Clays and Clay Minerals, Vol. 29, No. 6, 423~,28, 1981.

N. C. LOCKHART CSIRO Institute of Earth Resources, Physical Technology Unit, 338 Blaxland Road Ryde, New South Wales, 2112, Australia Abstract--The conductivites of the Na and H ion-exchanged forms of kaolinitic clay rejects from sand-washing operations, both purified and as found naturally as a complex with soil organic matter, were examined. The two Na-clays showed linear conductivity-concentration characteristics, each having two regions with different slopes intersecting at -3.3% by weight of clay, which probably reflect a structural change from sol to gel. In the gel region, only the Na-counterions conducted, the reduction in conductivity with concentration being due to a smaller proportion of these ions in the Gouy layer and/or a decrease in their mobilities. In the sol, an additional, concentration-dependent conductivity arose from the electrophoretic motion of clusters of clay particles which gradually broke down on dilution. The two acid clays showed curved conductivity-concentration characteristics consistent with a weak acid dissociation equilibrium; the PKa values of 6.37 to 6.56 are close to those determined independently from titration with alkali. A stronger acid species detected in the titrations was not seen in the conductivity. The MOH~+/MOH/MO- model of the claysurface species and one set of the predicted concentrations of each species (see preceding paper) are consistent with the observed conductivities. The MOH2+ species probably bridged the edges and faces of clay particles so that the H atoms were identical, but became different when alkali was added. Key Words--Electrical conductivity, Electrophoresis, Humic acid, Kaolinite, Surface properties. INTRODUCTION The preceding paper (Lockhart, 1981) presented data on the potentiometric and conductometric titration of the hydrogen and sodium forms of aqueous clay rejects from a sand-washing operation, with and without the organic matter complexed to the clay. Models for the acidic species which reacted with the alkali were suggested, and predictions were made for the concentrations of each species from the end points of the titrations. The results of the p r e s e n t study of the conductivity and electrophoretic mobility are ideal for testing these models and predictions. EXPERIMENTAL quired several hours to come to equilibrium. Also, for the untreated and HCI/H202 samples in dilute dispersion, it was necessary to stir every few minutes during the measurements to prevent settling. The resistance of the cell filled with each clay dispersion was measured at 100 Hz (where it is nearly equivalent to the dc conductivity) as a function of electrode separation (d) over the concentration range 0.05 to 75 g solids/100 ml dispersion. A correction for the electrode polarization resistance (Lockhart, 1979) was made where appropriate. The corrected resistance R was converted to specific conductivity K = d/AR, where A is the area of the sample in the central electrode region of the cell, and thence to 'equivalent' conductance A = 1000 K/c (I1-1 cm 2 per unit-cell formula weight of the clay). The (electrophoretic) mobility of the clay particles was measured independently using a glass microscope slide to which two parallel strips of gold foil were attached 2 mm apart to serve as electrodes. The motion of the particles in dilute dispersion was observed at 50 to 90 • magnification, and the average time over a fixed distance was found for several particles in each sample using two different electric field strengths. The microscope was focused at the electroosmotic stationary level. RESULTS AND ANALYSIS

The untreated and NaCi-, HCI/H202-, and NaCI/ H~Oz-treated samples from batch A of the clay rejects described in Lockhart (1981) were examined. The peroxide treatment removed the organic matter, whereas the salt or acid treatment provided Na § or H § exhangeable cations. The untreated sample from batch B was also studied. Details of the preparations are given in the preceding paper (Lockhart, 1981).

