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Magnesium Ion Inhibition of Calcium Carbonate Precipitation and Its Relation to Water Quality

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Magnesium Ion Inhibition of Calcium Carbonate Precipitation and Its Relation to Water Quality Utah State University DigitalCommons@USU All Graduate Theses and Dissertations Graduate Studies 5-1970 Magnesium Ion Inhibition of Calcium Carbonate Precipitation and its Relation to Water Quality John J. Hassett Utah State University Follow this and additional works at: https://digitalcommons.usu.edu/etd Part of the Other Chemistry Commons, and the Soil Science Commons Recommended Citation Hassett, John J., "Magnesium Ion Inhibition of Calcium Carbonate Precipitation and its Relation to Water Quality" (1970). All Graduate Theses and Dissertations. 4574. https://digitalcommons.usu.edu/etd/4574 This Dissertation is brought to you for free and open access by the Graduate Studies at DigitalCommons@USU. It has been accepted for inclusion in All Graduate Theses and Dissertations by an authorized administrator of DigitalCommons@USU. For more information, please contact [email protected]. MAGNESIUM ION INHIBITION OF CALCIUM CARBONATE PRECIPITATION AND ITS RELATION TO WATER QUALITY by John J . Hassett A dissercation submitted in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY in Soil Chemis'try Approved: UTAH STATE UNIVERSITY Logan , Utah 1970 ACKNOWLEDGMENTS I would like to express my deep appreciation to Dr . Jerome J, Jurinak for his encouragement and helpful guidance during my studies. I sincerely appreciated my acquaintance with him and the chance of working with him. I would also like to express my thanks to Dr. Raymond L. Kerns, Dr. James W. Sinclair, Dr. R. L. Smith and Dr. Alvin R. Southard for serving as committee members. This dissertation is dedicated to my wife , Gloria , without her help and sacrifices this dissertation would never have been completed. John J . Hassett TABLE OF CONTENTS Page INTRODUCTION 1 REVIEW OF LITERATURE Effect of Mg Solution phase 5 Solid phase 7 METHODS AND MATERIALS 9 RESULTS AND DISCUSSION 20 SUMMARY AND CONCLUSIONS 40 PROPOSALS FOR FUTURE WORK '+'I LITERATURE CITED 46 APPEND! XES . 48 Appendix A. Development of the Carbonate Saturometer Theory after Weyl (24) . 49 Appendix B. Calculation of aca++, aMg++ and aHco; as Effected by Ion-pair Formation 54 Appendix C. Computer Program 59 VITA 61 LIST OF TABLES Table Page l. Composition of wa1:ers (Series 2) 11 2. Composi t:ion of wa"ters (Series 1) 12 3. F(x) and the amount of Caco dissolved upon addition 3 of carbonat:e material . 17 4 . F(x) and the amount of CaC0 dissolved upon addit:ion 3 of carbonate material . 17 F(x) and the dissolved upon addition s. amoun~ of CaC0 3 of carbonate mater1al . 18 6 . F(x) and the amount of CaC0 dissolved upon addition 3 of carbonate material . 18 7. F(x) and the amount of CaC0 dissolved upon addition 3 of carbonate material 19 Calculation of amount of CaC0 dissolved or e. 3 precipitated 26 LIST OF FIGURES Figure Page l. Reaction vessel 14 2. Change in pH (llpH) resulting fl'om addition of T, U, M, P to waters 1 29 3. llpH resulting from addition of T, U, M, p to waters 2 30 4. llpH resulting from addition of T, u, M, p to waters 3 31 5 . llpH ' s resulting from addition ofT, u, M, p to waters 4 32 6 . llpH ' s t•esulting n-.om addition ofT, u, M, p to waters 5 33 7. Comparison of calculated llpH's waters 1 with actual llpH( ":' ) 34 8 . Comparison of calculated llpH's water 2 and actual llpH(T) 35 9 . Comparison of calculated llpH's water 3 and actual llpH(T) 36 10 . Comparison of calculated llpH ' s waters 4 with actual llpH(T) 37 11. Comparison of calculated llpH's water 5 with actual llpH(T) 38 ABSTRACT Magnesium Ion Inhibi•ion of Calcium Carbonate Precipitation and its Relation To Water Quality by John J. Hasse••, Doctor of Philosophy Utah State University , 1970 Major Professor: Dr . Jerome J . Jurinak Departmen•: Soils and Meteorology The effect of Mg++ ion on the solubility of calcium carbonate was determined using P. K. Weyls "carbonate sa•urometer. " The amount of calcium carbonat:e precipitated or dissolved was measured for five series of wa•ers when equilibrated with solid It was found that the effect of Mg ++ ion on solubility depended upon the nature of the solid phase: surface area , coprecipitated Mg++ , mineralogy , etc. Pure low area calcite showed an increase in solubility which could be explained by ion-pair formation , while its other carbon- ates departed from this behavior . ( 67 pages) INTRODUCTION The precipitation or solution of Caco in terms of water quality 3 is important. From the industrial and municipal view, the solution of Caco and MgC0 by irrigation return flow waters