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SCI和EI收录∣中国化工学会会刊
本期目录
2011年 第19卷 第5期 刊出日期:2011-10-28
    Computer Simulation of Adsorption and Separation of CO2/CH4 in Modified COF-102
    朱玉俊, 周建海, 胡军, 刘洪来, 胡英
    Chinese Journal of Chemical Engineering. 2011, 19(5):  709-716. 
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    Covalent organic framework (COF) is a porous material with low density and large BET (Brun-auer-Emmett-Teller) surface area. They have great potential in gas adsorption and separation. In this work, the ad-sorption of pure CO2 and CO2/CH4 mixture on modified COF-102 was simulated by using GCMC (grand canonical Monte Carlo). Metal Li was incorporated into COF-102 through three doping methods, including charge exchange, O--Li+ dipolar interaction and O--Li+ chemical bonding. The influence of Li doping on the adsorption of CO2 was studied. The results showed that among the three methods, the dipole doping is the best way to improve CO2 ad-sorption performance. Further, the ligands of COF-102 were replaced by extended aromatic moieties, such as di-phenyl and pyrene. The adsorption capacity of CO2 and CH4, and the selectivity of CO2/CH4 on the ligand-replaced COF-102 were studied. The capacity of CO2 and CH4 on the ligand-replaced COF-102 had obvious changes; hence the selectivity of CO2/CH4 can be adjusted accordingly.
    A New Model for the Simulation of Distillation Column
    李文彬, 刘伯潭, (K. T. YU)余国琮, 袁希钢
    . 2011, 19(5):  717-725. 
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    A new computational mass transfer model is proposed for simulating the distillation process by solving the fluctuating mass flux for ?i'c' the closure of turbulent mass transfer equation in order to obtain the concentration profile and the separation efficiency of distillation column. The feather of the proposed model is to abandon the conventional way of introducing the turbulent mass transfer diffusivity (dispersion coefficient) to the turbulent mass transfer equation. To verify the validity of the proposed model, a commercial scale packed column and a sieve tray column were simulated and compared with published experimental data. The simulated results were satisfactorily confirmed in both concentration distribution and separation efficiency.
    Comparison of Gas Distribution Properties of Conventional and High Capacity Structured Packings
    Žarko Olujić
    . 2011, 19(5):  726-732. 
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    This paper presents the results of an experimental study carried out using large scale equipment to ob-serve the effect of geometry on gas distribution properties of a high capacity corrugated sheet structured packing (Montz-pak B1-250M) and to compare it with that of its conventional counterpart (Montz-pak B1-250). Although the high capacity packing exhibits a significantly lower overall pressure drop, the gas distribution performance is similar to that of the conventional packing, and in both cases consistently good one.
    A Research Note on the Adsorption of CO2 and N2
    张中正, 阮红证, 周亚平, 苏伟, 孙艳, 周理
    . 2011, 19(5):  733-737. 
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    Experiments were made for the adsorption of CO2 and N2 on typical adsorbents to investigate the effects of porous structure and surface affinity of adsorbents as well as those of adsorption temperature and pressure that might cause the variation of adsorption mechanism. It is shown that polar surface tends to enlarge the adsorption difference between CO2 and N2, and the difference is more sensitive to temperature than the adsorbents with non-polar surface. The adsorbents with non-polar surface are not much sensitive to the effect of water vapor, though the water vapor interferes the separation remarkably. The separation coefficient linearly increases with the micro-pore volume per unit surface area of activated carbons, but no rule is shown on mesoporous silicon materials. The function of adsorption mechanism on the separation is not as much as expected.
    Connection Between Liquid Distribution and Gas-Liquid Mass Transfer in Monolithic Bed
    许闽, 刘辉, 李成岳, 周媛, 季生福
    . 2011, 19(5):  738-746. 
