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Removal of Soluble Phosphorus from Surface Water using Iron (Fe-Fe) and Aluminum (Al-Al) Electrodes Tanner Ryan Devlin, Alessandro di Biase, Victor Wei, Maria Elektorowicz, and Jan Oleszkiewicz Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.7b02353 • Publication Date (Web): 09 Nov 2017 Downloaded from http://pubs.acs.org on November 10, 2017
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GRAPHICAL ABSTRACT 224x123mm (150 x 150 DPI)
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Removal of Soluble Phosphorus from Surface Water using Iron (Fe-Fe) and
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Aluminum (Al-Al) Electrodes
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T.R. Devlin1, *, A. di Biase1, V. Wei1, M. Elektorowicz2, J.A. Oleszkiewicz1
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R3T 5V6, Canada
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Maisonneuve Blvd. W., Montreal, QB H3G 1M8, Canada
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* Corresponding author. E-mail address:
[email protected] Civil Engineering, University of Manitoba, 15 Gillson St. Room E1-368A, Winnipeg, MB
Building, Civil, & Environmental Engineering, Université Concordia, 1455 De
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Abstract
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Soluble phosphorus removal using iron and aluminum electrodes was studied on water
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samples from the Red River, a hyper-eutrophic stream in Winnipeg, Canada. Four trials
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were conducted: I) mixed batch with 150-900 mA applied for 1 min to 1 L; II) stagnant
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batch with 600-900 mA applied for 1 min to 1 L; and III, IV) continuously stirred-tank
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reactor with 6.25-10 min hydraulic retention times and constant 900 mA. Maximum
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soluble phosphorus removals of 70-80% were observed in mixed batch and there was
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no significant difference between aluminum and iron electrodes (i.e., P-value 0.0526 to
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0.9487). Aluminum electrodes performed significantly worse than iron electrodes under
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higher hydraulic loads, with iron removing >70% soluble phosphorus and aluminum
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70% of
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soluble phosphorus at an HRT of 10 min, would be the preferred choice of material
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when applied under natural, flowing conditions. In comparison, aluminum electrodes
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failed to achieve >40% removal at HRTs of 6.25-10 min.
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In general, flowing conditions with turbulence would be preferred over stagnant
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conditions, which had a significant negative impact on soluble phosphorus residual in
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batch. For this reason, ponds and lakes are not ideal locations to apply electrodes,
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while streams and rivers would provide more appropriate mixing conditions. In addition,
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higher phosphorus loads provided greater efficiency per ampere applied. A 350%
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increase in soluble phosphorus load (from 0.28 to 0.97 mg-P min–1) resulted in a 300%
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increase in specific removal rate (from 0.21 to 0.64 mg-P C–1) for iron electrodes when
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900 mA was applied (Fig. 5). Therefore, tributary streams with higher phosphorus load
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and concentration should be targeted to improve efficiency.
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Fig. 5. Specific sequestration rate as a function of soluble phosphorus load for iron
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electrodes at 900 mA applied current intensity.
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Scale-up and application to other watersheds would require bench-scale testing
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to determine site specific design parameters. For instance, water characteristics such
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as conductivity would likely influence process design and performance (Fig. 6). Bench-
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scale testing would help assess site specific SARs and SRRs for desired levels of
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phosphorus removal. Furthermore, electrode configuration and operational procedures 26 ACS Paragon Plus Environment
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must be developed to maximize process efficiency. It would be interesting to examine
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the ratio of power consumption to phosphorus removal as it related to operational
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changes such as electrode spacing, submerged electrode surface area, and electrode
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shape and number. The configuration must also be designed such that electrode
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material could be readily replaced, since the sacrificial anode will be constantly losing
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mass as it is solubilized to remove phosphorus.
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Fig. 6. Current density as a function of applied voltage for iron and aluminum
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electrodes, grouped into two sets of conductivity, shown with extrapolated trendlines for
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water conductivity (K).
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Typically, smaller electrode spacing would result in lower power requirements
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and therefore lower operational costs for electricity. However, smaller electrode
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spacings would also restrict the flow of water between the cathode and anode which 27 ACS Paragon Plus Environment
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could have both positive and negative impacts. On one hand, smaller cross-sectional
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areas between the electrodes would increase flow-though velocities and may therefore
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mitigate surface fouling of the electrodes. If significant fouling was observed, however,
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smaller electrode spacings may have a negative impact since the flow of water through
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the cross-sectional area may be completely restricted.
