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The Mechanisms for Free Chlorine Oxidation Ofreduced

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The Mechanisms for Free Chlorine Oxidation Ofreduced ö’3 The Mechanisms for Free Chlorine Oxidation of Reduced Manganese in Mixed—Media Filters by Suzanne Christine Occiano ' Thesis submitted to the Faculty of the Virginia Polytechnic Institute and State University of“ in partial Fulfillment oF the requirements For the degree _ Master of Science in EnvironmentalAPPROVED:Sciences and Engineering I I Dr. William R. nocke, Chairman zé ; Üregory D. Boardman Dr. Robert C. Hoehn $ II December, 1988 H Blacksburg, Virginia ä · a The Mechanisms for Free Chlorine Oxidation of Reduced l , Manganese in Mixed·Media Filters by Suzanne Christine Occiano Dr. William R. Knocke, Chairman Environmental Sciences and Engineering (ABSTRACT) ' The removal mechanisms of soluble manganese [Mn (1l)] through mixed-media filters were investigated. Experimentation was directed toward the continuous supply of an oxidant during column filter studies. Free chlorine (llOCl, OC1‘) was chosen to increase soluble manganese removal efficiency because chlorine is readily available and inexpen- sive. Filter media from four different water treatment plants were used in this study. Continuous-flow filter columns were operated in the presence and absence of 2.0 milli- grams per Liter (mg/ L) free chlorine. Maintaining constant influent manganese con- l centrations of 1.0 mg/L and flow rates of 2.5 gallons per minute per foot squared ' (gpm/ftz), the operational pH values of 6-6.2, 7.8 and 8.8 were investigated. : 1 ‘ Results indicate that a continuous feed of free chlorine (2 mg/L) applied to the filter columns could increase manganese (Il) removal efficiency. However, the amount andoxidationstate of the MnOx(S) surface coating initially on the media and the influent pH 1 had major influences upon the uptake of soluble manganese. From numerous Mn (II)uptakestudies with different media and varying pH conditions, oxide-coated filter media i continuously regenerated with free chlorine could result in increased soluble manganeseP l I removal through adsorption upon the MnOx(s) surface coating and subsequent oxidation directly on the media surface. The relationships of manganese removal and chlorine consumed were also explored. To further investigate the mechanisms of free chlorine oxidation for the removal of re- duced manganese, pl—I 5.0 backtitrations were conducted following exhaustion of the filter media. The exposure of such low pll conditions to columns operated in the pres- ence and abscnce of HOCI would ascertain if oxidation of the adsorbed Mn2+ was al- ways occurring, regardless of an oxidant feed. Results indicated that in the abscnce of I HOCI, the mechanisms for manganese removal on oxide-coated filter media were adsorption only. With the additional of HOCI, the adsorbed Mn2+ is oxidized directly on the surface of the media, thereby, continuously regenerating the surface oxide coat- ing. Additional work was begun to ascertain if free chlorine could be used as a viable alter- native to potassium permanganate (KMnO4) regeneration of oxide~coated filter media. Preliminary findings indicate from column cycling experiments that free chlorine could be used to regcnerate oxide-coated filter media prior to backwashing. I I ” I I I II I I Acknowledgements iv INTRODUCTION ................................................1 LITERATURE REVIEW...........................................4 Water Quality Concerns for Manganese .................................4 Chemistry of Manganese ............................................5 Reactions of Mn (II) with Oxygen ............{.......................5 Reactions of Mn (II) with Alternative Oxidants ..........................7 l. Free Chlorine ...............................................7 2. Potassium Permanganate ......................................10 3. Chlorine Dioxide ............................................10 4. Ozone ....................................................12 Removal and Control Techniques .....................................I2 Ion Exchange .......