Journal Information
China Petroleum Processing and Petrochemical Technology
Included in the Science Citation Index(SCI)
Sponsor: Research Institute of Petroleum Processing, SINOPEC
Publisher: Editorial Office of China Petroleum Processing and Petrochemical Technology
Editor: Editorial Office of China Petroleum Processing and Petrochemical Technology
Editor in Chief: Member of Chinese Academy of Engineering, Wang Xieqing
Deputy Editor in Chief: Liu Hongzhou
ISSN 1008-6234
CN 11-4012/TE
Current Issue
30 March 2023 Volume 25 Issue 1
2023, 25(1):  0. 
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Scientific Research
Morphology, nanostructure and oxidation reactivity of particulate matter emitted by diesel blending with various aromatics
Yang He, Li Bo, Liu Shuntao, Wang Yajun, Zhang Ran, Guo Lingyan
2023, 25(1):  1-9. 
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This study aims to analyze the influence of the polycyclic aromatic hydrocarbon (PAH) content in diesel on the physical and chemical properties of diesel soot particles. Four diesel fuels with different PAH content were tested on a 11.6 L direct- injection diesel engine. The raw particulate matter (PM) before the after-treatment devices was collected using the thermophoresis sampling system and the filter sampling system. A transmission electron microscope and Raman spectrometer are used to analyze the physical properties of the soot particles, including morphology, primary particle size distribution, and graphitization degree. A Fourier transform infrared spectrometer and thermogravimetric analyzer are
used to characterize the surface chemical composition and oxidation reactivity of soot particles, respectively. The results show that as the PAH content in the fuel decreases, the size of the primary soot particles decreases from 29.58 to 26.70 nm. The graphitization degree of soot particles first increases and then decreases, and the relative content of the aliphatic hydrocarbon functional groups of soot particles first decreases and then increases. The T10, T50, and T90 of soot from high-PAH fuel are 505.3, 589.3, and 623.5 °C, while those from low-PAH fuel are 480.1, 557.5, and 599.2 °C, respectively. This indicates that exhaust PM generated by the low-PAH fuel has poor oxidation reactivity. However, as the PAH content in fuel is further decreased, the excessively high cetane number may cause uneven mixing and incomplete combustion, leading to enhanced oxidation reactivity.
Demulsification Behavior, Characteristics, and Performance of Surfactant Stabilized Oil-in-Water Emulsion under Bidirectional Pulsed Electric Field
Ren Boping, Kang Yong, Zhang Xianming, Gong Haifeng, Chen Ling, Liu Yunqi
2023, 25(1):  10-22. 
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As a novel electric demulsification method, bidirectional pulsed electric field (BPEF) was employed to demulsify the surfactant stabilized oil-in-water (SSO/W) emulsion for oil/water separation in this work. The demulsification behavior, characteristics, and stages under BPEF were explored. It was discovered that BPEF drove SSO/W emulsion to move and form vortexes, during which the oil droplets aggregated and accumulated to generate an oil droplet layer (ODL). ODL subsequently transformed into a continuous oil layer (COL) leading to the demulsification and separation of SSO/W emulsion. The conversion rate of ODL to COL was defined and used to evaluate the demulsification process and reflect the coalescence ability and transformation efficiency of dispersed oil droplets into COL. Furthermore, the effects of BPEF voltage, frequency, duty cycle, ratio of pulse output time, and surfactant type and content on the demulsification performance were examined. The optimal values of BPEF parameters for demulsification operation were 400 V, 25 Hz, 50%, and 4:1. O/W emulsion containing anionic surfactant was apt to be demulsified by BPEF, nonionic surfactant took the second place and cationic surfactant was the most difficult. A high surfactant content was not conducive to the BPEF demulsification. This work is anticipated to provide useful guidance for oil/water separation and oil recovery from actual emulsified oily wastewater by BPEF.
Synthesis and Performance of an Associative Anti-shear Drag Reducer Based on Hydrogen Bond Association of Dodecyl Methacrylate#br#
Lu Yong, Li Chenhao, Li Hao, Chen Yue, Xu Dan, Wang Yiran, Meng Yeqiao, Zhang Xiaolai
2023, 25(1):  23-33. 