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    With a particular focus on the connection between liquid flow distribution and gas-liquid mass transfer in monolithic beds in the Taylor flow regime, hydrodynamic and gas-liquid mass transfer experiments were carried out in a column with a monolithic bed of cell density of 50 cpsi with two different distributors (nozzle and packed bed distributors). Liquid saturation in individual channels was measured by using self-made micro-conductivity probes. A mal-distribution factor was used to evaluate uniform degree of phase distribution in monoliths. Overall bed pressure drop and mass transfer coefficients were measured. For liquid flow distribution and gas-liquid mass transfer, it is found that the superficial liquid velocity is a crucial factor and the packed bed distributor is better than the nozzle distributor. A semi-theoretical analysis using single channel models shows that the packed bed distributor always yields shorter and uniformly distributed liquid slugs compared to the nozzle distributor, which in turn en-sures a better mass transfer performance. A bed scale mass transfer model is proposed by employing the single channel models in individual channels and incorporating effects of non-uniform liquid distribution along the bed cross-section. The model predicts the overall gas-liquid mass transfer coefficient with a relative error within ±30%.
    Technical Challenges and Progress in Fluidized Bed Chemical Vapor Deposition of Polysilicon
    李建隆, 陈光辉, 张攀, 王伟文, 段继海
    . 2011, 19(5):  747-753. 
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    Various methods for production of polysilicon have been proposed for lowering the production cost and energy consumption, and enhancing productivity, which are critical for industrial applications. The fluidized bed chemical vapor deposition (FBCVD) method is a most promising alternative to conventional ones, but the homo-geneous reaction of silane in FBCVD results in unwanted formation of fines, which will affect the product quality and output. There are some other problems, such as heating degeneration due to undesired polysilicon deposition on the walls of the reactor and the heater. This article mainly reviews the technological development on FBCVD of polycrystalline silicon and the research status for solving the above problems. It also identifies a number of chal-lenges to tackle and principles should be followed in the design of a FBCVD reactor.
    Simulation for Transesterification of Methyl Acetate and n-Butanol in a Reactive and Extractive Distillation Column Using Ionic Liquids as Entrainer and Catalyst
    蔡贾林, 崔现宝, 杨志才
    . 2011, 19(5):  754-762. 
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    A new reactive and extractive distillation process with ionic liquids as entrainer and catalyst (RED-IL) was proposed to produce methanol and n-butyl acetate by transesterification reaction of methyl acetate with n-butanol. The RED-IL process was simulated via a rigorous model, and high purity products of methanol and n-butyl acetate can be obtained in such a process. The effects of reflux ratio, feed mode, holdup, feed location, en-trainer ratio and catalyst concentration on RED-IL process were investigated. The conversion of methyl acetate and purities of products increase with the holdup in column, entrainer ratio and catalyst content. An optimal reflux ratio exists in RED-IL process. Comparing to the mixed-feed mode, the segregated-feed mode is more effective, in which the optimal feed locations of reactants exist.
    Coupled Transport Phenomena in Corrugated Photocatalytic Reactors
    Adam A. Donaldson, ZHANG Zisheng
    . 2011, 19(5):  763-772. 
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    Corrugated reactors are known for their use in applications requiring UV-exposure, whereby media flowing within the corrugated channel react with a photo-active catalyst impregnated on the surface (i.e. TiO2). The performance in these systems is dependent on catalyst properties and reactivity for a given light source, in conjunc-tion with the coupled transport of reactants within the media and photons falling incident to the catalyst surface. Experimental and computational analyses of local mass transfer and radiation patterns for a broad range of corruga-tion angles, depths, and non-idealities introduced during manufacture (i.e. fold curvature) are thus integrated to the design and optimization of these systems. This work explores techniques for determining incident energy distribu-tions on the surface of corrugated reactor geometries with non-ideal cross-sectional profiles, and the local and over-all mass transfer rates obtained using computational fluid dynamics and experimental analysis. By examining the reaction kinetics for the photo-degradation of 4-chlorophenol over a TiO2 catalyst, the effects of surface area, en-ergy incidence with photon recapture, and local mass transfer on overall reactor performance are presented to high-light optimization concerns for these types of reactors.
    Enzymatic Hydrolysis of Cellulose with Different Crystallinities Studied by Means of SEC-MALLS
    张名佳, 苏荣欣, 齐崴, 杜若愚, 何志敏
    . 2011, 19(5):  773-778. 
