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Accepted Manuscript © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 Filterability of surface water from Tbilisi Sea: Preliminary assessment of ultrafiltration as a process alternative Accepted for publication as a Note in Separation Science and Technology journal on April 15, 2019 Published article DOI: 10.1080/01496395.2019.1614063 Avtandil Kobaladzea; Irakli Lomidzea; Sandro Maludzea; Archil Sakevarashvilia;, Kakha Didebulidzea*; Zaza Metrevelia; Volodymyr V. Tarabarab**; Giorgi Titvinidzec; Tamara Tkeshelashvilic,d a School of Engineering and Technologies, Agricultural University of Georgia, Kakha Bendukidze University Campus, 240 David Aghmashenebeli Alley, Tbilisi, Georgia b Department of Civil and Environmental Engineering, Michigan State University, East Lansing, MI 48824, USA c Institute of Chemistry and Molecular Engineering, Agricultural University of Georgia, Kakha Bendukidze University Campus, 240 David Aghmashenebeli Alley, Tbilisi, Georgia d Gardabani Thermal Power Plant, Water Treatment Plant Laboratory, 2b David Aghmashenebeli Ave., Gardabani, Georgia. * Corresponding author: Phone: +995 (593) 34-44-81; [email protected] ** Corresponding author: Phone: +1 (517) 432-1755; [email protected] Financial support: V. V. Tarabara was supported by a U.S. Fulbright Scholar fellowship; T. Tkeshelashvili was supported by Volkswagen Foundation grant (Az: 93 331). 1 © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 Abstract This preliminary laboratory scale study evaluated the feasibility of ultrafiltration as an alternative technology for treating water from Tbilisi Sea (Republic of Georgia). The analysis was performed with both raw source water and with the source water pretreated by coagulation and flocculation. Coagulation/flocculation pretreatment improved ultrafiltration performance in terms of permeate flux and rejection of dissolved organic carbon (DOC). The pretreatment led to a change in the dominant membrane fouling mechanism from pore blocking to cake filtration. The observed improvement in DOC rejection was attributed to the cake layer’s action as a secondary membrane. Both permeate flux and DOC removal data support retaining coagulation and flocculation as a part of the overall treatment process. Keywords: ultrafiltration, coagulation, flocculation, membrane fouling, blocking laws 1. Introduction Tbilisi Sea (თბილისის ზღვა) is a man-made freshwater lake located northeast of Tbilisi at an altitude of 580 m. Also known as Tbilisi Reservoir (თბილისის წყალსაცავი), Tbilisi Sea is ~ 8.75 km long and ~ 2.85 km wide with the average depth of 26.6 m, maximal depth of 45 m and the total surface area of ~ 11.6 km2. Tbilisi Sea has two main tributaries: Aragvi channel (also called Bodorna- Grmagele tunnel), which delivers water of the Aragvi river, and Zemo Samgori channel, which delivers water of the Iori river (Figure 1). The flow rate of another tributary, Kvirikobis Khevi river, is much smaller than that of the first two (flow rate data not available). The outflow is an irrigation channel, which is a part of Samgori irrigation system. Tbilisi Sea is characterized by weak winter and well- expressed summer direct stratification and is classified as oligotrophic; more 2 © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 recently, eutrophic behavior has been observed during summer seasons. The average summer and winter temperatures in the Tbilisi Sea are 23.3 °C and 7.5 °C, respectively [1]. Tbilisi Sea is a source of drinking water for Tbilisi, the capital city of Georgia. The water is treated by the water supply company Georgian Water and Power (GWP) to comply with the national drinking water standards. As of July 2018, Tbilisi Sea was a source of drinking water to ~ 111,300 customers in Tbilisi supplementing other sources including water from the Zhinvali reservoir (also fed by Aragvi river). The treatment train in the GWP-managed water treatment plant includes gravity settling, coagulation/flocculation (C/F), sand filtration and, finally, disinfection by chlorine. The treated water is tested with respect to several water quality parameters to ascertain compliance with government-issued water standards (Drinking Water Technical Regulations). For high quality feed waters suitable to direct or inline filtration, membranes present a good alternative to conventional surface water treatment processes. With an appropriate choice of the membrane pore size, membranes can ensure very high microbiological quality of the permeate. With the pore size smaller than the size of most viruses (between 2 nm and 100 nm) tight ultrafiltration membranes are especially well suited for application such as drinking water treatment where pathogen removal is of paramount