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Using K2S2O8-Na2SO3 as the redox initiation system, a hydrogen-bond-association-based dodecyl methacrylate system associative anti-shear drag reducer was synthesised by standard emulsion polymerisation. The reaction process was simple and gentle as well as safe and stable. Molecular design was carried out using molecular dynamics simulation methods. The results of infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, gel chromatography, and laser light scattering showed that the reaction polymerisation was relatively complete, the product was uniform, the molecular weight distribution was controllable, and the synthesised polymer had good flexibility. The donor lauryl methacrylate-styrene-methacrylic acid (LMA-St-MAA) and acceptor lauryl methacrylate-styrene-dimethylaminoethyl methacrylate (LMA-St-DMA) polymers had an associative intermolecular interaction force, which increased the molecular cluster size of the associative system complex. The complex had good shear resistance, and the test results of the tube pump shear test showed that the synthesised associative oil-soluble polymer drag reduction system exhibited better drag reduction rate performance than poly-α-olefins over repeated cycles. The research results provide a reference plan for minimising the number of station-to-station inputs, thereby ensuring the stability of oil pipelines and reducing transportation costs.
Determination of the Henry’s Law Constant of Hexane in High-Viscosity Polymer Systems
Qi Jibing, Li Yuliang, Liu Youzhi, Yang Tong, Liu Yandong, Yuan Zhiguo, Yi Jianjun
2023, 25(1):  34-43. 
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Henry's coefficient of volatiles in the polymer system is a crucial parameter reflecting the gas-liquid equilibrium, which is very important for the devolatilization process. In this research, POE-cyclohexane and PDMS-hexane systems were taken as examples, using the gas-liquid equilibrium method, Henry's coefficient was obtained by measuring the gas phase equilibrium partial pressure when polymer solution containing different mass fractions of volatiles reached a saturated state. The effects of temperature, kinds of volatiles and polymer viscosity on the gas phase equilibrium partial pressure and Henry's coefficient of volatiles were investigated. Experimental results indicate that, with the increase of temperature and polymer viscosity, the gas phase equilibrium partial pressure and Henry's coefficient of volatile cyclohexane increase. As temperature increases, the solubility of gas in liquid decreases. In POE-cyclohexane system, the relationship between Henry's coefficient of cyclohexane and temperature can be expressed by lnH=389.39-244402.54×(1/T)+3.86×10^7×(1/T)^(2 ). While in the PDMS-cyclohexane, it can be expressed by lnH=106.57-60139.08×(1/T)+8.69×10^6×(1/T)^2 . In PDMS-hexane system, the gas phase equilibrium partial pressure and Henry's coefficient of n-hexane with straight chain structure are higher than those of cyclohexane with cyclic structure. Henry's coefficient obtained in this study can provide a reference for perfecting the devolatilization process and improving the devolatilization effect.
2D Co2(OH)2BDC-HNTs nanocomposite-reinforced epoxy coating with outstanding corrosion resistance
Zhao Huarong, Zhang Yueshuang, Cheng Zhilin
2023, 25(1):  44-53. 
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Introducing inorganic nanomaterials into a polymer matrix greatly improves the anticorrosion performance of epoxy coatings(EP); however, poor compatibility between the materials can limit the improvement in properties. In this work, based on the high interface compatibility of two-dimensional (2D) Co2(OH)2BDC (BDC = 1,4-benzenedicarboxylate) in the epoxy coating that we reported in previous work, we fabricated a 2D Co2(OH)2BDC-halloysite nanotube (HNT) nanocomposite have a structure consisting of alternating of nanosheets and nanotube by in situ synthesis. The nanocomposite was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, and scanning electron microscopy. The mechanical and anticorrosion performance of the 2D Co2(OH)2BDC-HNT/EP coating was evaluated by mechanical tests and electrochemical impedance spectroscopy spectra. Compared with a conventional unreinforced epoxy coating, the 2D Co2(OH)2BDC-HNT/EP coating had higher mechanical strength and toughness, and the low-frequency impedance modulus of 2D Co2(OH)2BDC-HNT/EP coating was increased by three orders of magnitude, demonstrating the high corrosion resistance of our reinforced coating.
Preparation of Ionic Liquids Immobilized on FMIL-101 Catalysts for Conversion of CO2 to Propylene Carbonate
Sun Wenjie, Ran Weiting, Guo Liying, Song Xiaohui, Lü Donghao
2023, 25(1):  54-65. 
