Treatment of oil field fracturing flowback wastewater based on 3D/O3 process
ZHANG Yi-xin1, CUI Xin-xin2, LIU Shu-qin1, ZHU Wei3, HAN Xia3, WANG Yu-jue2
1. School of Chemical and Environmental Engineering, China University of Mining and Technology, Beijing 100083, China; 2. School of Environment, Tsinghua University, Beijing 100084, China; 3. Sinopec Petroleum Engineering Co., Ltd., Dongying 257026, China
Abstract：In this study, a three-dimensional electrode/ozone (3D/O3) system was developed by combining ozonation with electrolysis using granular activated carbon (GAC) as the particle electrodes, the developed 3D/O3 system was then used to treat the fracturing flowback wastewater from Shengli oil field. The reaction mechanism of the 3D/O3 system and the effects of process parameters (e.g., current, ozone concentrations) on COD removal were investigated systematically. Results show that COD removal efficiency reached~78% after 3h of the 3D/O3 treatment, and could be maintained stably above 60% during 8cycles of operation. In comparison, 3D electrolysis and ozonation alone removed only~37% and 17% COD under similar reaction conditions. These results indicate that the 3D/O3 system effectively couples activated carbon adsorption, electrochemical oxidation, and catalytic ozonation to enhance hydroxyl radical generation to oxidize organic pollutants in the fracturing flowback wastewater and regenerate activated carbon. Therefore, it may provide a promising method to remove COD in hydraulic fracturing flowback wastewater.
张一欣, 崔欣欣, 刘淑琴, 祝威, 韩霞, 王玉珏. 三维电极耦合臭氧技术处理油田压裂返排液[J]. 中国环境科学, 2020, 40(5): 2270-2275.
ZHANG Yi-xin, CUI Xin-xin, LIU Shu-qin, ZHU Wei, HAN Xia, WANG Yu-jue. Treatment of oil field fracturing flowback wastewater based on 3D/O3 process. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(5): 2270-2275.
高挺,王伟华,王涛,等.油田返排液处理技术研究与应用[J]. 石油化工应用, 2016,35(11):72-76. Gao T, Wang W, Wang T, et al. Research and application of oilfield fracturing flowback wastewater technology[J]. Petrochemical Industry Application, 2016,35(11):72-76.
王顺武,赵晓非,李子旺,等.油田压裂返排液处理技术研究进展[J]. 化工环保, 2016,36(5):493-499. Wang S, Zhao X, Li Z, et al. Research progresses on treatment technologies of oilfield fracturing flow-back fluid[J]. Environmental Protection of Chemical Industry, 2016,36(5):493-499.
Moreira F C, Soler J, Fonseca A, et al. Electrochemical advanced oxidation processes for sanitary landfill leachate remediation:evaluation of operational variables[J]. Applied Catalysis B:Environmental, 2016,182:161-171.
Chaplin B P. Critical review of electrochemical advanced oxidation processes for water treatment applications[J]. Environmental Science:Processes and Impacts, 2014,16(6):1182-1203.
R. Backhurst J, M. Coulson J, Goodridge F, et al. A preliminary investigation of fluidized bed electrodes[M]. 1969.
汤哲人,陈泉源,邓东升,等.以黄铜矿作为颗粒三维电极的电Fenton氧化处理维尼纶废水中的COD研究[J]. 中国环境科学, 2017, 37(1):95-101. Tang Z, Chen Q, Deng D, et al. COD of vinylon waste-water oxidizing treatment by three-dimensional electrode electricity-fenton using brass copper grains[J]. China Environmental Science, 2017, 37(1):95-101.
Fockedey E, Van Lierde A. Coupling of anodic and cathodic reactions for phenol electro-oxidation using three-dimensional electrodes[J]. Water Research, 2002,36(16):4169-4175.
Wu Z, Cong Y, Zhou M, et al. p-Nitrophenol abatement by the combination of electrocatalysis and activated carbon[J]. Chemical Engineering Journal, 2005,106(1):83-90.
Zhang C, Jiang Y, Li Y, et al. Three-dimensional electrochemical process for wastewater treatment:A general review[J]. Chemical Engineering Journal, 2013,228:455-467.
Lücking F, Köser H, Jank M, et al. Iron powder, graphite and activated carbon as catalysts for the oxidation of 4-chlorophenol with hydrogen peroxide in aqueous solution[J]. Water Research, 1998,32(9):2607-2614.
Faria P C C, Órfão J J M, Pereira M F R. Activated carbon catalytic ozonation of oxamic and oxalic acids[J]. Applied Catalysis B:Environmental, 2008,79(3):237-243.
Yakout M S, Daifullah A M A, El-Reefy S. Adsorption of naphthalene, phenanthrene and pyrene from aqueous solution using low-cost activated carbon derived from agricultural wastes[M]. 2013.
R.M. Narbaitz, J. Cen Electrochemical regeneration of granular activated carbon[J]. Water Research, 1994,28:1771-1778.
Zhou M, Lei L. The role of activated carbon on the removal of p-nitrophenol in an integrated three-phase electrochemical reactor[J]. Chemosphere, 2006,65(7):1197-1203.
A. Ban, A. Schafer, H. Wendt. Fundamentals of electrosorption on activated carbon for wastewater treatment of industrial effluents[J]. Journal of Applied Electrochemistry, 1998,28(3):227-236.
Zhan J, Li Z, Yu G, et al. Enhanced treatment of pharmaceutical wastewater by combining three-dimensional electrochemical process with ozonation to in situ regenerate granular activated carbon particle electrodes[J]. Separation and Purification Technology, 2019,208:12-18.
Foo K Y, Hameed B H. A short review of activated carbon assisted electrosorption process:an overview, current stage and future prospects[J]. Journal Hazardous Materials, 2009,170(2/3):552-559.
Lee Y, Gerrity D, Lee M, et al. Prediction of micropollutant elimination during ozonation of municipal wastewater effluents:use of kinetic and water specific information[J]. Environmental Science and Technology, 2013,47(11):5872-5881.
Yao W, Ur Rehman S W, Wang H, et al. Pilot-scale evaluation of micropollutant abatements by conventional ozonation, UV/O3, and an electro-peroxone process[J]. Water Research, 2018,138:106-117.