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    The reactions of exo-cellulase (cellobiohydrolase, CBH) and endo-cellulase (endoglucanase, EG) were investigated by analyzing the insoluble residues of microcrystalline cellulose (MCC) and filter paper cellulose (FPC) during enzymatic hydrolysis. Molecular parameters including molecular weight and its distribution, degree of po-lymerization, and radii of gyration were measured by size exclusion chromatography coupled with multi-angle laser light scattering. No significant change in MCC chains was found during the whole reaction period, indicating that CBH digestion follows a layer-by-layer solubilization manner. This reaction mode might be the major reason for slow enzymatic hydrolysis of cellulose. On the other hand, the degree of polymerization of FPC chains decreases rapidly in the initial reaction, indicating that EG digestion follows a random scission manner, which may create new ends for CBH easily. The slopes of the conformation plots for MCC and FPC increase gradually, indicating stronger chain stiffness of cellulose during hydrolysis.
    Pressure Drop Measurements on Distillation Columns
    T. J. Cai, M. R. Resetarits
    . 2011, 19(5):  779-783. 
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    Pressure drops are of major importance for distillation/absorption columns. This paper mainly discusses how to correctly measure, interpret and use pressure drop data. The possible causes of incorrect pressure drop measurements are studied including the effects of pressure tap dimensions, locations, and vapor condensation etc. The effect of the static head of vapor on the pressure drop data and column pressures is evaluated. Variations of sec-tional pressure drops along the column are investigated based on the experimental data obtained from commercial size distillation columns at Fractionation Research, Inc. (FRI). For a packed column, it is found that the spacing between the liquid distributor and the top of the bed affects the overall pressure drop measurements, which is con-firmed by a fundamental fluid dynamics analysis.
    Recovery of Hydrogen from Ammonia Plant Tail Gas by Absorption-Hydration Hybrid Method
    刘蓓, 王秀林, 唐绪龙, 杨兰英, 孙长宇, 陈光进
    . 2011, 19(5):  784-791. 
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    In this work, the absorption-hydration hybrid method was used to recover (hydrogen+nitrogen) from (hydrogen+nitrogen+methane+argon) tail gas mixtures of synthetic ammonia plant through hydrate formation/dissociation. A high-pressure reactor with magnetic stirrer was used to study the separation efficiency. The in-fluences of the concentration of antiagglomerant, temperature, pressure, initial gas-liquid volume ratio, and oil-water volume ratio on the separation efficiency were systematically investigated in the presence of tetrahydro-furan (THF). Antiagglomerant was used to disperse hydrate particles into the condensate phase for water-in-oil emulsion system. Since nitrogen is the material for ammonia production, the objective production in our separation process is (hydrogen+nitrogen). Our experimental results show that by adopting appropriate operating conditions, high concentration of (hydrogen+nitrogen) can be obtained using the proposed technology based on forming hydrate.
    A Study on Enhancement of Filtration Process with Filter Aids Diatomaceous Earth and Wood Pulp Cellulose
    都丽红, 陈旭, 李文苹, 朱企新
    . 2011, 19(5):  792-798. 
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    In this paper, a study to enhance the filtration for solid/liquid materials difficult to be filtered, such as highly viscous, highly compactible or gel like materials, is presented. Filter aids diatomaceous earth and wood pulp cellulose are used to enhance the filtration by improving filter cake structure and properties in the filtration of a biological health product and a highly viscous chemical fiber polymer melt product. The property of solid/liquid systems, filtration at different flow rates, specific cake resistance, cake wetness, filtration rate, filtrate turbidity for filter aid selection and evaluation, and operation optimization are investigated. The results are successfully applied to industrial process, and can be used as a reference for similar filtration applications.
    Numerical Simulation of Concentration Field on Liquid Side around Bubble during Rising and Coalescing Process in Non-Newtonian Fluid
    朱春英, 付涛涛, 高习群, 马友光
    . 2011, 19(5):  799-807. 
