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PETROLEUM SCIENCE AND TECHNOLOGY · 2022 · IF 1.695

Effect of supercritical CO2 flooding on the produced water quality and performance of the scale inhibitors in a typical tight sandstone oilfield

Kaixiang Cui,Yufei Xia,Linlin Tian,Shuai Wang,Yongyao He

In order to enhance oil recovery, supercritical CO2 (scCO2) flooding has been applied in many oilfields to extract oil and gas post primary recovery. However, it causes serious scaling problems in the reservoir, oil well and production tubing. In this article, the produced water quality before and after scCO2 flooding in carbonate reservoirs are analyzed. The scaling trend of produced water before and after scCO2 flooding was calculated by using the Davis-stiff saturation index and Ryznar stability index methods. Static experiments and scanning electron microscope (SEM) are used to study the scale inhibition performance and mechanism of HEDP, ATMP, MA-AA, and PAA on CaCO3 in produced water before and after scCO2 flooding. The results show that after scCO2 flooding, the quality of produced water changes obviously, thus the scaling trend of produced water increases, the growth of CaCO3 crystal is affected and the scale inhibition efficiency of conventional scale inhibitors decreases.

CAS / MDL: 2809-21-4 6419-19-8
研究领域: 石油工程 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Membrane fouling alleviation by combination of sodium percarbonate oxidation and coagulation during microfiltration of shale gas produced water

Haiqing Chang,Naiming Liu,Fangshu Qu,Xiaoxiang Cheng,Zhiwei Zhou,Ying Liang,Ying Yu,Heng Liang

Membrane fouling is the Achilles heel of membrane-based technologies. Severe membrane fouling occurs when a single microfiltration (MF) membrane is used to treat shale gas produced water (SGPW). Activated by Fe(II), sodium percarbonate (SPC) oxidation combined with aluminum sulfate coagulation was used in this study to evaluate the alleviation of MF fouling for the treatment of two typical SGPW samples with different water quality characteristics from Sichuan Basin. Results showed that pre-treated by oxidation and coagulation, more than 88% of turbidity, 11%–23% of UV 254 , and 11%-36% of DOC were removed. With the increase in SPC dosage, there was a decrease in fluorescent organics, primarily reducing soluble microbial by-product-like components by up to 37.0% for sample 1 and aromatic protein and soluble microbial by-product-like components by up to 66.7% and 71.2% for sample 2, respectively. Compared to low normalized fluxes (2%-6%) for the raw SGPW, 61%-79% of normalized fluxes were obtained using the combination of 10 mmol/L SPC and 0.9 mmol/L Al 2 (SO 4 ) 3 ·18H 2 O. There was a general evolution of complete blocking to intermediate blocking or cake layer filtration for membrane fouling mechanism. Scanning electron microscopy observation, deposited foulants on membrane surface and Fourier transform infrared analysis further confirmed the superior performance of the combination of SPC oxidation and coagulation. Correlation analysis showed that UV 254 ( R 2  = 0.79–0.95) played the most significant role in membrane fouling. Overall, this combined pretreatment process showed a great potential in MF membrane fouling control during the treatment of SGPW.

CAS / MDL: 15630-89-4
研究领域: 环境科学 · 水处理工程
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Energies · 2021 ·Vol. 15 ·期 1 ·153 · IF 3.004

Reusing Flowback and Produced Water with Different Salinity to Prepare Guar Fracturing Fluid

Erdong Yao,Hang Xu,Yuan Li,Xuesong Ren,Hao Bai,Fujian Zhou

Economical and environmental concerns have forced the oil and gas industry to consider reusing flowback and produced water for fracturing operations. The major challenge is that the high-salinity of flowback water usually prevents its compatibility with several fracturing fluid additives. In this paper, the authors explored an economic and effective method to prepare guar fracturing fluids with different salinity waters. The main research idea was to use chelating agents to mask metal ions, such as calcium and magnesium, that are harmful to crosslinking. Firstly, a complexometric titration test was conducted to measure the chelating ability of three chelating agents. Secondly, through viscosity, crosslinking, and hanging tests, it was verified that the complex masking method could cope with the problem of high-valence metal ions affecting crosslinking. Thirdly, the preferred chelating agent was mixed with several other additives, including thickeners, crosslinkers, and pH regulators, to prepare the novel guar fracturing fluid. The comprehensive performances of the novel fluid system were tested such as temperature and shear resistance, friction reduction, gel-breaking performance, and core damage rate. The results show that the organophosphate chelating agent (i.e., CA-5) had the greatest ability to chelate calcium and magnesium ions. There was a good linear relationship between the dosage of CA-5 and the total molar concentration of calcium and magnesium ions in brine water. The main mechanism was that the chelating agent formed a complex with calcium and magnesium ions at a chelation ratio of 1:5. The test results of the comprehensive performance evaluation indicate that the prepared guar fracturing fluid met the requirements for field application, and the lower the salinity of the flowback water, the more it is economical and effective.Keywords:flowback and produced water;chelating agent;complex masking method;crosslinker;chelation ratio

