276 Journal of the Japan Petroleum Institute, 57, (6), (2014) [Regular Paper] Examinations of Effective Coagulant for Polymer Flood Produced W

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1 276 Journal of the Japan Petroleum Institute, 57, (6), (2014) [Regular Paper] Examinations of Effective Coagulant for Polymer Flood Produced Water and Pilot Trial in Oman Keisuke KOJIMA 1), Masaharu TASAKI 1), Kazuo OKAMURA 1), Mark SUEYOSHI 1), and Rashid S. AL-MAAMARI 2) 1) Institute of Technology, Shimizu Corp., Etchujima, Koto-ku, Tokyo , JAPAN 2) Petroleum & Chemical Engineering Dept., Sultan Qaboos University, P.O. Box 33, Al-Khoudh, PC 123, SULTANATE of OMAN (Received July 30, 2014) Polymer flooding is being used as an enhanced oil recovery (EOR) method in Oman. In polymer flooding, injection water of increased viscosity reduces mobility difference between water and oil, thereby improving sweep and oil recovery. The quality of polymer flood produced water (PFPW) is different from produced water (PW) without polymer, and various techniques are being studied for the effective treatment of PFPW. In this paper, the effects of two different coagulants, aluminum sulfate (AS) and polyaluminum chloride (PAC), were examined for the treatment of PFPW. Laboratory tests indicated that the effects of coagulation by PAC were decreased when used for PFPW, compared to PW. This decrease was attributable to interaction of polymer and inorganic carbon, rather than to high ph or high alkalinity alone. On the other hand, laboratory tests indicated that AS would be an effective alternative coagulant for PFPW treatment. Based on these results, a treatment trial with actual PFPW, was conducted with a pilot plant. The pilot trials confirmed that with appropriate level of AS addition and a second coagulation step, PFPW could be effectively treated with AS. Keywords Polymer flood, Produced water, Enhanced oil recovery, Coagulation, Polyaluminum chloride, Aluminum sulfate 1. Enhanced Oil Recovery: EOR1970 EOR thermal recovery 1),2) gas injection 3),4) chemical flood 5)9) 5)7) 8),9) OPEC 2000 EOR ) EOR CO 2 11) Produced Water: DOI: dx.doi.org/ /jpi To whom correspondence should be addressed. tasakim@shimz.co.jp PW ),13) PW EOR PW 14),15) EOR Polymer Flood Produced Water: PFPW PW PFPW PW 16) PFPW 17)23) PFPW

2 277 Table 1 Water Quality of Tested Produced Water (PW) and Polymer Flood Produced Water (PFPW) from the Same Oilfield (for laboratory tests) PW PFPW-1 (for pilot trial) PFPW-2 salinity [%] ph conductivity [S/m] turbidity [FTU] viscosity [cp] M alkalinity SS a) 190 COD Mn 31 - a) 200 c) COD Cr 86 - a) 190 TOC IC Oil_TD500 d) Oil_nHex e) 15 - a) 180 anion Cl NO 3 ND b) ND b) ND b) 3 PO 4 ND b) ND b) ND b) 2 SO cation Na NH K Mg Ca Total nitrogen a) 83 Total phosphate a) phenols a) B F Al ND b) - a) 0.17 a) -: no data. b) ND: not detected. c) measured by PACKTEST COD High Range (Kyoritsu Chemical-Check Lab., Corp.). d) measured by TD-500 (TURNER DESIGNS, USA) extracted in n-hexane. e) weight of n-hexane extracts. PFPW PW polyaluminum chloride: PAC aluminum sulfate: AS 50 m 3 /day PFPW PFPW PW PFPW PW PFPW M PW PFPW PW PFPW Table 1PFPW PW PW 7 TOC: Total Organic CarbonPFPW PW PFPW-1 M 100 mg/l PFPW-2 Corrugated Plate Interceptor: CPI PW PFPW AS PAC PW PFPW-1 AS PAC Table 2Test-1 Test-3 AS PAC A-103T; 2 mg/l