increases the concen­ 3 3 tration of Mgt+ and Ca++ ions in solution. Eldridge (11) considers the increase of water hardness due to Ca++ and Mgt+ ions to be the most important single adverse effect contributed by irrigation return flows. Hardness results in increased cost of soap, water softening and boiler scale . From an agronomic approach Caco precipitation, while reducing 3 the total salt load of the water, can increase the sodium hazard of the water when used for irrigation purposes. Eaton (10) recognized the potential hazard caused by caco precipitation from the irrigation 3 waters when he introduced the concepts of (a) possible sodium percent- age and (b) residual sodium carbonate (RSC) . These were attempts to estimate the sodium hazard by assuming that all Mgt+ and Ca++ ions in solution would precipitate quantitatively in the presence of excess Hco; and co; ions . Possible sodium percentage Residual sodium car bonate where ( ) represents concentrations expressed in meq/liter. Wilcox (25) in field and laboratory studies came to the conclusion that waters with more than 2. 5 meq/liter RSC were not suitable for 2 irrigation purposes . Waters concaining 1.25 to 2.5 meq/liter RSC were marginal and those concaining less than 1.25 meq/liter RSC were prob- ably safe. Babcock et al. (2) found in a 4-year lysimeter study, using artificial waters, that the amount of exchangeable Na+ produced did noc appear to be closely relaced to che Hco; in the water. This is in contrast to what might be expected from Eaton ' s (10) principle of possible sodium percentage. Langelier (16) devised an index co indicate the extenc of waters flowing in a closed system (no loss of C0 ) to precipitate or dissolve 2 Caco . The saturation index is defined as the actual pH of the water 3 (pHa) minus the theoretical pH (pHc) that the water would have if it were in equilibrium wich Caco (calcite). 3 Saturation index pHa - pHc Positive values of the index indicate that Caco will precipitate 3 from the water, whereas negative values indicate that the water will dissolve Caco . Langelier's equation for the pHc is: 3 pHc (pK~ 2 - p~p) + pea + pAlk I I where pKa and pKsp are, respectively, the second dissociation constant 2 and the solubility constant of H co and CaC0 corrected for ionic 2 3 3 strength. pCa is the negative logarithim of the calcium ion concen- tration and pAlk is the negative logarithim of the equivalent concen­ tration of titratable base (co; + Hco;). Bower (4) , and Pratt , Bronson and Chapman (21) found the fraction of applied Hco; that precipitated in the soil was highly related to a modified Langelier saturation index. The modification was the 3 replacement of the actual pHa of water with the pH of the highly- buffered soil (pHs). The saturation index used was: (Modified) Saturation index pHs - pHc Bower , Ogata and Tucker (5) further modified the saturation index, to obtain a better fit with experimental data , by replacing pCa with a linear combination of the concentration of magnesium and calcium in the solution , p(Ca + Mg) . pH~ (p~ 2 - pK~p) T p(Ca + Mg) t pAlk 6 where saturation index = pHs - pHc. The above equations assume that the chemical reactions of magne­ sium are the same as calcium and that Ca++ +Mgt+ can be combined in a linear combination to allow for the precipitation of both caco and 3 It is the contention of the author that this type of additivity is not valid since (a) MgC0 has a greater solubility than Caco , 3 3 (b) Mg++ ion may inhibit precipitation by interfering with nucleation, (c) Mg++ can increase the total amount of Caco which will dissolve 3 due to the formation o£ ion-pairs and (d) Mgrt can interact with the Caco crystal forming a more soluble crystal than pure calcite. 3 REVIEW Of LITERATURE The solution and precipitation of caco are controlled by several 3 variables. Ponnamperuma (20), Garrels and Christ (13) and others give the following equilibria which control simple Caco systems (Mg++ ion 3 absent) . co Cgas) + K = AH co /PC0 2 H20 :; H2co3 1 2 3 2 + H co :;: H Ka AH-t 2 3 + Hco; 1 AHCO;/ AHio3 Hco; :_ H+ ;- co; Ka2 AH+ · ACO;/AHCO; Caco :;: Ca++ + Ksp ACa++ · 3 co; AC03/ACaC0 3 (~) Usually the ACaCOJ(s) is taken to be unity reducing Ksp to: Ksp ACa++ · Aco; Kern (15) showed that the solution of C0 (gas) to give H co is two 2 2 3 separate processes . K is the correct value for the equil~brium con- 1 stant of the first reaction and the value for Ka is a composite of 1 the second process and the value for the first dissociation of carbonic acid . K = AH co /AC0 (aq) 2 2 3 2 Ka = AH+ · AHC0 /AH co 1 3 2 3 In addition to these equilibria , the system is complicated by ion-pair formation , which involves the co; , Hco; , OH and Ca++ ions.
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