研究领域: 石油工程 · 环境科学
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WATER RESEARCH · 2024 · IF 11.4

Improving membrane distillation performance by Fe(II) activated sodium percarbonate oxidation during the treatment of shale gas produced water

Suhua Gu,Fangshu Qu,Dan Qu,Zhongsen Yan,Yuchuan Meng,Ying Liang,Haiqing Chang,Heng Liang

Membrane distillation (MD) offers promise for recycling shale gas produced water (SGPW), while membrane fouling is still a major obstacle in standalone MD. Herein, sodium percarbonate (SPC) oxidation was proposed as MD pretreatment, and the performance of the single MD, SPC-MD hybrid process and Fe(II)/SPC-MD hybrid process for SGPW treatment were systematically evaluated. Results showed that compared to raw SGPW, the application of SPC and Fe(II)/SPC led to the decrease of the fluorescent organics by 28.54 % and 54.52 %, respectively. The hydrophobic fraction decreased from 52.75 % in raw SGPW to 37.70 % and 27.20 % for SPC and Fe(II)/SPC, respectively, and the MD normalized flux increased from 0.19 in treating raw SGPW to 0.65 and 0.81, respectively. The superiority of SPC oxidation in reducing the deposited membrane foulants and restoring membrane properties was further confirmed through scanning electron microscopy observation, attenuated total reflection fourier transform infrared, water contact angle and surface tension analyses of fouled membranes. Correlation analysis revealed that hydrophobic/hydrophilic matters and fluorescent organics in SGPW took a crucial role in MD fouling. The mechanism of MD fouling mitigation by Fe(II)/SPC oxidation was attributed to the decrease in concentrations and hydrophobicity of organic by synergistic oxidation, coagulation and adsorption.

CAS / MDL: 816-94-4
研究领域: 环境科学 · 化学工程
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RSC Advances · 2017 ·Vol. 7 ·期 77 ·48904-48912 · IF 3.108

Surface modification of piperazine-based nanofiltration membranes with serinol for enhanced antifouling properties in polymer flooding produced water treatment

Ruijun Zhang,Shuili Yu,Wenxin Shi,Xiaoying Wang,Jun Cheng,Zhiqiang Zhang,Li Li,Xian Bao,Bing Zhang

In order to deal with the membrane fouling problem when treating the polymer flooding produced water (PFPW) with a typical thin film composite (TFC) nanofiltration (NF) membrane, a facile and effective serinol surface modification method has been introduced in this study, which is based on the membrane fouling mechanism proposed in our previous research. Serinol molecules were grafted on the nascent piperazine-based PA-TFC membrane through the acylation reaction between the serinol molecule’s amino group and the nascent membrane’s residual acyl chloride group. A series of characterizations indicated that this modification process could enhance membrane hydrophilicity and decrease the surface carboxyl density without changing the membrane’s morphology. Compared with the unmodified PA-TFC membrane, the serinol-grafted PA-TFC membrane had higher water permeability, stronger antifouling ability and equivalent solute rejection, which would be rather meaningful for improving membrane performance when treating PFPW.

研究领域: 环境科学 · 材料科学 · 化学工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Simultaneous detection of transcribed functional assA gene and the corresponding metabolites of linear alkanes (C4, C5, and C7) in production water of a low-temperature oil reservoir

Jin-Feng Liu,Yu-Wei Lu,Lei Zhou,Wei Li,Zhao-Wei Hou,Shi-Zhong Yang,Xiao-Lin Wu,Ji-Dong Gu,Bo-Zhong Mu

Methanogenic hydrocarbon degradation is an important biogeochemical process in oil reservoirs; however, genomic DNA-based analysis of microorganisms and metabolite detection are not conclusive for identification of the ongoing nature of this bioprocess. In this study, a suite of analyses, involving the study of microbial community and selective gene quantification of both genomic DNA and RNA together with signature metabolites, were performed to comprehensively advance the understanding of the methanogenic biodegradation of hydrocarbons in a low-temperature oilfield. The fumarate addition products for alkanes—C 4 , C 5 , and C 7 -alkylsuccinates—and transcribed assA and mcrA genes were simultaneously detected in the production water sample, providing robust and convincing evidence for both the initial activation of n -alkanes and methane metabolism in this oilfield. The clone library of assA gene transcripts showed that Smithella was active and most likely responsible for the addition of fumarate to n -alkanes, whereas Methanoculleus and Methanothrix were the dominant and active methane-producers via CO 2 reduction and acetoclastic pathways, respectively. Additionally, qPCR results of assA and mcrA genes and their transcribed gene copy numbers revealed a roughly similar transcriptional activity in both n -alkanes-degraders and methane producers, implying that they were the major participants in the methanogenic degradation of n -alkanes in this oilfield. To the best of our knowledge, this is the first report presenting sufficient speculation, through detection of signature intermediates, corresponding gene quantification at transcriptional levels, and microbial community analysis, of methanogenic degradation of n -alkanes in production water of an oil reservoir.