3 PFPW AS PAC PFPW AS PAC PFPW AS PAC 24)26) AS PAC Table 3Test-4 Test-10 M 0.40 % Test-4 M EOR Flopaam 3630S; SNF s.a.s company 500 mg/l Flopaam 3630S 2000 dalton 27),28) A 100 mg/l Table 2 Conditions of Coagulation Tests for PW and PFPW Solvent Oil a) Polymer b) Test-1 PW c) - Test-2 PW c) 500 Test-3 PFPW-1 d) - a) crude oil of site M was added and shaken overnight. b) Flopaam 3630S. c) does not contain polymer from EOR site. d) contains polymer from EOR site. M M 5 mm1 M1 mol dm 3 ph8.0 ph8.0 1 mm ph TOC Inorganic Carbon: IC M ph PFPW PW TOC AS PAC IC IC 500 mg/l mm Table 4; Test-11 Test-17 A 500 mg/l Table 5; Test-18 Test-22 IC Test-11 Test-17 TOC Test-18 Test-22 TOC Solvent Oil a) Table 3 Results of Coagulation Tests for Oil, Polymer and Alkalinity Polymer b) NaHCO 3 [mm] Effective coagulant concentration TOC removal and turbidity c) Test-4 Tap water PAC (TOC removal, %) (100) (turbidity, FTU) Test-5 UPW d) PAC (TOC removal, %) (300) (turbidity, FTU) Test-6 UPW d) PAC (TOC removal, %) (50) (turbidity, FTU) Test-7 UPW d) AS (TOC removal, %) (400) ND f) 18 (turbidity, FTU) Test-8 UPW d) PAC (TOC removal, %) (300) (turbidity, FTU) Test-9 UPW d) AS (TOC removal, %) (400) (turbidity, FTU) Test-10 UPW d) (ph8) e) PAC (TOC removal, %) (300) (turbidity, FTU) a) bunker A was added and mixture was shaken overnight. b) Flopaam 3630S. c) at same concentration for both coagulants. d) ultrapure water. e) ph adjusted by NaOH. f) ND: not detevted. AS PAC

4 279 NaHCO 3 a) [mm] Table 4 Results of Coagulation Tests as for Various Concentrations of M-alkalinity Coagulant Coagulant conc. TC IC TOC TOC removal [%] Turbidity [FTU] ph M-alkalinity b) Test before coagulation AS PAC Test before coagulation AS PAC Test before coagulation AS PAC Test before coagulation AS PAC Test before coagulation ND c) AS PAC ND c) Test before coagulation ND c) AS ND c) PAC ND c) Test before coagulation ND c) AS PAC ND c) All tests contain 500 mg/l polymer (Flopaam 3630S), and solved in ultrapure water. The bold-faced rows show the results at effective coagulant concentrations for each NaHCO 3 concentration. a) NaHCO 3 : final concentration (mm). b) M-alkalinity: mg-caco 3 /L. c) ND: not detected PFPW AS PAC mg/l

5 280 Table 5 Results of Coagulation Tests for Various Concentrations of M-alkalinity with Oil a) NaHCO 3 [mm] Coagulant Coagulant conc. TC IC TOC TOC removal [%] Turbidity [FTU] ph M-alkalinityb) Oil Oil removal [%] Test before coagulation AS ND c) 100 PAC ND c) ND c) ND c) ND c) 100 Test before coagulation AS ND c) ND c) 100 PAC ND c) ND c) ND c) ND c) 100 Test before coagulation AS ND c) ND c) ND c) 100 PAC ND c) ND c) 100 Test before coagulation AS ND c) ND c) 100 PAC ND c) ND c) 100 Test before coagulation AS ND c) ND c) ND c) 100 PAC ND c) ND c) 100 All tests contain 500 mg/l polymer (Flopaam 3630S), and solved in ultrapure water. The bold-faced rows show the results at effective coagulant concentrations for each NaHCO 3 concentration. a) NaHCO 3 : final concentration (mm). b) M-alkalinity: mg-caco 3 /L. c) ND: not detected. A-103T 2 mg/l AS PAC PFPW AS AS mg/l A-103T 1 mg/l PFPW

6 281 1: Raw water tank (20 m 3 ), 2: Mixing tank-1 (0.4 m 3 ), 3: Mixing tank-2 (0.4 m 3 ), 4: Flotation tank (1.4 m 3 ), 5: Filtration tower (0.4 m 3 ), 6: Adsorption tower (0.4 m 3 ), 7: Treated water tank (4 m 3 ), 8: Coagulant tank (200 L), 9: Spare chemical tank (200 L), 10: Polymer tank (1 m 3 ), 11: PSA, 12: Microbubble pump, 13: Flotation rake, 14: Scum tank, 15: Scum dewatering press. Fig. 1 Pilot Plant Process Flow RW: raw water (PFPW), NF: nitrogen flotation, 2F: second coagulation/floculation, AF: anthracite filtration, AC: activated carbon adsorption. Fig. 2 PFPW Trial Treatment Process Flow 5 mm 14),15) Fig. 1 PFPW 12 AS AS PW PSA SS KW; PFPW RW- NF-2F- AF-AC Fig m 3 /day COD Mn HI 93703; TOC IC TOC-V CSH ; M WAD-AL-M; ph ph ToupH D; M H-997 Fourier Transform Infrared Spectroscopy: FTIRFTIR-8400; FTIR 29) A TD- 500Turner Designs Hydrocarbon Instruments COD Mn WAK-CODD WAK-CODWAK-CODH;

282 a) coagulation in PW without EOR polymer addition, b) coagulation in PW with EOR polymer addition, c) coagulation in PFPW. Fig. 3 Coagulation Tests by AS and PAC 3. 3. 1.