°...........................................12 Mn (II) Removal by Mn Greensand .................................14 Mn (II) Removal by Oxide—Coated Filter Media ........................16 Stabilization ...................................................1 8 METHODS AND MATERIALS.....................................22 Experimental Design ..............................................22 Laboratory Procedures .............................................24 'Preparation of Stock Solutions and Reagents ...........................24 Characterizing Water Treatment Filter Media ..........................25 Procedures for HAS Extraction ...................................25 Manganese Removal Studies by Oxide·Coated Filter Media .................26 Potassium Permanganate Demands of Oxide·Coated Filter Media ...........27 Release of Mn2+ from Oxide·Coated Filter Media .......................30 Repeated Mn2+ Uptake Studies with KMnO4 and HOCI Regeneration .......31 RESULTS ......................................................33 Mn (II) Removal Studies ...........................,...............33 Characterization of Water Treatment Plant Filter Media ..................34 . Column Experiments in the Absence of Free Chlorine .........,..........34 Effects of Surface Oxide Concentration on Adsorption Capacity at Constant pH 34 Effects of pH on Adsorption Capacity for Oxide·Coated Filter Media .......37 Column Studies in the Absence and Presence of Free Chlorine ..............37 Column Experiments in the Presence of Free Chlorine ....................51 Effects of Surface Oxide Concentration on Adsorption Capacity at Constant pH 51 Effects of pH on Adsorption Capacity for Oxide-Coated Filter Media .......51 Manganese and Chlorine Relationships51 Potassium Permanganate Demands of Oxide-Coated Filter Media ...........57 Release of Mn2+ from Oxide·Coated Filter Media .......................64 Repcated Mn2+ Uptake Studies with KMnO4 and HOCI Regeneration .......67 l vi1 I I DISCUSSION . .‘................................................79 Mn (II) Removal Studies ...........................................79 Characterization of Water Treatment Plant Filter Media ..................79 Removal of Mn (II) in the Absence of Free Chlorine .....................81 Effects of Surface Oxide Coating and Solution pH on Adsorption Capacity . 82 Mn (II) Removal in the Presence of Free Chlorine . .‘....................86 Repeated Mn2+ Uptake Studies with KMnO4 or I—IOCl Regeneration .........90 CONCLUSIONS.................................................93 REFERENCES ..................................................95 VITA...........................................................98 vii List of Figures Figure 1. pE—pIl Stability Diagram for Various Manganese Species in Water [Temp = 25°C; from (7)] .........................................6 Figure 2. lnfluence of pH on the Sorption of Mn (Il) on MnO; at 25°C [from (19)] ..................................................11 Figure 3. Ozonation Effects on Mn (II) Removal by Sand Filtration in the Presence of Organics .............................................13 Figure 4. Relationship of Chlorine Applied, Residual Chlorine and Effectiveness of Mn (II) Oxidation and Removal ...........................17 Figure 5. Effect of pH upon Mn (Il) Removal by Oxide·Coated Filter Media in the Absence of an Oxidant [from (3)] .............................19 Figure 6. Effect of Solution pH and Free Chlorine Addition on Mn (II) Removal by Oxide·Coated Media [from (3)] ............................20 Figure 7. Experimental continuous-flow column apparatus .................23 Figure 8. Mn (II) Uptake in the Absence of2 mg/L Free Chlorine for Media #3 at pH 6-6.2 (lnfluent Mn (II) = 1.0 mg,’L) .....................28 Figure 9. KMnOa Demand Performed on Exhausted, Oxide-Coated Filter Media 29 Figure 10. Mn (II) Sorption by Fe(OH); as a function of pH [from Morgan (19)] . 35 Figure I1. Effect of Surface Oxide Concentration on Mn (ll) Uptake by Different Media at pl-I 6-6.2 ................Y........................38 Figure 12. Effect of Surface Oxide Concentration on Mn (I1) Uptake by Different Media at pl-I 7.8 .........................................39 Figure 13. Effect of Surface Oxide Concentration on Mn (Il) Uptake by Different Media at pH 8.8 .........................................40 Figure 14. Effect of Solution pH upon Mn (II) Removal by Media #1 [3 mg/g Mn (II) on surfaee] in the Absence of Free Chlorine ..................41 viii Figure 15. Effect of Solution pH upon Mn (II) Removal by Media #2 [4 mg/g Mn(II)on surface] in the Absence of Free Chlorine ..................42 · I Figure 16. Effect of Solution pl·I upon Mn (II) Removal by Media #3 [14 mg/g Mn (II) on surface] in the Absence of Free Chlorine ..................43 Figure 17. Effect of Solution pH upon Mn (II) Removal by Media #4 [42 mg/g Mn (II) on surface] in the Absence of Free Chlorine ..................44 Figure 18. Mn (II) Uptake for Media #2 at pH 6-6.2 in the Absence and Presence of 2 mg/L IIOCI in the Filter Applied Water ....................46 Figure 19. Mn (II) Uptake for Media #2 at pl·I 7.8 in the Absence and Presence of 2 mg/ L IIOCL in the Filter Applied Water......................47 Figure 20. Mu (II) Uptake for Media #2 at pH 8.8 in the Absence and Presence of 2 mg/L HOCI in the Filter Applied Water ......................48 Figure 21. Mn (II) Uptake for Media #3 at pH 6-6.2 in the Absence and Presence of 2 mg/L HOCI in the Filter Applied Water ....................49 • Figure 22. Effect of Surface Oxide Concentration on Mn (II)
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