研究领域: 微生物学 · 环境基因组学 · 生物地球化学 · 烃类生物降解
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WATER RESEARCH · 2025 · IF 12.4

Role of multivalent iron in enhancing sodium percarbonate oxidation for alleviating membrane distillation fouling caused by shale gas produced water

Haiqing Chang,Yuan Huang,Suhua Gu,Xiaoxiang Cheng,Fangshu Qu

Membrane distillation (MD) shows significant potential for treating shale gas produced water, yet membrane fouling remains a persistent challenge in conventional MD systems. This study investigates an innovative pretreatment approach using sodium percarbonate (SPC) oxidation combined with various iron-based catalysts, systematically evaluating five distinct treatment processes, including standalone MD and four hybrid systems incorporating iron species. The experimental results demonstrated progressive improvement across all pretreatment methods, with the most effective Fe(VI)/Fe(II)/SPC-MD hybrid process achieving a 27.28% reduction in fluorescent organics, a decrease in hydrophobic fraction from 52.19% to 39.97%, and a notable enhancement in normalized flux from 0.42 to 0.79 compared to untreated shale gas produced water. Comprehensive membrane characterization through advanced analytical techniques, including electron microscopy, infrared spectroscopy, and surface property measurements, conclusively demonstrated the effectiveness of these oxidation pretreatments in mitigating foulant deposition and preserving membrane performance. Statistical analysis highlighted hydrophobic, hydrophilic organic components, and organics along with coagulation effects as primary contributors influencing membrane fouling. The superior performance of the combined Fe(VI)/Fe(II)/SPC oxidation system stems from its multifaceted mechanism that simultaneously leverages oxidative degradation, coagulation, and adsorption processes to reduce both organic concentration and hydrophobicity, thereby significantly alleviating membrane fouling.

CAS / MDL: 7782-63-0 816-94-4
研究领域: 环境工程 · 化学工程 · 水处理技术 · 膜科学 · 高级氧化工艺
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WATER RESEARCH · 2024 · IF 11.4

Ferrate(VI)-based oxidation for ultrafiltration membrane fouling mitigation in shale gas produced water pretreatment: Role of high-valent iron intermediates and hydroxyl radicals

Xiaoxiang Cheng,Dongshun Sai,Xinsheng Luo,Haiqing Chang,Peijie Li,Jingtao Xu,Daoji Wu,Heng Liang

Ultrafiltration (UF) is increasingly used in the pretreatment of shale gas produced water (SGPW), whereas severe membrane fouling hampers its actual operation. In this work, ferrate(VI)-based oxidation was proposed for membrane fouling alleviation in SGPW pretreatment, and the activation strategies of calcium peroxide (CaO 2 ) and ultraviolet (UV) were selected for comparison. The findings indicated that UV/Fe(VI) was more effective in removing fluorescent components, and the concentration of dissolved organic carbon was reduced by 24.1 %. With pretreatments of CaO 2 /Fe(VI) and UV/Fe(VI), the terminal specific membrane flux was elevated from 0.196 to 0.385 and 0.512, and the total fouling resistance diminished by 52.7 % and 76.2 %, respectively. Interfacial free energy analysis indicated that the repulsive interactions between pollutants and membrane were notably enhanced by Fe(VI)-based oxidation, thereby delaying the deposition of cake layers on the membrane surface. Quenching and probe experiments revealed that high-valent iron intermediates (Fe(IV)/Fe(V)) played significant roles in both CaO 2 /Fe(VI) and UV/Fe(VI) processes. Besides, hydroxyl radicals ( • OH) were also important reactive species in the UV/Fe(VI) treatment, and the synergistic effect of Fe(IV)/Fe(V) and • OH showed a positive influence on SGPW fouling mitigation. In general, these findings establish a theoretical underpinning for the application of Fe(VI)-based oxidation for UF membrane fouling mitigation in SGPW pretreatment.