The dielectric cell and a.c. bridge used to measure the conductivity are described elsewhere (Lockhart and Snaith, 1978). The samples were prepared by successive dilution with conductivity water in the cell itself, stirring at intervals until the conductivity became nearly constant. The more concentrated samples reCopyright 9 1981, The Clay Minerals Society

Electrophoretic mobility
The particles were always repelled from the cathode and were attracted to the anode if the voltage was not 423

4 for the NaCI/ H202 sample. the square root of concentration. V~ plot. The acetic acid data do not extend beyond ~ . The curved plots for the untreated samples from each batch resemble that for the acetic acid.5 _+ 0. Ka is proportional to A2c and hence to A X/'~. 1932) for the common weak acid.6 (J.0 | LI 8 8 c '~ 7 e. Literature data (Maclnnes and Shedlovsky. so that for weak-acid behavior. The error represents one standard deviation over about ten readings in each case. clay concentration for batch A: AI = NaCI/HzO2. 1. clay concentration for the untreated sample of batch B.1 0 0. A values taken from Figures 1 and 2 at convenient intervals of ~ are listed along with the products AX/-c.424 Lockhart 12 A4 Clays and Clay Minerals 50 4.265 on AI. Figure 2. The organic-free sample in acid form also has a curved A vs. The similarity of the latter two values tends to confirm that the 'untreated' sample is naturally acid treated.3 for the untreated sample. 1970). According to the theory of weak electrolytes (Robinson and Stokes. where A0 is the equivalent conductance at infinite dilution. In these circumstances the approximate constancy of the AX/-c products for each of the three clays is strong evidence for the weak acid picture.3 0'.{unit c e t t s / t i t e r ) Izz Figure 1. so high as to cause charge injection. Note that the cation-exchange capacity (expressed as a square root of concentration) is located at 0. acetic acid. Thus the clay particles in all samples possessed a net negative surface charge. Conductivity The conductivity results are summarized in Figures 1 and 2 as plots of A vs.5 0'.0. Thus.8.4. 1970) a is given by A/A0. the molar activity). The dissociation constant K~ for a weak acid is approximately a2X.15 to 0.8 1-0 1.2% (see Lockhart.3 for the HCl/HzO2 sample. because the weight loss of 6-6. The actual value of Ka may now be calculated from the averages of the AX/-c products over the range ~ = 0.9 4. Equivalent conductivity vs. Untreated Batch B A3 I-0 AI A2 0'. knowing that A0 is the sum of the H + ion .0. This variation in AX/'E is also exected for the clays.4 0'.1 -+ 0. A2 = HC1/H202. acetic acid is shown for comparison. it is also worth noting that the conductivity of the clay particles themselves is concentration dependent because of the gradual association into edge-to-face and edge-to-edge clusters whereby the particles are eventually immobilized in a network structure.4 for the NaCI sample.0. A4 = untreated. the product AV'c should be a constant.334 on A3 and 0. indicating that the conductivity in these samples is controlled largely by a dissociation equilibrium.7 0:8 019 t-'0 J~.2 0. 1981) is probably synonymous with the organic acid content.2 {unit cetts / t i t e r ) 1/2 0!2 0'. also X is equal to the clay concentration (c) for the HC1/H202 sample and about 6% of c for the two untreated samples. The calculated mobilities are (in 10-4 cm2/v sec) 3. but the product A V ~ should continue to decrease as ~ rises because neglect of the activity coefficient in Ka = ~2X become serious at higher concentrations (Robinson and Stokes.i E 6 5 E Acetic Acid /. where a is the degree of dissociation ('~ 1) and X the molar concentration of the acid (strictly. and 0.4 05 0.0 +. are also shown in Figure 2 for comparison. it is partly due to the difficulty of measuring exactly at the stationary level. In Table 1. A3 = NaC1. 2. Equivalent conductivity vs. In comparing the acetic acid data and the clay data.