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    On the basis of Navier-Stockes equation and convection-diffusion equation, combined with surface ten-sion and penetration models, the equations of moment and mass transfer between bubble and the ambient non-Newtonian liquid were established. The formation of a single bubble from a submersed nozzle of 1.0 mm di-ameter and the mass transfer from an artificially fixed bubble into the ambient liquid were simulated by the volume-of-fluid (VOF) method. Good agreement between simulation results and experimental data confirmed the validity of the numerical method. Furthermore, the concentration distribution around rising bubbles in shear thinning non-Newtonian fluid was simulated. When the process of a single ellipsoidal bubble with the bubble deformation rate below 2.0 rises, the concentration distribution is a singletail in the bubble’s wake, but it is fractal when the bubble deformation rate is greater than 2.0. For the overtaking of two in-line rising bubbles, the concentration distribution area between two bubbles broadens gradually and then coalescence occurs. The bifurcation of concentration distribution appears in the rear of the resultant bubble.
    Kinetic-Thermodynamic Analysis of the Reactive Distillation Process of the Cyclohexene Hydration Using the Zeolite Catalyst
    叶建初, 黄佳丽, 林晗丹, 曹克腾, 沙勇
    . 2011, 19(5):  808-814. 
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    Reactive distillation could be utilized to produce cyclohexanol through the cyclohexene hydration. By means of highly active zeolite catalyst HZSM-5, the kinetic-thermodynamic analysis of this reactive distillation has been carried out to get the characteristics of the reactive distillation. Results from kinetic and thermodynamic analysis indicate that the optimal pressure of this reactive distillation process should be set to higher pressure such as 0.3 or 0.4 MPa. To avoid the recovery of cyclohexanol at the top of the column, an unreactive section should be allo-cated at the upper column. In addition, the inert component benzene is more unfavorable to the reactive distillation process in comparison with the inert cyclohexane.
    CFD Simulation and Experimental Validation of Fluid Flow in Pre-distributor
    张吕鸿, 高国华, 隋红, 李洪, 李鑫钢
    . 2011, 19(5):  815-820. 
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    Liquid distributor is a very import internal for distillation columns. Pre-distributor is usually set on the top of distributor for initial distribution. Fluid flow in pre-distributor is a complex system of variable mass flow with many orifices and sub-branches. Consequently, the two phase modeling of pre-distributors was carried out and the homogeneous model with free surface model was applied. The numerical method was validated by comparing with experimental data. Using the simulated results for different pre-distributors, the impacts of inflow rate, location and orientation upon the outflow distribution were investigated. Furthermore, influences of the outflow distribution for pre-distributor on liquid uniformity in trough were also analyzed. The conclusions can be adopted for the struc-tural design of liquid distributor and pre-distributor of large scale.
    An Effective Method to Improve the Performance of Fixed Carrier Membrane via Incorporation of CO2-selective Adsorptive Silica Nanoparticles
    于型伟, 王志, 赵娟, 袁芳, 李诗纯, 王纪孝, 王世昌
    . 2011, 19(5):  821-832. 
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    Fixed carrier membrane exhibits attractive CO2 permeance and selectivity due to its transport mecha-nism of reaction selectivity (facilitated transport). However, its performance needs improvement to meet cost targets for CO2 capture. This study attempts to develop membranes with multiple permselective mechanisms in order to enhance CO2 separation performance of fixed carrier membrane. In this study, a novel membrane with multiple permselective mechanisms of solubility selectivity and reaction selectivity was developed by incorporating CO2-selective adsorptive silica nanoparticles in situ into the tertiary amine containing polyamide membrane formed by interfacial polymerization (IP). Various techniques were employed to characterize the polyamide and polyamide-silica composite membranes. The TGA result shows that nanocomposite membranes exhibit superior thermal stability than pure polyamide membranes. In addition, gas permeation experiments show that both nanocomposite membranes have larger CO2 permeance than pure polyamide membranes. The enhanced CO2/N2 separation performance for nanocomposite membranes is mainly due to the thin film thickness, and multiple permselective mechanisms of solubility selectivity and reaction selectivity.
    Prediction of Distillation Column Performance by Computational Mass Transfer Method
    孙志民, 刘春江, 余国琮, 袁希钢
    . 2011, 19(5):  833-844. 