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The FMOFs-[HeMIM]Cl/(ZnBr2)2, FMOFs-[CeMIM]Cl/(ZnBr2)2, and FMOFs-[AeMIM]Cl/(ZnBr2)2 were, respectively, immobilized in functional metal -organic framework materials (FMOFs). They were used to catalyze the cycloaddition reaction of carbon dioxide (CO2) and epoxides. The results from the investigation showed that the three metal-based ionic liquid catalysts were the target products. Under the conditions of reaction temperature 110 oC, reaction pressure 2.0 MPa, and catalyst dosage accounting for 2.0% of the mass of epoxide, the conversion of epoxide was 96.63% and the selectivity of propylene carbonate was 98.64%, thus forming the optimal catalyst FMOFs-[CeMIM]Cl/(ZnBr2)2. Moreover, the catalyst has no obvious change in catalytic performance after being recycled four times.
Process Research
Heteroatomic Modification of Solid-Waste-Based Mesoporous Carbon for Volatile Organic Compound Adsorption
Liu Jun, Li Zhi, Xu Ke, Zhang Xinyang, Li Yunpeng, Wang Ya, Zhang Yongfa, Yang Song, Liu Shoujun, Li Junhua
2023, 25(1):  66-78. 
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Solid waste-based activated carbon (AC) was utilized as a carbon source to synthesize a series of carbon-based functional material RAC-X (X= P and S). The toluene adsorption capacities of RACs samples can be significantly improved adopting the heteroatomic modification strategy. TheRACs modified by phosphoric acid and sulfuric acid have the same specific surface area (1156 m2/g) and the similar porous structure. However, their exists the different toluene adsorption capacities, RAC-P of 316.22 mg/g and RAC-S of 460.12 mg/g, respectively, which are 1.6 and 2.4 times greater than that of RAC. Through X-ray photoelectron spectroscopy measurements, it is found that the increase in the amount of π–π* chemical bond over the AC surface results in an improvement in the toluene adsorption performance. Density functional theory results show that the S-containing functional groups loaded near the defect sites of RAC-S promote the adsorption energy for the toluene. Moreover, reusability tests show that RAC-S still retains 86% of the adsorption activity after four consecutive adsorption–desorption experiments. This indicates that the heteroatomic modification method exhibits an excellent toluene adsorption performance and recycling practicability, which not only is beneficial for achieving the rational utilization of solid waste resources but also provides a practical method for the efficient elimination of VOCs.
Effect of Different Loadings on the Performance of Ni2P/Al2O3 Catalysts for Low-Temperature Thioethering and Selective Hydrogenation of Diolefins in Liquefied Petroleum Gas
Xiao Han, Sun Jinru, Song Guoliang, Xie Xianna, Ke Ming, Tong Yanbing, Zhao Zhiping, Wang Zijian, Li Jiahan
2023, 25(1):  79-90. 
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In this study, different loadings of x%Ni2P/γ-Al2O3 (x = 6%, 9%, 12%, 15%, 18%) catalysts with aluminum oxide (Al2O3) as the carrier, nickel chloride (NiCl2) as the nickel (Ni) source, and ammonium hypophosphite (NH4H2PO2) as the phosphorus (P) source were prepared by the equal volume impregnation method to investigate the effects of different loadings on the performance of the selective hydrogenation of diolefins and thiol etherification in LPG. The physicochemical properties of the catalysts were characterized by XRD, BET, SEM, TEM, H2-TPR, and XPS, and the catalytic activity of the catalysts was evaluated in a fixed-bed microreactor. The results showed that a change in the loading affected the catalyst crystalline phase structure and size, specific surface area, P coverage, active phase dispersion, and catalytic activity. At 6%, 9%, and 12% loadings the catalysts had an Ni phase but there was no obvious Ni2P phase in the nickel phosphide; at 15% loading a single Ni2P phase was obtained, and at 18% loading both Ni2P and Ni12P5 phases appeared. There was a P enrichment on the catalyst surface, and the higher the loading the more P species were enriched on the surface, but some of the P was lost during the catalyst reduction process due to the production of phosphine (PH3) gas. The 15%Ni2P/γ-Al2O3 catalyst had the largest Ni/Al ratio and the best dispersion. The Ni2P active phase size was small at about 4.25 nm and Ni2P was uniformly dispersed on the catalyst surface without agglomeration. The 15%Ni2P/γ-Al2O3 catalyst had the best catalytic activity at a pressure of 2.0 MPa, a liquid hourly space velocity (LHSV) of 3.0 h-1, and a hydrogen to hydrocarbon ratio of 12. The 1,3-butadiene conversion was 97.45% and the methanethiol removal was 100% at a temperature of 140°C.