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address physicochemical fouling of the electrodes would be to operate with intermittent
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DC or transformed AC. The alternating role of anode-cathode in both cases would allow
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for scouring of accumulated material on the electrodes through hydrogen gas
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production (3). Biological fouling could be addressed by operating at current intensities
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that inhibit the growth of microorganisms within the microenvironment of the anode and
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cathode. 30
A foreseeable measure to
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The simplest mechanism of phosphorus removal by the electrochemical device
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would be by sedimentation and burial as precipitated/entrapped matter within iron or
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aluminum hydroxides. Larger, natural basins such as lakes that have sufficient retention
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time for settling of the chemical complexes would act as phosphorus sinks if the
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electrochemical device was applied in more turbulent locations such as rivers and
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streams. However, natural basins with highly active anaerobic sediment may not be
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suitable for the burial method of phosphorus compounds or may require additional
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treatment to increase oxidation reduction potential.10,11 There is potential to modify the
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electrochemical device to extract precipitated/entrapped phosphorus, although this
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method would need to be studied in more detail to determine capture rates and
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operational efficiency. Instead of operating the electrochemical device to remove
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accumulated physicochemical foulant and release it into the environment, the process
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may be optimized to collect the accumulated material and completely remove it from
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suspension. Thereby, the precipitated/entrapped phosphorus in the physicochemical
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foulant would be removed from the watershed. Further considerations for the
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development of this method include the mechanism of removal from the electrode,
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mechanism of material transfer to a drying/processing area, and ultimately end use of
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the “recovered” material. In the worst case the material would be landfilled, while in the
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best case it could be used as slow-release phosphorus fertilizer.
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A more detailed discussion on the electrical and material costs for operation
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based on experimental parameters determined from this study is provided in Supporting
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information S.1. In general, consumable costs, reported per million litres treated, to
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remove 70% soluble phosphorus from Red River water with soluble phosphorus of 0.35
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g m-3 would include 5 USD to 17.5 USD electricity costs and material costs of 5.3 USD
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to 12.2 USD for iron and 39.2 USD for aluminum. Further discussion is provided in
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Supporting information S.2 to S.4 on the impact of the electrochemical process on pH,
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conductivity, and sediment properties.
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Acknowledgements
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The authors are grateful to graduate students Damian Kruk, Mario Poveda, and
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Kamil Wisniewski, who assisted with collecting water samples from the Red River. The
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authors acknowledge the Natural Sciences and Engineering Research Council of
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Canada for the Undergraduate Student Research Award (USRA) and Canada Graduate
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Scholarship-Master’s (CGS-M) to the senior author.
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References (1) Withers, P.J., Haygarth, P.M. Agriculture, phosphorus and eutrophication: A European perspective. Soil Use Manag. 2007, 23, 1–4. (2) Han, C.W., Xu, S.G., Liu, J.W., Lian, J.J. Nonpoint-source nitrogen and phosphorus
503
behavior and modeling in cold climate: a review. Water Sci. Technol. 2010, 62, 2277–
504
2285.
505
(3) Azevedo, L.B., van Zelm, R., Leuven, R.S.E.W., Hendriks, A.J., Huijbregts, M.A.J.
506
Combined ecological risks of nitrogen and phosphorus in European freshwaters.
507
Environ. Pollut. 2015, 200, 85–92.
508
(4) White, S.H., Duivenvoorden, L.J., Fabbro, L.D. Impacts of a toxic Microcystis bloom
509
on the macroinvertebrate fauna of Lake Elphinstone, Central Queensland, Australia.
510
Hydrobiologia. 2005, 548, 117–126.
511
(5) Song, L., Chen, W., Peng, L., Wan, N., Gan, N., Zhang, X. Distribution and
512
bioaccumulation of microcystins in water columns: A systematic investigation into the
513
environmental fate and the risks associated with microcystins in Meiliang Bay, Lake
514
Taihu. Water Res. 2007, 41, 2853–2864.
515
(6) Oberholster, P.J., Botha, A.M., Ashton, P.J. The influence of a toxic cyanobacterial
516
bloom and water hydrology on algal populations and macroinvertebrate abundance in
517
the upper littoral zone of Lake Krugersdrift, South Africa. Ecotoxicology. 2009, 18, 34 30 ACS Paragon Plus Environment
Environmental Science & Technology
518 519 520 521 522 523 524
46. (7) Nørring, N.P., Jørgensen, E. Eutrophication and agriculture in Denmark: 20 years of experience and prospects for the future. Hydrobiologia. 2009, 629, 65–70. (8) Withers, P., Neal, C., Jarvie, H., Doody, D. Agriculture and eutrophication: where do we go from here? Sustainability. 2014, 6, 5853–5875. (9) Schindler, D.W. The dilemma of controlling cultural eutrophication of lakes. Proc. R. Soc. B Biol. Sci. 2012, 279, 4322–4333.
525
(10) Wauer, G., Gonsiorczyk, T., Kretschmer, K., Casper, P., Koschel, R. Sediment
526
treatment with a nitrate-storing compound to reduce phosphorus release. Water Res.
527
2005, 39, 494–500.
528
Page 32 of 35
(11) Yamada, T.M., Sueitt, A.P.E., Beraldo, D., A.S., Botta, C.M.R., Fadini, P.S.,
529
Nascimento, M.R.L., Faria, B.M., Mozeto, A.A. Calcium nitrate addition to control the
530
internal load of phosphorus from sediments of a tropical eutrophic reservoir : Microcosm
531
experiments. Water Res. 2012, 46, 6463–6475.
532
(12) Schoumans, O.F., Chardon, W.J., Bechmann, M.E., Gascuel-Odoux, C., Hofman,
533
G., Kronvang, B., Rubæk, G.H., Ulén, B., Dorioz, J.-M. Mitigation options to reduce
534
phosphorus losses from the agricultural sector and improve surface water quality: A
535
review. Sci. Total Environ. 2014, 468-469, 1255–1266.