7 282 a) coagulation in PW without EOR polymer addition, b) coagulation in PW with EOR polymer addition, c) coagulation in PFPW. Fig. 3 Coagulation Tests by AS and PAC PFPW PW PFPW AS PAC Table 2 PW PFPW-1 AS PAC Fig. 3PW PFPW-1 55 FTU37 FTU AS PAC Fig. 3 PWFig. 3 a) PAC 300 mg/l AS 500 mg/l PW Fig. 3 b) PFPW-1Fig. 3 c)as PAC PW PAC AS PAC AS TOC PFPW AS PAC Table 3Table 3 PAC AS effective coagulant TOC effective coagulant Table 3 Test-4Test-6 AS PAC Test-4100 mg/l AS PAC Gao et al ) Test-4Test-8 PAC 100 mg/l 300 mg/l PAC AS TOC 400 mg/l

-8, -9 TOC 3. 1. 3. AS PAC IC Table 4 AS PAC 0 1.0 mm 0 mm 300 mg/l PAC TOC 0.2 mm AS PAC TOC 0.5 mm AS TOC Table 4 Fig.

8 283 The right figure b) is an enlarged figure of the boxed area in left figure a). Fig. 4 Change in IC at Optimum Concentrations of Each Coagulant 1 2 _ COOH _ AS PAC AS AS PAC AS PAC AS PAC PAC AS ph Test-10PAC AS TOC IC PW PAC AS Test-4, -6, -8, -9 TOC AS PAC IC Table 4 AS PAC mm 0 mm 300 mg/l PAC TOC 0.2 mm AS PAC TOC 0.5 mm AS TOC Table 4 Fig. 5 Change in IC at Optimum Concentrations of Each Coagulant (laboratory test with oil) IC Fig. 4 Fig. 4 IC 0 25 mg/l IC 2 5 mg/l PAC AS mm Table 5 Fig. 5 IC 0.2 mm PAC 0.5 mm PAC AS Fig. 5 IC 2 mg/l 5 mg/l PAC AS TOC Fig mm Table 5 TOC AS Fig. 6 AS

284 Top figure shows coagulation by PAC, bottom shows coagulation by AS. Fig.

0 mm NaHCO 3 with Oil From the left, NF (before 2nd addition), AS 30, 60, 90, 120 mg/l with

9 Jar Tests for 2nd AS Addition Top figure shows coagulation by AS, bottom shows coagulation

Fig. 7AS 600 mg/l PAC 700 mg/l PFPW PAC AS AS AS AS 500 mg/l 850 mg/l Fig.

9 284 Top figure shows coagulation by PAC, bottom shows coagulation by AS. Fig. 8 Water Quality at Different AS Concentrations Fig. 6 Coagulation Test Results under 1.0 mm NaHCO 3 with Oil From the left, NF (before 2nd addition), AS 30, 60, 90, 120 mg/l with polymer 1 mg/l. Fig. 9 Jar Tests for 2nd AS Addition Top figure shows coagulation by AS, bottom shows coagulation by PAC. Fig. 7 Coagulation Jar Tests for AS and PAC for Pilot Trial PAC PFPW Fig. 7AS 600 mg/l PAC 700 mg/l PFPW PAC AS AS AS AS 500 mg/l 850 mg/l Fig. 8 AS 700 mg/l 700 mg/l AS 700 mg/l AS AS Fig. 9 Fig. 9 AS 90 mg/l AS 90 mg/l Table 6 COD Mn Fig. 10 RW NF 2F NF 2F 90 % COD Mn NF 40 % AF AC COD Mn SS COD Mn EOR 4. EOR PFPW 1PFPW PW PAC PFPW PAC AS

285 Table 6 Water Quality through Different Stages of Treatment during PFPW Pilot Trial RW NF 2F AF AC salinity [%] 0.36 0.36 0.35 0.36 0.35 ph 7.49 6.78 6.83 6.87 7.