42 1.13 1.39 0. V~ plots. Conductivity multiplied by the square root of the concentration.6 12-1 cm2/ eq for the untreated and 8.42 0.1 0.231 0.76) controls the conductivity of the acid clays whether or not organic material is complexed to the clay. but on alkali addition the particles disperse [edge MOH + H § face-]. and 4.220 1. must reflect a gradual reduction in this mobility and/or a steady decrease in the proportion of Na ions in the diffuse Gouy part of the double layer.942 0. whereas 'free' MOH2 § (exchanged with Na § from the alkali) can release a 'stronger acid' proton to react with the alkali. 1 425 Concentration X/c (unit cells/ liter)t Conductivity A (ll x cm2/unit celt) Untreated Batch A Untreated Batch B HCI/H~O~ Batch A Acetic acid Untreated Batch A Product A x x/c Untreated Batch B HCI/H~O2 Batch A Acetic acid 0. The corresponding pKu values are 6. These values suggest that a rather weak dissociation equilibrium (cf.47 0. A0) representing the sum of the equivalent conductivities of the contributing ions.8% by weight of clay.59 0. Ka (x l0 T) is thus 2.07 0. where only the Na counterions are mobile.664 0.22 15. for example.00 4.e. MODEL TESTING In the accompanying paper dealing with conductometric and potentiometric titrations.56 from the curved A vs.235 0. The two species must have been basically the same.768 0.40 4. while the concentration dependence of A reflects increasing ionic interactions that can be described in terms of activity coefficients (Robinson and Stokes.804 0.15 0..67 7. which is about 7. No.61 ----- 1 Data taken from Figures 1 and 2.830 0.795 0. It is reasonable to suppose the linear components in Figure 1 represent the sol and gel regions of the clays.163 0.720 0.90 0.13 5.69 3.4 1)-1 cmZ/eq (at 21.37.214 0.37-6. and HC1/HzOz batch A. plots are remarkably close to the 6. untreated batch B.5 0.4. making the H atoms different.6 0. with the value of A at V'-c = 0 (i. 6. in an edge-to-face structure [edge MO:~" + ~':face-] " .77 0.85 range obtained quite independently for the weaker acid reaction in the titrations.75 x 10-5. 29.02 ----- 0. where the H atoms are clearly identical.83 0. It is interesting that the gel region of the NaCI sample extrapolates to A = 0 at a V~ value equivalent to 100% clay solids. James and Parks (1981) used surface ionization constants in modeling colloidal dispersions in general.885 0.670 0.8 1. Linear behavior is typical of strong electrolyte systems. two clay particles could associate via MOH2 § bridges as.66 1.224 0.90 0. More specifically.236 0.0 4.7 1) x cm2/eq for the HC1/ H202 samples which are calculated from the measured mobilities. The model MOH2+/MOH/MO . A more quantitative assessment requires that the predicted concentrations of each species in Table 2 of . The two Na-clay samples with and without the organic material present have linear A vs. 3. respectively.29 1. . There is no evidence from the conductivity results for the stronger acid species (pKa 4-5) revealed in the titrations.56. The decline in conductivity with concentration in the gel region.Vol.62 1.63 1.(where M = AI and/or Fe) proposed in the accompanying paper allows 'bound' MOH2 + to behave similarly to MOH groups. acetic acid Ka = 1.37 0.684 0.31 for the untreated batch A.77.'H'. This difference could represent the contribution from the e x t r a cation-exchange capacity associated with the organic matter. with the point of intersection being the minimum concentration of particles required to set up a continuous network structure.5~ in present experiments) and the clay contribution of 10.44.194 0.59 1.4 0. The pK a values of 6. models for the surface chemical species behaving as stronger and weaker acids in the various clay samples were proposed.48-6.01 1. pKa = 4.1 8. 1981 Conductivity of kaolinite-humic acid complexes Table 1.234 0. each comprising two regions with different slopes.469 0.77 0.61 2. and 6.95 2.783 0.61.558 0. 6.2 0.28 0. contribution of 332. which must also be concentration dependent due to variation in the number and size (and hence the mobility) of edge-toface and edge-to-edge associated clusters of particles. and predictions were made of the concentrations of each species from the end points of the titrations.64 1.822 0.42 2. In the sol region there is an additional contribution from the clay particles themselves.3 0.71 2. 1970).1 I 1.65 1.51 1. The present conductivity results provide independent tests of these models and predictions.852 0. Another empirical observation is that the conductivity difference between the NaC1 and NaCI/ H202 samples is constant at 1.28 0. n S.92 3.70 6.1 12-1 cmZ/unit cell up to = 0. but became distinguishable when alkali was added to the clays.

