Oxidative Efficiency of Ozonation Coupled with Electrolysis for Treatment of Acid Wastewater

Abstract

Establishment of an ozone-based advanced oxidation process (AOPs-O₃) for effective treatment of acid wastewater is an important and difficult task. The process of ozonation coupled with electrolysis (electrolysis-ozonation, E-O₃) has been reported to effectively degrade pollutants in neutral solution. We studied the efficiency of E-O₃ for degradation of acetic acid (HAc, an ozone inert chemical) in acid solution and found that E-O₃ had high oxidative efficiency at pH less than 3. For example, 52.2% of 100 mg·L^-1 HAc could be removed by E-O₃ in 120 min at pH 1.0, but only 2.2% and 3.5% by electrolysis and ozonation, respectively. Although the efficiency of E-O₃ decreased with the increase of acidity of solution, it still remained relatively high even at pH 0. An aromatic compound of acetophenone could also be effectively degraded by E-O₃ at pH 1.0. The results indicate that electrons can transfer from cathode to dissolved ozone or oxygen in acidic solution, thus resulting in generation of reactive species, e.g. hydroxyl radicals. A real acidic wastewater was also effectively pretreated by E-O₃. This study provides a promising AOPs-O₃ for treatment of acid wastewaters.

Keywords

electrolysis / ozone / acetic acid / efficiency / acid wastewater

References

[1] Hunt A J. Vanadium-catalysed oxidative bromination using dilute mineral acids and hydrogen peroxide: An option for recycling waste acid streams[J]. Org. Process Res. dev., 2000, 4(4): 270-274.

[2] Hoigné J, Bader H. Rate constants of reactions of ozone with organic and inorganic compounds in water-I: ociating organic compounds[J]. Water. Res., 1983, 17(2): 173-183.

[3] Wang N, Tong Z, Zhang G, Peng W. A review on Fenton-like processes for organic wastewater treatment[J]. J. Environ. Chem. Eng., 2016, 4(1): 762-787.

[4] Neyens E, Baeyens J. A review of classic Fenton’s peroxidation as an advanced oxidation technique[J]. J. Hazard. Mater., 2003, 98(1): 33-50.

[5] Lü X Y, Jin G P, Yuan D K, Ding Y F, Long P X. Improving generation of H₂O₂ and OH at coppernhexacyanocobal-tate/graphene/ITO composite electrode for degradation of levofloxacin in photo-electro-Fenton process[J]. Environ. Sci. Pollut. Res., 2021, 5: 1-12.

[6] Wu J J, Wu C C, Ma H W, Chang C C. Treatment of landfill leachate by ozone-based advanced oxidation processes chemosphere[J]. Chemosphere, 2004, 54(7): 997-1003.

[7] Legube B, Leitner N. Catalytic ozonation: a promising advanced oxidation technology for water treatment[J]. Catal. Today, 1999, 53(1): 61-72.

[8] Esplugas S, Giménez, Contreras S, Pascual E, Rodriguez M. Comparison of different advanced oxidation processes for phenol degradation[J]. Water Res., 2002, 36(4): 1034-1042.

[9] Wang Q W, Shen T D, Tong S P. Effect of iron oxide promoted sulfated zirconia on the oxidative efficiency of H₂O₂/O₃ for acetic acid degradation in strong acidic water[J]. Ind. Eng. Chem. Res., 2016, 55(46): 10513-10522.

[10] Goyal A, Srivastava V C, Kushwaha J P. Treatment of highly acidicwastewater containing high energetic compounds using dimensionally stable anode[J]. Chem. Eng. J., 2017, 325: 289-299.

[11] Kishimoto N, Morita Y, Tsuno H, Oomura T, Mizutani H. Advanced oxidation effect of ozonation combined with electrolysis[J]. Water Res., 2005, 39(19): 4661-4672.

[12] Yao W K, Rehman S W U, Wang H J, Yang H W, Yu G. Pilot-scale evaluation of micropollutant abatements by conventional ozonation, UV/O₃, and an electro-peroxone process[J]. Water Res., 2018, 138: 106-117.

[13] Zheng H S, Guo W Q, Wu Q L, Ren N Q, Chang J S. Electro-peroxone pretreatment for enhanced simulated hospital wastewater treatment and antibiotic resistance genes reduction[J]. Environ. Int., 2018, 115: 70-78.

[14] Saylor G L, Chao Z, Kupferle M J. Synergistic enhancement of oxidative degradation of atrazine using combined electrolysis and ozonation[J]. J. Water. Process. Eng., 2018, 21: 154-162.

[15] Ding Y L, Wang C, Yin F, X, Wu G Q, Tong S P. Quantitative investigation of the synergistic effect of electrolysis combined with ozonation for degradation of nitrobenzene[J]. Ozone Sci. Eng., 2019, 41(4): 351-357.

[16] Kishimoto N, Nakagawa T, Asano M, Abe M, Yamada M, Ono Y. Ozonation combined with electrolysis of 1, 4-dioxane using a two-compartment electrolytic flow cell with solid electrolyte[J]. Water Res., 2008, 42(1-2): 379-385.

[17] Kishimoto N, Nakagawa T, Okada H, Mizutani H. Effect of separation of ozonation and electrolysis on effective use of ozone in ozone-electrolysis process[J]. Ozone Sci. Eng., 2011, 33(6): 463-469.

[18] Wu D, Zhang R, Lu G, Lin Q H, Liu F L, Li Y. Degradation of octocrylene using combined ozonation and electrolysis process: optimization by response surface metho-dology[J]. Clean - Soil. Air. Water, 2017, 45(2): 1500664.

[19] Helz G R, Zepp R G, Crosby D G. Aquatic and surface photochemistry[M]. Lewis Publishers., 1994.

[20] Hoigné J, Bader H. Rate constants of reactions of ozone with organic and inorganic compounds in water—III. Inorganic compounds and radicals[J]. Water Res., 1985, 17(8): 993-1004.

[21] State Environmental Protection Administration(国家环保总局). Water and wastewater monitoring and analysis methods (Fourth edition)[M]. China Environmental Science Press(中国环境科学出版社), 2002.

[22] Bader H, Hoigné J, Hoigné。 Determination of ozone in water by the indigo method[J]. Water Res., 2013, 15(4): 449-456.

[23] Sellers R M. Spectrophotometric determination of hydrogen peroxide using potassium titanium (IV) oxalate[J]. An-alyst, 1980, 105: 950-954.

[24] Zhou Q (周琦), Zhang R (张蓉), Wang X H (王勋华), Ma C A (马淳安), Tong S P (童少平). Oxidative efficiency of the system of electrolysis coupled ozonation[J]. Envir. Sci.(环境科学), 2010, 31(9): 2080-2084.

[25] Ding Y L, Wang J J, Xu S S, Lin K Y A, Tong S P. Oxy-gen vacancy of CeO₂ improved efficiency of H₂O₂/O₃ for the degradation of acetic acid in acidic solutions[J]. Sep. Purif. Technol., 2018, 207: 92-98.

[26] Chen Y, Peng R F, Shen T D, Tong S P, Ma C A. promising ozone-based advanced oxidation process for effective generation of hydroxyl radicals in acidic solution[J]. Sep. Purif. Technol., 2015, 151(2): 269-275.

[27] Tomiyasu H, Fukutomi H, Gordon G. Kinetics and mechanism of ozone decomposition in basic aqueous solution[J]. Chem. Inform., 1985, 24(19): 2962-2966.