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    A computational mass transfer model is proposed for predicting the concentration profile and Murphree efficiency of sieve tray distillation column. The proposed model is based on using modified c'2c' two equations formulation for closing the differential turbulent mass transfer equation with improvement by considering the vapor injected from the sieve hole to be three dimensional. The predicted concentration distributions by using proposed model were checked by experimental work conducted on a sieve tray simulator of 1.2 meters in diameter for desorbing the dissolved oxygen in the feed water by blowing air. The model predictions were confirmed by the experimental measurement. The validation of the proposed model was further tested by comparing the simulated result with the performance of an industrial scale sieve tray distillation column reported by Kunesh et al. for the stripping of toluene from its water solution. The predicted outlet concentration of each tray and the Murphree tray efficiencies under different operating conditions were in agreement with the published data. The simulated turbulent mass transfer diffusivity on each tray was within the range of the experimental result in the same sieve column reported by Cai et al. In addition, the prediction of the influence of sieve tray structure on the tray efficiency by using the proposed model was demonstrated.
    Characterization of Rayleigh Convection in Interfacial Mass Transfer by Lattice Boltzmann Simulation and Experimental Verification
    付博, 袁希钢, 刘伯潭, 陈淑勇, 张会书, 曾爱武, 余国琮
    . 2011, 19(5):  845-854. 
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    Concentration gradient induced Rayleigh convection can influence effectively interfacial mass transfer processes, but the convection phenomena are known as mesoscopic and complex. In order to investigate this phenomenon, a two-equation Lattice Boltzmann Method (LBM) is proposed to simulate the velocity and the concentra-tion distributions of Rayleigh convection generated in the CO2 absorption into ethanol liquid. The simulated results on velocity distributions are experimentally verified by PIV (particle image velocimetry technique) measurements. In order to simplify the analysis, the convection in the simulation as well as in the experiment, the Rayleigh convection was manipulated into a single down flow pattern. The simulated results show that the concentration contours agree qualitatively with the schlieren images in the literature. The experimental and simulated results show that the Rayleigh convection under investigation is dominated by the flow in the downward direction and impels exchange of the liquid between the interfacial vicinity and the liquid bulk promoting the renewal of interfacial liquid, and hence enhances mass transfer. The comparison between the simulated and experimental results demonstrated that the proposed LBM is a promising alternative for simulating mass transfer induced Rayleigh convection.
    Integral PVA-PES Composite Membranes by Surface Segregation Method for Pervaporation Dehydration of Ethanol
    吴洪, 李宪实, 聂明成, 李犇, 姜忠义
    . 2011, 19(5):  855-862. 
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    A facile surface segregation method was utilized to fabricate poly(vinyl alcohol)-polyethersulfone (PVA-PES) composite membranes. PVA and PES were first dissolved in dimethyl sulfoxide (DMSO), then casted on a glass plate and immersed in a coagulation bath. During the phase inversion process in coagulation bath, PVA spontaneously segregated to the polymer solution/coagulation bath interface. The enriched PVA on the surface was further crosslinked by glutaraldehyde. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and energy dispersive spectrometer (EDS) confirmed the integral and asymmetric membrane structure with a dense PVA-enriched surface and a porous PES-enriched support, as well as the surface enrichment of PVA. The coverage fraction of the membrane surface by PVA reached up to 86.8% when the PVA content in the membrane recipe was 16.7% (by mass). The water contact angle decreased with the increase of PVA content. The effect of coagulation bath type on membrane structure was analyzed. The membrane pervaporation performance was evaluated by varying the PVA content, the annealing temperature, feed concentration and operation temperature. The membrane exhibited a fairly good ethanol dehydration capacity and long-term operational stability.
    Ultrafiltration Enhanced with Activated Carbon Adsorption for Efficient Dye Removal from Aqueous Solution
    董亚楠, 苏延磊, 陈文娟, 彭金明, 张岩, 姜忠义
    . 2011, 19(5):  863-869. 