22 0.43 2.78 0 1. The total predicted Ao is the sum of the CI-.75 3.83 0. NaCI/HzO2. so that detailed comparisons which follow are restricted to the range 1. on the other hand. The negative electrophoretic mobilities actually observed in the present study clearly eliminate this alternative. The ion conductivites h0 at infinite dilution for the present temperature of 21.65 1. t977) and experimental (Lockhart.5~ are (Robinson and Stokes.59 Sol 7. which also compares well with the observed values at the lowest concentrations in Figure 2.55 ~ 5. 24. .16 to obtain meq/unit cell of clay.0 ~ 2. 4.39 $ 7.7 for NaCI.61 6.ko Conc.6. The ratio of 2-3 between the predicted and observed values for both the sol and gel regions of the two samples is also reasonable. The overall charge on the clay particles is the algebraic sum of the + and .65 ~ 0 meq/ t00 g. 10.0 and 11. with the clay contribution being excluded from the gel totals.07 ~ 0 Sol 2. It is understood that the values in meq/100 g clay listed in Table 2 of the preceding paper for the NaC1/H202 and HCI/H202 samples also apply to the NaC1 and untreated samples. The units of h0 are f~-~ cm2/eq. Therefore. This allows direct comparison with the experimental A values in these units in Figures 1 and 2.61 4.61 2. clay = 28. The predicted contribution of the clay to the conductivity of the NaCI and NaC1/H202 samples is.65 ~ 3.65 0 0. Even for the two-step weaker acid reaction. the model and one set of predictions based on the end points of potentiometric and conductometric titrations are also quantitatively in agreement . Lockhart (1981) be consistent with the conductivities in Figure 1 of the present paper.o Cone . The predicted A0 for the untreated sample from batch B (not shown in Table 2) is 13. and then by the appropriate ko values to get ~ ~ cm2/unit cell.65 1. the concentrations are first multiplied by 5.values for the sol. the contribution of the clay to the total conductivity is predicted to be small.0 19.87 0. and is also in accord with the observed results. The concentration dependence of the conductivity should indeed have quite different origins than in the two acid clays. I6 2.13 Sol 7.84 $ 2.35 meq/100 g of clay-MOH2 + stronger acid sites in the untreated sample.4 4. ~.65 1. 1980) observations that between two-fifths and two-thirds of the Na counterions are located in the Gouy layer and are able to contribute to the conductivity.65 ~ 0 0 0. whereas the remaining counterions bound in the Stern layer contribute only to the permitivity.03 ~.35 Ao calculated Ao observed 4. as obtained from the electrophoretic mobilities. The predicted A0 values for the NaCI clay are nearly twice those for the NaC1/H20~ clay. For the HCI/H~O2 and untreated samples the predicted values are close to the observed A values for the most dilute dispersions that were measured (the experimental A0 itself is not available from the curved plots).05 11.65 meq. Since the unit-cell formula weight of kaolinite is 516.0 fl -~ cm2/unit cell. 1 NaC1/H~O2 Cone? Calc.4. the p r e d i c t e d net charge is positive for MOH2+C1 . ~. approximately reflecting the relative values actually observed.05 ~ 9.o 0 1. The predicted net charge is strongly positive (14.09 .95 meq/100 g of MON a + weaker acid sites in the NaCI sample and an extra 2." Untreated Calc.> 1. untreated.22 0 1.~ 7. with (for batch A) an additional 7.0 ~ 17.14 1 Procedure described in text.26 0.55 2.65 19.9.17 Gel 4. This follows from the theoretical (Van Olphen. CI.426 Lockhart Clays and Clay Minerals Table 2.65 meq/100 g) for the HC1/H202 and untreated samples when the one-step weaker acid situation is considered. Table 2 summarizes the concentrations in meq/100 g clay of the species concerned for the four samples of batch A.65 0 0.sites in each case. 1970) H + = 332.4.90 $ 3.61 2.17 Sol Gel 2. and clay.44 0 1.2. and 8.38 $ 1.1. quite significant.0 4. Na + or H +. Conductivities (f~-i cm2/unit cell) calculated from the predicted concentrations (meq/100 g) of each species. ho Cone.35 0 0. and HC1/H202 samples respectively." NaCI Calc. In addition. A0 is the sum of the ho values.= 71. which explains why the weak acid type of dissociation equilibrium is adequate to explain the near constancy of the AX/-~ products in Table 1. ~ HCI/HzOz Calc. Na + = 46.61 Na + or MOHz+ Clay 11.