Efficient Absorptive Oxidation of H2S Using a Fe(III)-Cu(II) Coupled DES (ChCl/EG) Desulfurizer
Jin Zhaobo, Wang Xuening, Wang Yingjie, Liu Zhihao, Chen Hongyuan, Liu Jiawei, Qiu Kui
2023, 25(1):  91-104. 
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Abstract: In this experiment, an EG/ChCl deep eutectic solvent (DES) was synthesized using choline chloride (ChCl) and ethylene glycol (EG) as the raw materials. The synthesized DES was characterized by Fourier transform infrared spectroscopy and thermogravimetric analysis. The results demonstrate the successful synthesis of DES. A certain amount of FeCl 3 and CuSO 4 was added to the DES to promote the absorption of H 2 S; thus, a Fe(III)-Cu(II) coupled DES desulfurization system was obtained. The effects of DES raw materials’ ratio, FeCl 3 concentration, water content, CuSO 4 concentration, and reaction temperature on the desulfurization efficiency and the regeneration conditions were studied. The results show that ChCl/EG DES with a molar ratio of 1:2 has a better desulfurization effect, and the addition of an appropriate amount of water can effectively promote the dissolution of CuSO 4 and the absorption of H 2 S. An appropriate increase in reaction temperature and CuSO 4 concentration would also promote the absorption of H 2 S. When the concentration of CuSO 4 in DES desulfurizer was 0.15 mol/L, the gas speed was 20 mL/min, and the sulfur capacity could reach 10.23 g/L. The desulfurizer could be regenerated by passing O 2 , and the desulfurization efficiency did not change much after repeated use of desulfurization-regeneration many times. The desulfurization product was characterized by XRD as rhombohedral sulfur.
Investigation of the aplication of NiMo-YSx catalyst with different SiO2 content in LCO hydrocracking to BTXE
Zhong Fu, Zuo Tongjiu, Xie Yonggang, Lu Jiangyin
2023, 25(1):  105-114. 
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A series of functionalized USY/SiO2 zeolite composite supports were synthesized using the coating coprecipitation method, with tetraethyl orthosilicate (TEOS) as the silicon source and different ratios of USY to TEOS. Active metals nickel (Ni) and molybdenum (Mo) were loaded onto the supports using the impregnation method. Finally, a series of hydrogenation catalysts were synthesized. The characterization results showed that, compared with the USY catalyst, the addition of a certain quantity of SiO2 resulted in the disappearance of the strong acid sites on the catalyst, the number of weak acid and medium strong acid sites decreased, and a certain number of secondary mesoporous structures were formed. The addition of SiO2 reduced the secondary cracking of benzene, toluene, xylene, and ethylbenzene (BTXE) effectively, while excessive amounts of SiO2 reduced the hydrogenation activity of the catalyst, leading to a decline in the final yield of BTXE. At a maximum SiO2 content of 45%, the hydrogenation depth of light cycle oil (LCO) reached an optimum value. The hydrogenation performance of LCO was investigated in a fixed bed reactor at 380 °C, 4 MPa, and H2/ oil volume ratio of 800:1, where the gasoline and diesel fractions reached 80.00% and 16.74%, respectively. NiMo-YS45 had the highest BTXE selectivity, and the final yield of BTXE reached 21.27%.
A Simple Method for Preparing CuCl/Activated Carbon for Selective CO Adsorption from Hydrogen
Liu Di, Wang Qianqian, Huang Jiaxing, Zheng Jinyu, Jin Ye, Su Shikun
2023, 25(1):  115-122. 