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    In this study, orange G dye was efficiently removed from aqueous solution by ultrafiltration (UF) membrane separation enhanced with activated carbon adsorption. The powdered activated carbon (PAC) was deposited onto the UF membrane surface, forming an intact filter cake. The enhanced UF process simultaneously exploited the high water permeation flux of porous membrane and the high adsorption ability of PAC toward dye molecules. The influencing factors on the dye removal were investigated. The results indicated that with sufficient PAC incorporation, the formation of intact PAC filtration cake led to nearly complete rejection for dye solution under optimized dye concentration and operation pressure, without large sacrificing the permeation flux of the filtration process. Typically, the dye rejection ratio increased from 43.6% for single UF without adsorption to nearly 100% for the enhanced UF process, achieving long time continuous treatment with water permeation flux of 47 L·m2·h-1. The present study demonstrated that adsorption enhanced UF may be a feasible method for the dye wastewater treatment.
    Experimental Study on Local Mass Transfer of Structured Packing with the Method of Flow Visualization
    张燕来, 朱慧铭, 尹秋响
    . 2011, 19(5):  870-875. 
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    A chromochemical reactive mass transfer technique has been employed to study local mass transfer characteristics of structured packing. This technology adopted by experiment is an Ammonia Adsorption Method (AAM) that yields the surface distribution of transferred mass by analyzing the color distribution on a filter paper with the results of the color chemical reaction. A digital image processing technology is applied for data visualiza-tion. The three-dimensional plot of the local mass transfer coefficients shows that there exist three peak values on different positions of a unit cell of structured packing. In order to improve mass transfer efficiency of the structured packing, one piece of baffle is added between packing sheets. As a result, the average mass transfer coefficient in-creases by (10-20)% and the pressure drop decreases by (15-55)%.
    Isolation of Lysozyme from Chicken Egg White Using Polyacrylamide-based Cation-exchange Cryogel
    晏禄丁, 沈绍传, 贠军贤, 姚克俭
    . 2011, 19(5):  876-880. 
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    An effective cation-exchange chromatographic method for lysozyme isolation from chicken egg white is presented, using supermacroporous cryogel grafted with sulfo functional groups. The chromatographic processes were carried out by one-step and sequential elution, respectively. Sodium phosphate buffer (pH 7.8) containing different concentrations of NaCl is used as elution agent. The corresponding breakthrough characteristics and elution behaviors in the cryogel bed were investigated and analyzed. Purity of lysozyme in the elution effluent was assayed by sodium dodecyl sulfate-polyacrylamide gel electrophoresis (SDS-PAGE). The maximum purity of the obtained lysozyme was about 96%, and the cryogel is demonstrated as a potential separation medium for purification of high-purity lysozyme from chicken egg white.
    Synergism of Novel Sequence Bio-ecological Process and Biological Aerated Filter for Sewage Treatment in Cold Climate
    张鹏, 海热提, 周东凯, 何一群, 白志远
    . 2011, 19(5):  881-889. 
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    A lab-scale integrated treatment system including the novel sequence bio-ecological process (SBEP) and biological aerated filter (BAF) for a sewage mixture (chemistry laboratory wastewater and domestic sewage) was presented in this paper. The main objective of the study was to test the contribution of artificial aeration, recirculation ratio and mass concentration of steel slag on pollutant removal in winter when the plants are dormant. It had been shown that SBEP and BAF play different roles in removing contaminants from wastewater. During the airflow experiment, the removal efficiency of COD and TP in SBEP was higher than that in BAF, whereas BAF can compensate for the deficiency of SBEP where no significant improvement on ammonium nitrogen removal is observed. Yet, the removal efficiencies of COD, TP and NH4+-N in SBEP could be improved apparently when different recirculation ratio or various mass concentration of steel were applied. Especially, when the airflow of 0.06 L·h-1, the recirculation ratio rate of 80% and the mass concentration of steel of 2.2-2.4 g·L-1 were applied, the highest efficiency of 94.6%, 77.9% and 80.7% for COD, TP and NH4+-N were achieved, respectively. The inte-grated treatment system of SBEP and BAF was proved to be an effective wastewater treatment technique and a better alternative to treat domestic sewage.