importance. While the coagulation and flocculation are critical for the proper functioning of the granular media filtration process, their effect on downstream membrane filtration is incompletely understood despite being a subject of significant research efforts [2- 4]. The objective of this preliminary laboratory-scale study was to evaluate filterability of Tbilisi sea water by ultrafiltration membranes and to assess the potential of this membrane technology for replacing granular media filtration. The analysis was performed with both raw source water and with water pretreated by 3 © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 coagulation and flocculation. The study tested the hypothesis that retaining coagulation/flocculation as pretreatment would decrease intrapore blocking and improve ultrafiltration performance in terms of both water throughput and rejection of feed organics. 2. Materials and Methods 3.1 Reagents and sampling procedure Aluminum sulfate Al2(SO4)3 was high purity as specified by the State Standard GOST 12966-85. The water used for membrane compaction was double distilled using an in-house distillation system. Tbilisi Sea water samples were collected from the depth of ~ 0.5 m at two locations in the Tbilisi Sea (Figure 1) in September 2017 ~ 50 meters from the shore at sampling point A and ~ 15 meters from the shore at sampling point B. The summer and early Fall is when the water temperature is evaluated and the load of anthropogenic pollution is expected to be higher [1]. The 20 L samples were transported to the laboratory and stored at 4 °C until further use. The containers were stirred before withdrawing water samples for each treatment test. 3.2 Coagulation and flocculation as an optional pretreatment step First, 10 g of Al2(SO4)3 was dissolved in 1 L of distilled water to produce 10 mg/L (as Al2(SO4)3) coagulant solution . 50 mL of the solution was added to 950 mL of sample water for each test to result in 10 mg/L concentration of coagulant in the water sample. This solution was placed in a 1 L cylindrical jar (internal diameter of 10 cm) and rapidly mixed for 1 min at 200 rpm (coagulation stage) and then mixed slowly at 20 rpm for 20 min (flocculation stage). The 76 mm 25 mm 3 mm impeller was positioned ~ 20 mm above the bottom of the jar. The coagulation / flocculation sequence was followed by 30 min of settling in the absence of mixing. After settling, 180 mL of water was carefully withdrawn from 4 © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 the top of the jar by a syringe for further treatment. The coagulation/flocculation tests were performed at room temperature, which was in the 15.5 °C to 17.9 °C range. 3.3 Ultrafiltration experiments Ultrafiltration tests were performed using a dead-end filtration cell (200 mL, Amicon 8200, Millipore) at 10 °C. The cell was connected to a pressurized N2 tank to maintain constant transmembrane pressure of 1 bar. The ultrafilters were regenerated cellulose membrane disks (Ultracel® PL-100, Millipore), 63.5 mm in diameter, with the nominal molecular weight cutoff of 100 kDa. Permeate was collected in a reservoir placed on a digital balance (JA 2003B, Chrom Tech) connected to a data acquisition PC. Permeate mass data was recorded at 0.25 s intervals and converted to permeate flux based on the membrane area (28.7 cm2) and water density (0.986 g/mL). 3.4. Water quality analysis UV254 absorption was measured using M501 Single Beam Scanning UV/VIS spectrophotometer (CAMSPEC, Sawston, UK) with 1 cm optical path length and photometric repeatability of ± 0.0002 Abs. Prior to measurements, all water samples were filtered through a 0.45 µm syringe filter and average values were obtained by triplicate measurements. Zeta-potential values were measured at 25°C using a Malvern Zetasizer Nano Series Nano-ZS (Malvern Instruments Inc.). Dissolved organic carbon (DOC) content in water samples was determined using the persulfate oxidation method (DR 1900, Hach). 3. Results and Discussion 3.1. Water quality 5 © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0 - UV254 absorbance by the feed water was reproducibly very low: 0.202 ± 0.007 m 1 and 0.254 ± 0.003 m-1 for samples A and B respectively. The measured values of DOC were also low - 0.17 ± 0.06 (sample A) and 0.20 ± 0.10 mg/L (sample B), which was at or below the detection limit (0.3 mg/L) of the DR 1900 instrument. We used the DOC value of 0.2 mg/L to obtain an estimate of the specific UV254 absorbance (SUVA254) for the water samples. SUVA254 is known to positively correlate with the percent aromaticity of dissolved organics in natural water [5, 6]: SUVA254 values above 4 L/(mgm) are taken to indicate that organic constituents [7] are predominantly hydrophobic .
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