N. 509-519.37 J~O 6. orHapyxenHble nyTeM TnTpOBaHitg. (1970) Etectroyte Solutions: Butterworths.qX: qHCTOM H eCTeCTBeHHOM C HpncyTCTBHeM rloqaealtoro oprax~qecKoro MaTepua3~a. qTo. 13o~ee cn.C. Die MOHz +Spezies iiberbriickten wahrscheinlich die Kanten und FIS. 11.56 liegen nahe bei den Werten.II14MOCTH C KOnt~enTpaRnefi 6hl~O pe3y~bTaTOM MeHbtuefi nponoptlnn aTaX aouon B c~oe Fyn n/a~n yMenbmenua Hx MO6HJ1bHOCTH. Part II--Kaolinite. Robinson. 74.und H+-ausgetauschten Formen von Kaolinit-Tonen untersucht.tlOqaMH. orpa3oBadlH MOCTHKHMe~Z. D. N. C. (1978) Apparatus for dielectric measurements on fluids and dispersions: J. Colloid Interface Sci. 29. (1980) Electrical properties and the surface characteristics and structure of clays. A.37 bis 6. was wahrscheinlich einen strukturellen Obergang vom Sol zum Gel widerspiegelt. B ~IByX COCTOflHH. R. Chem.corJlacoBanHble C paBHOBeCHeM BBccoLutaRlttt cylarofi KHCJIOTbl. (1932) The determination of the ionization constant of acetic acid at 25~ from conductance measurements: J. wobei jeder zwei Bereiche mit verschiedenen Anstiegen hat. [E. C. Phys. (1981) Surface characteristics of kaolinitic clays and clay-humic acid complexes by potentiometric and conductometric titrations: Clays & Clay Minerals 29. [U. Maclnnes. KOTOpble nocTellemto pa36aa. die unabh~ingig davon aus Titrationen mit Alkalien erhalten wurden. dab die Wasserstoffatome strukturell gleichartig wurden sich abet trotzdem beim Zusatz von Alkalien unterschiedlich verhielten. Van Olphen. REFERENCES James. (Received 14 July 1980. 413--422. H. N. New York. 6.Vol. 520-529. Im Solbereich entwickelte sich eine zus~itzliche. Soc. lnstrum. Lockhart. G.J1oro BelHeCTBa (CMOTpH npeJ~blJ1ylHylo CTaTblO) naxoJlyITCfl B coFJlacim c HafdlIOJlaeMblMit HpOBO/114MOCT~MIt. Konzentrations-abh~ingige Leitf'fihigkeit aus der elektrophoretischen Bewegung von Aggregaten von Tonteilchen. OTrpaCblBaeMblX noc.aetttecTB ua noBepXHOCTn r~nnbl. BepOs yKa3bmaeT na nepeMeny CTpyKTypbI H3 3031a B reflb. uepeceKamItmMHCa npn --3. ~Be Na-r31nrihl noKa3a. 6bt~a peay~hTaTOM 3JleKTpOqbope3tIOfi IIO~BtDKHOCTMBronJleHl4~ FflHHHCTblXqacTmll. (1981) Characterisation of aqueous colloids by their electrical double layer and intrinsic surface chemical properties: Surface Colloid Sci.3 Gew.~oBa3"IHCb HpOBOJIHMOCTH Na rl H KaTHOHOOrMeHHblX ~OpM Kao2IHHHTOBbiX FJIHH. in both the acid form and the sodium form. C. a non-swelling clay: J. 12. E: Scient.qHnhl.rlOTHbIe rJInHbl noKa3a. Konzentration-Abh~ingigkeiten.rlbHble KI4C3IOTHble BeHIeCTBa. BeJlnqHHbl pK a OT 6. n yMenbmeune npOBO. R. N.rn4 n3ornyTble xapaKTepI4CTltrn npoaoJ11tMOCTb-KOnRenTpaaUl. lnstrum. Eine starker saure Spezies. 433--435. Im Gelbereich leiteten nur die Na-Gegenionen. A. die mit der Verdfinnung allm/ihlich zusammenbrach.56 621H3KH BeflHtlHUaM. London. Mo/leab MOH2+/MOH/MO . W.l. die sich bei etwa 3. 571 pp. wurde bei der Leitfiihigkeit nicht beobachtet. BelRecTBa MOH2+. HarJIIO/la2tHCh BO BpeM$1 npot~ecca npOBO~I.3% aeca r. 1981 Conductivity of kaolinite-humic acid complexes 427 with the c o n d u c t i v i t y results for the o r g a n i c . die pKa-Werte yon 6.was auf das Dissoziationsgleichgewicht einer schwachen S/iure hinweist.rlRytttcb. B 3o. Diese Proben wurden sowohl in gereinigter Form als auch in natiirlicher Form---als Komplexe mit organischem Bodenmaterial--untersucht. BepO~tTnO. wobei die Verringerung der Leitf'fihigkeit mit der Konzentration auf einen