10 285 Table 6 Water Quality through Different Stages of Treatment during PFPW Pilot Trial RW NF 2F AF AC salinity [%] ph turbidity [FTU] viscosity [cp] SS a) COD Mn COD Cr TOC IC Oil_TD Oil_nHex anion Cl NO 3 ND b) ND b) ND b) ND b) ND b) 3 PO 4 ND b) ND b) ND b) ND b) ND b) 2 SO cation Na NH K Mg Ca Total nitrogen Total phosphate phenols B F Al a) measured by PACKTEST COD High Range (Kyoritsu Chemical- Check Lab., Corp.). b) ND: not detected. Fig. 10 PFPW Trial Water Quality through Different Stages of Treatment 2 PFPW AS PAC IC EOR AS PAC ph AS PAC PAC 3500 mg/l IC 25 mg/l PAC AS 4 PFPW AS II References 1) Kovscek, A. R., J. Petrol. Sci. Eng., 98-99, 130 (2012). 2) Chaipornkaew, M., Wongrattapitak, K., Chantarataneewat, W., Boontaeng, T., Opdal, S. T., Maneeintr, K., Procedia Earth and Planetary Science, 6, 326 (2013). 3) Al-Abri, A., Sidiq, H., Amin, R., J. Natural Gas Sci. Eng., 9, 166 (2012). 4) Belhaj, H., Abukhalifeh, H., Javid, K., J. Petrol. Sci. Eng., 111, 144 (2013). 5) Babadagli, T., Al-Bemani, A., Boukadi, F., Al-Maamari, R., J. Petrol. Sci. Eng., 48, 37 (2005). 6) Lu, J., Weerasooriya, U. P., Pope, G. A., Fuel, 124, 76 (2014). 7) Ko, K. M., Chon, B. H., Jang, S. B., Jang, H. Y., J. Ind. Eng. Chem., 20, 228 (2014). 8) Wang, Z., Le, X., Feng, Y., Zhang, C., J. Petrol. Sci. Eng., 111, 139 (2013). 9) Algharaib, M., Alajmi, A., Gharbi, R., J. Petrol. Sci. Eng., 115, 17 (2014). 10) Japan Petroleum Energy Center, JPEC Report, No. 33, 1-16 (2013)., JPEC, No. 33, 1-16 (2013). 11) Hamada, H., Japan Oil, Gas and Metals National Corp., oilgas-info.jogmec.go.jp/report_pdf.pl?pdf=1312_out_h_00_ Oman_Resource_trend_2013HPUpload%2epdf&id=5043, (2013).,, JOGMEC, oilgas-info.jogmec.go.jp/report_pdf.pl?pdf=1312_out_h_00_ Oman_Resource_trend_2013HPUpload%2epdf&id=5043, (2013). 12) Al-Bemani, A., Proc. of International Symposia on ESAA & DG, Abu Dhabi, UAE (2001). 13) Asada, M., Hirayama, A., Sueyoshi, M., Kawaguchi, M., Ishikawa, A., Maegaito, M., Okamura, K., Al-Maamari, R., Al- Bemani, A., Al-Mazrui, S., Proc. of Environment Symposium on Sustainable Development and Climate Change, Doha, Qatar (2007). 14) Tasaki, M., Okamura, K., Sueyoshi, M., Al-Maamari, R. S., J. Jpn. Petrol. Inst., 56, (6), 406 (2013). 15) Al-Maamari, R. S., Sueyoshi, M., Tasaki, M., Okamura, K., Al-Lawati, Y., Nabulsi, R., Al-Battashi, M., SPE J., 3, 56 (2014). 16) Ma, B., Gao, B., Yue, Q., J. Petrol. Sci. Eng., 110, 27 (2013). 17) Deng, S., Bai, R., Chen, J. P., Jiang, Z., Yu, G., Zhou, F., Chen, Z., Sep. Purif. Technol., 29, 207 (2002). 18) Zhao, X., Liu, L., Wang, Y., Dai, H., Wang, D., Cai, H., Sep. Purif. Technol., 62, 199 (2008). 19) Bao, M., Chen, Q., Li, Y., Jiang, G., J. Hazard. Mater., 184, 105 (2010). 20) Zhang, Y., Gao, B., Lu, L., Yue, Q., Wang, Q., Jia, Y., J. Petrol. Sci. Eng., 74, 14 (2010). 21) Gao, B., Jia, Y., Zhang, Y., Li, Q., Yue, Q., J. Environ. Sci., 23, 37 (2011).

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