研究领域: 环境工程 · 水处理 · 膜技术 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Characterization of microbial communities and functions in shale gas wastewaters and sludge: Implications for pretreatment

Shangbo Zhou,Shuchan Peng,Zhiqiang Li,Daijun Zhang,Yantao Zhu,Xingquan Li,Mingyu Hong,Weichang Li,Peili Lu

As hydraulic fracturing (HF) practices keep expanding in China, a comparative understanding of biological characteristics of flowback and produced waters (FPW) and sludge in impoundments for FPW reserve will help propose appropriate treatment strategies. Therefore, in this study, the microbial communities and functions in impoundments that collected wastewaters from dozens of wells were characterized. The results showed that microbial richness and diversity were significantly increased in sludge compared with those in FPW. The vast majority of microorganisms found in FPW and sludge are organic degraders, providing the possibility of using these indigenous microorganisms to biodegrade organic compounds. Our laboratory findings first show that wastewater pretreatment using these microorganisms was effective, and organic compounds in FPW from different shale formations were removed by 35–68% within 72 h in a wide temperature range (8 – 30 ℃). Meanwhile, highly toxic compounds such as phthalate esters (PAEs), polycyclic aromatic hydrocarbons (PAHs), and petroleum hydrocarbons were effectively eliminated in reactors. The main microorganisms, key functional genes, and putative pathways for alkanes, PAHs, and PAEs degradation were also identified.

研究领域: 环境微生物学 · 生物修复 · 废水处理 · 水力压裂
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY · 2021 · IF 2.262

Synthesis of polytriethanolamine based surfactant and its flotation performance evaluation of oilfield produced water treatment

Shenwen Fang,Weixin Hu,Qingqing Tang,Manlin Wang,Xiujun Wang,Ming Duan

As the amount of oilfield produced water (PW) keeps going up, highly efficient flotation agent is needed. In this paper, a series of surfactants (abbreviated as Q-PTEA-Cn) derived from polytriethanolamine were synthesized. Their surface activities and flotation performance were evaluated. The result showed that the Q-PTEA-Cns can effectively reduce the surface tension of water and interface tension of crude oil/water. The Q-PTEA-C12-1 had the best flotation performance and the rational flotation condition was recommended as follows: Q-PTEA-C12-1 dosage 100 mg/L, gas flow 3 L/min, and flotation time 20 minutes. At this condition, the oil removal efficiency of two commonly used flotation agents (FL-1 and FL-2) and Q-PTEA-C12-1 were 62.3%, 69.1%, and 83.6%, respectively. The flotation kinetic of Q-PTEA-C12-1 can be described by Maruyama’s flotation model, which presented that there was adsorption of oil droplet adsorbed surfactant onto bubble. Floatation mechanism study confirmed that the Q-PTEA-C12-1 can absorb onto the oil droplet and showed that the Q-PTEA-C12-1 can enhance the bubble–drop attachment efficiency and the stability of bubble–drop agglomerates.

研究领域: 环境工程 · 化学工程 · 水处理 · 表面活性剂化学
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Environmental Technology & Innovation · 2023 · IF 7.1

Improved degradation of petroleum contaminants in hydraulic fracturing flowback and produced water using laccase immobilized on functionalized biochar

Hanghai Zhou,Xiaomin Huang,Lijia Jiang,Qi Shen,Hong Sun,Ming Yi,Xin Wang,Xiaohong Yao,Yifei Wu,Chunfang Zhang,Jiangwu Tang

Large quantities of hydraulic fracturing flowback and produced water (HF-FPW) represent an important environmental issue owing to their inclusion of toxic petroleum contaminants. Enzymatic degradation is a promising approach for treating these pollutants. However, the low stability and poor reusability of free enzymes greatly inhibit their applications. This study investigated the effect of biochar-immobilized laccases on the biodegradation of petroleum contaminants in HF-FPW. Acid functionalization of corn straw biochar increased its surface area and pore volume, allowing it to adsorb additional laccase on the surface. Biochar-immobilized laccase exhibited a high tolerance to a low pH and high temperatures and retained >81.0% of its relative activity at 4 °C for 20 d. In addition, the immobilized laccase displayed reusability after six reaction cycles, retaining 40.9% of its activity. Supplementation with immobilized laccase substantially improved microbial growth and fluorescein diacetate hydrolase activity in HF-FPW, which were up to 25.5 times and 4.9 times higher than those of the free laccase treatment, respectively. The immobilized laccase also elevated the transcription levels of degradation genes such as rub and xylE , and greatly enhanced the biodegradation of n -alkanes (reduction from 112.4 mg/L to 41.9 mg/L) and polycyclic aromatic hydrocarbons (reduction from 2606 . 2 μ g /L to 1526 . 6 μ g /L). Full-length 16S rRNA gene sequencing revealed that Pseudomonas stutzeri , Pseudomonas balearica , and Stenotrophomonas maltophilia dominated the microbial community and were potential functional populations. This study represents the first attempt of utilizing biochar-immobilized laccase to treat HF-FPW and has important implications for efforts to develop strategies for HF-FPW remediation.

研究领域: 环境科学 · 生物技术 · 微生物学 · 废物管理
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