536
(13) Yin, H., Kong, M. Simultaneous removal of ammonium and phosphate from 31 ACS Paragon Plus Environment
Page 33 of 35
Environmental Science & Technology
537
eutrophic waters using natural calcium-rich attapulgite-based versatile adsorbent.
538
Desalination. 2014, 351, 128–137.
539
(14) Dobbie, K.E., Heal, K.V., Aumônier, J., Smith, K.A., Johnston, A., Younger, P.L.
540
Evaluation of iron ochre from mine drainage treatment for removal of phosphorus from
541
wastewater. Chemosphere. 2009, 75, 795–800.
542
(15) Buda, A.R., Koopmans, G.F., Bryant, R.B., Chardon, W.J. Emerging technologies
543
for removing nonpoint phosphorus from surface water and groundwater: introduction. J.
544
Environ. Qual. 2012, 41, 621.
545
(16) Meis, S., Spears, B.M., Maberly, S.C., Perkins, R.G. Assessing the mode of action
546
of Phoslock in the control of phosphorus release from the bed sediments in a shallow
547
lake (Loch Flemington , UK). Water Res. 2013, 47, 4460–4473.
548
(17) Wei, V., Elektorowicz, M., Oleszkiewicz, J.A. Electrically enhanced MBR system
549
for total nutrient removal in remote northern applications. Water Sci. Technol. 2012, 65,
550
737–742.
551
(18) Kruk, D.J., Elektorowicz, M., Oleszkiewicz, J.A. Struvite precipitation and
552
phosphorus removal using magnesium sacrificial anode. Chemosphere. 2014, 101, 28
553
33.
554 555
(19) Ebbers, B., Ottosen, L.M., Jensen, P.E. Electrodialytic treatment of municipal wastewater and sludge for the removal of heavy metals and recovery of phosphorus. 32 ACS Paragon Plus Environment
Environmental Science & Technology
Page 34 of 35
556
Electrochim. Acta. 2015, 181, 90–99.
557
(20) Parga, J.R., González, G., Moreno, H., Valenzuela, J.L. Thermodynamic studies of
558
the strontium adsorption on iron species generated by electrocoagulation. Desalin.
559
Water Treat. 2012, 37, 244–252.
560
(21) Kim, S.O., Moon, S.H., Kim, K.W., Yun, S.T. Pilot scale study on the ex situ
561
electrokinetic removal of heavy metals from municipal wastewater sludges. Water Res.
562
2002, 36, 4765–4774.
563
(22) Ottosen, L.M., Pedersen, A.J., Hansen, H.K., Ribeiro, A.B. Screening the
564
possibility for removing cadmium and other heavy metals from wastewater sludge and
565
bio-ashes by an electrodialytic method. Electrochim. Acta. 2007, 52, 3420–3426.
566
(23) Huang, J., Elektorowicz, M., Oleszkiewicz, J.A. Dewatering and disinfection of
567
aerobic and anaerobic sludge using an electrokinetic (EK) system. Water Sci. Technol.
568
2008, 57, 231–236.
569
(24) Ibeid, S., Elektorowicz, M., Oleszkiewicz, J.A. Electro-conditioning of activated
570
sludge in a membrane electro-bioreactor for improved dewatering and reduced
571
membrane fouling. J. Memb. Sci. 2015, 494, 136–142.
572
(25) Yousuf, M., Mollah, A.R., Parga, J.R., Cocke, D.L., Mokovsky, P., Gomes, J.A.G.,
573
Kesmez, M. Fundamentals, present and future perspective of electrocoagulation. J.
574
Hazard. Mater. 2004, B114, 199–210. 33 ACS Paragon Plus Environment
Page 35 of 35
Environmental Science & Technology
575
(26) Moreno, H., Cocke, C.D.L., Gomes, J.A., Morkovsky, P., Parga, J.R., Peterson, E.,
576
Garcia, C. Electrochemical generation of green rust with electrocoagulation. ECS Trans.
577
2007, 3, 67–76.
578
(27) Zhu, Y., Wu, F., He, Z., Guo, J., Qu, X., Xie, F. Characterization of organic
579
phosphorus in lake sediments by sequential fractionation and enzymatic hydrolysis.
580
Environ. Sci. Technol. 2013, 47, 7679–7687.
581 582
583
(28) Lakshmanan, D., Clifford, D.A. Ferrous and ferric ion generation during iron electrocoagulation. Environ. Sci. Technol. 2009, 43, 3853–3859. (29) Veli, S., Ozturk, T., Dimoglo, A. Treatment of municipal solid wastes leachate by
584
means of chemical- and electro-coagulation. Sep. Purif. Technol. 2008, 61, 82–88.
585
(30) Wei, V., Elektorowicz, M., Oleszkiewicz, J.A. Influence of electric current on
586
bacterial viability in wastewater treatment. Water Res. 2011, 45, 5058-5062.
34 ACS Paragon Plus Environment