kleineren Anteil dieser lonen in den Gouy-Schichten und/oder auf eine Abnahme ihrer Beweglichkeit zuriickgeht. O. KOTOpble aMeJm /Iae ~Rne~Hble xapaKTepHCTitKI! IIpOBO~IHMOCTb-KOHIleHTpalIIt~I. accepted 3 March 1981) Pe31oMe----I/Iccfle. IMOCTH.l. die bei der Titration gefunden wurde. and Parks. and Shedlovsky. No.3aaRcnMaJ~ OT KonaettTpatmrl. a TaKxe oglna CI4CTeMa npeJlcKa3annofi KOnRenTpal~nll /UI~I Kakv. Amer. J. T. (1977) An Introduction to Clay Colloid Chemistry: Wiley-Interscience. fiOflyqeHHbIM He3aBItCHMO IIyTeM THTpOBaHIt~I IRe. A. die Abfallprodukte aus den Sandwaschvorg~mgen sind.rlacTn c pa3HblMlt rlaKJiOl-laMl.W. Die beiden sauren Tone zeigten nichtlineare Leitf'fihigkeitskonzentrationsabh/ingigkeiten.qyKpa~tMH n rpan~lMrl r~mnncTblX qacTmL Tat( qTo aTOMbl H 6hbqn TO>I~eCTBennble. R. Die beiden Na-Tone zeigten lineare Leitf'fihigkeit vs. ~Be Kitc.I Resiimee---Es wurden die Leitf'fihigkeiten von Na +. (in press). Das MOH~+/MOH/ MO--Modell fiir die Arten der Tonoberfl~iche und die vorhergesagten Konzentrationen fiir jede Spezies (siehe vorhergehende Publikation) stimmen mit den beobachteten Leitfiihigkeiten iiberein. C.rle ~oraaoqnaR flpOBO/It4MOCTb. H. 318 pp. and Stokes. Part I--Swelling clays. 1011-1014.] . Lockhart. and Snaith.chen der Tonteilchen derart. B 06~acTn re3Lq TOflbKO Na-npOTltaOl. Lockhart. Lockhart. 1429-1438. (1979) Calibration of the reactive properties of resistors: J. Phys. lOHbl npono~aaa.-% Ton kreuzen. E: Scient.rle npot~ecca rlpOMblBaHH~l HeCKOB.c o m p l e x e d and organic-free clays. 54. no CTaItOBH~IIlCb pa3nblMI4 nocae ao6aaaeaaa mraoqn.

qui s'effondrent progressivement 5. Dans le sol. d6pendante de la concentration. une diminution de leurs mobilit6s. l'augmentation de la concentration 6tant due 5. 3.J. une conductivit6 additionelle. L'esp~ce MOH2 + a probablement travers6 les bords et les faces des particules d'argiles de sorte que les atomes H 6taient identiques. Une esp~ce d'acide plus fort d6tect6e dans les titrations n'a pas 6t6 trouv6e dans la conductivit6. un 6quilibre de dissociation d'acide faible.3% par poids d'argile.] .56 sont proches de celles d6termin6es de mani~re ind6pendante de titration d'alkalins.428 Lockhart Clays and Clay Minerals R6sum6--On a examin6 les conductivit6s de formes 6chang6es aux ions Na et H de rebuts d'argiles kaolinitiques d'op6rations de lavage de sable. ce qui r6fl/~te probablement un changement structural de sol 5. Les deux argiles-Na ont montr6 des caract6ristiques de conductivit6-concentration lin6aires. gel. Les deux argiles acides ont montr6 des caract6ristiques de conductivit6-concentration courb6es compatibles l'esp~ce de la surface de l'argile et une s6rie des concentrations pr6dites de chaque esp~ce (voir article pr6c6dent) sont compatibles aux conductivit6s observ6es. mais devenaient diff6rents quand un alkalin 6tait ajout6. Le module MOHz+/MOH/MO . [D. Dans la r6gion de gel. ayant une intersection 5. et/ou 5. seuls les contre-ions Na 6talent conductifs. formes purifi6es et aussi formes trouv6es naturellement en tant que complexes avec de la matibre de sol organique. la moindre proportions de ces ions dans la couche Gouy. la r6duction de la conductivit6 proportionelle 5. chacune ayant deux r6gions avec des inclinaisons diff6rentes. la dilution. les valeurs pKa de 6. 6.37 5. est survenue de la motion 61ectrophor6tique de grappes de particules d'argile.

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