSTRATE S 4.1 Introduction
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