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Carbon monoxide (CO) is an impurity gas that can poison the precious metal catalysts of hydrogen fuel cells, so it is necessary to separate CO from hydrogen. In this paper, an isovolumetric impregnation method was developed to prepare Cu(I)-supported activated carbon (AC), which is simple and easy to industrialize. The prepared cuprous chloride CuCl/AC adsorbent displayed a high CO adsorption capacity of 82.1 cm3/g and a high CO/H2 separation factor of 20 at 20 bar and 298 K. This material can adsorb and remove CO from CO/H2 mixed gas (5 μL/L CO-balanced H2) to less than 0.2 μL/L under dynamic flow conditions, and showed excellent regeneration performance. The results show that CuCl/AC is an effective adsorbent for separating trace CO in high-purity hydrogen.
Coupling agent grafting assisted synthesis of C3N4-ZrO2 heterojunction composites with enhanced photocatalytic performance
Liu Yanxiu, Luo Jing, Li Jinqi, Wang Xueqin, Song Hua
2023, 25(1):  123-132. 
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Heterojunction composites were prepared by silane coupling agent grafting from synthesized graphitic carbon nitride (g-C3N4) and commercially available zirconia (ZrO2). The samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) spectroscopy, UV-vis diffuse reflectance spectroscopy (DRS), photoluminescence (PL) spectroscopy, and electrochemical impedance spectroscopy (EIS). The photocatalytic activity of the composites was evaluated by the degradation of methylene blue (MB) under visible light irradiation. The results showed that heterojunction composites of g-C3N4 and ZrO2 could be successfully prepared by coupling agent grafting. The optimal mass ratio of g-C3N4 and ZrO2 was 2:1, with an activity that was 3.8 times higher than g-C3N4 and 15.3 times higher than ZrO2. This was ascribed to the stronger light absorption, faster interfacial charge transfer, and lower photogenerated carrier recombination of the heterojunction composites.
Highly active sulfided NiPMo hydrodesulfurization catalyst prepared from Keggin-type phosphomolybdic acid
Zhu Tianhan, Li Wenxu, Wang Haiyong, Wang Chenguang, Yang Bin
2023, 25(1):  133-143. 
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A highly active sulfided NiPMo/MCM-41 (NiPMo-S/M41) hydrodesulfurization (HDS) catalyst was successfully synthesized using Keggin-type phosphomolybdic acid as the phosphorus and molybdenum source, and thioacetamide as the sulfur source. The supported NiPMo/M41, Ni2P-Mo/M41 and Ni2P/M41 catalysts were also prepared to investigate the effects of Mo, S, and Keggin structure on the HDS performance of the catalysts. The HDS activities of NiPMo/M41 and NiPMo/M41-S for dibenzothiophene (DBT) were much higher than that of Ni2P-Mo/M41, demonstrating that the active phases in the Keggin-structured catalysts were significantly superior than that of the Mo-modified Ni2P phase. The HDS activity of the catalysts followed the order NiPMo/M41-S (96.7%) > NiPMo/M41 (89.9%) > Ni2P-Mo/M41 (53.5%) > Ni2P/M41 (48.9%). For all the Ni2P/M41, Ni2P-Mo/M41 and NiPMo/M41 catalysts, phenyl cyclohexane (CHB) was formed in small concentrations (<21.0%), indicating that direct desulfurization (DDS) was the favored reaction route and that it did not change for Keggin-structured NiPMo/M41. What’s more, the selectivity towards CHB of NiPMo/M41-S increased to 44.6%, much higher than that of NiPMo/M41 catalyst (17.6%), showing the sulfurization deduced the improved hydrogenation ability, which was attributed to the metal-acid synergistic effect.
The Preparation of B2O3/SBA-15 and Its Application in Nickel-Tolerated FCC Catalyst as Matrix Component
Yuan Chengyuan, Ju Guannan, Chen Qiang, Yan Tao, Li Zhongfu
2023, 25(1):  144-150. 
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Fluid catalytic cracking (FCC) is still a key process in the modern refining area, in which nickel-contamination for FCC catalyst could obviously increase the dry gas and coke yields and thus seriously affect the stability of FCC unit. Therefore, in this paper, B2O3-modified SBA-15 molecular sieves (B2O3/SBA-15) with different B2O3 contents were prepared, characterized and further used in preparation of Ni-tolerated FCC catalyst as matrix component. Characterization results suggested that, B2O3/SBA-15 samples possessed excellent Ni-passivation ability and structure properties of SBA-15 parent such as high-ordered mesopores, big surface area and high pore volume, which made B2O3/SBA-15 sample could greatly improve the Ni-tolerance performance of FCC catalyst by promoting the Structure properties and Ni-passivation ability of the prepared FCC catalyst. The evaluation results of heavy oil catalytic cracking indicated that, at the same Ni-contamination condition, the dry gas, coke and heavy oil yields for the FCC catalyst containing B2O3/SBA-15 could obviously decrease by 0.92, 1.65 and 1.26 percentage points respectively with total liquids yield increasing by 3.83 percentage points in compared with conventional FCC catalyst.
Preparation of Cu/N-TiO2 nano photocatalyst using high gravity technology for photodegradation of phenol wastewater
Ren Xueqing, Zhang Qiaoling, Zhang Yanfen, Qi Guisheng, Guo Jing, Gao Jing
2023, 25(1):  151-161. 
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TiO2 is a promising photocatalyst, but the limited contact area of liquid-liquid interface and low catalytic efficiency caused by catalysts with large particle size and uneven distribution restrict the practical application. As an effective process intensification equipment, the impinging stream-rotating packed bed (IS-RPB) overcomes the mixing limitation of traditional stirred tank reactor, and provides a micro-mixing environment at the molecular scale for liquid-liquid two phase, which could reduce the particle size and distribution range. Cu/N-TiO2 nanoparticles were successfully prepared by one-step precipitation method using urea as the nitrogen source, titanyl sulfate as the titanium source, copper chloride as the copper source and ammonium hydroxide as the precipitant in an IS-RPB. The particle size of obtained photocatalyst was about 11.40 nm with narrow size-distribution via SEM and TEM. According to XPS, N replaced part of O, and was uniformly dispersed in the TiO2 lattice in the form of interstitial N and substitutional N. Cu replaced part of Ti and existed in the form of Cu2+. The synergistic effect of these two elements forms a new impurity energy level and reduces band gap energy of TiO2 nanoparticles. The specific surface areas of Cu/N-TiO2 are 152.97 m2/g. The influence of the main factors on the degradation rate was studied, the results showed that the removal efficiency could reach 100% under the optimal operating conditions after 2 hours UV light irradiation. The EPR measurement showed that the superoxide radical (O2-·) played a leading role in the degradation process, while the effect of photogenerated holes (h+) and hydroxyl radicals (OH·) were relatively weak.
Attenuation of Chlorinated Contamination in Three Different Depths of Aquifers at Remediation Site
Sun Shaodong, Li Weisi, Huang Yongjun, Jiang Qing, Bai Yu, Wang Kunhua, Xue Jianliang, Wang Bo, Yan Dongdong, Xu Conghai
2023, 25(1):  162-178. 
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The cleanup of carbon tetrachloride (CCl4) in groundwater is challenging due to its high volatility and tendency to form a dense nonaqueous liquid phase. From the engineering applications perspective, the pump-and-treat (PAT) technology has substantial advantages owing to its large-scale implementation ability to solve groundwater contamination. However, few studies focused on the variation in chloride contaminants in remediation sites after the contaminated groundwater was pumped and treated. Herein, we monitored the changes in chlorinated contamination in groundwater from 12 aquifers at the field level for 6 months. Considering that the natural attenuation of chlorinated contamination is inseparable from the action of microorganisms, the major environmental factors influencing biodegradation were also evaluated. A redundancy analysis (RDA) showed that inorganic salts (DS, DN, and DF) were the most important factor (>60%) affecting the concentration of chloride contaminants, including the negative correlation between DN and the degradation of contaminants in shallow aquifers. In deep aquifers, DS, DF, and pH explained most of the degradation of chloride contaminants. For bedrock layers, DCl was positively relevant to the chloride contaminants in wells PTJ2 and PTJ10. In addition, EC and DS accounted for 73.2% and 92.4% of the contaminant’s variance in wells PTJ4 and PTJ8, respectively. Moreover, the concentrations of the corresponding contaminations and physicochemical variation in three different depths of aquifers were compared; the shallower aquifers showed a higher biodegradation. The in situ monitoring and analysis of contaminated groundwater in remediation sites under PAT will promote practical wastewater treatment technologies in engineering applications.