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2019年 第21卷 第1期    刊出日期:2019-03-30
目录-Content
 Content
2019, 21(1):  0-00. 
摘要 ( 90 )  
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 The content of this issue
Review
X型分子筛在吸附中的应用研究进展
王玉冰 王辉国
2019, 21(1):  1-6. 
摘要 ( 230 )   PDF (432KB) ( 1172 )  
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综述了X型分子筛在对二甲苯吸附分离、N2/O2分离等领域中的应用,骨架硅铝比、阳离子种类、含水量等均会对其吸附选择性、吸附容量产生显著影响。作为对二甲苯吸附分离吸附剂的活性组分,X型分子筛的硅铝比为2.2~2.4、阳离子为Ba2+和K+、含水量为4.0%~5.0%时具有较高的对二甲苯吸附选择性。对于N2/O2分离,硅铝比为2.0、阳离子为Li+的X型分子筛表现出较高的N2吸附容量和N2/O2分离系数,通过引入第二种阳离子还可进一步提高其N2/O2分离系数,但是H2O的吸附会显著降低其N2吸附容量。此外,X型分子筛还可用于高纯He的吸附分离,以及CO2、CO、CH4、N2、Ar、H2的选择性吸附。
Catalyst Research
Phosphorous-modified carbon nanotube-supported Pt nanoparticles for the propane dehydrogenation reaction
刘杰 刘昌呈 达志坚 郑辉东
2019, 21(1):  7-14. 
摘要 ( 154 )   PDF (1345KB) ( 1015 )  
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The sintering of Pt nanoparticles is one of the main reasons for catalyst deactivation during the high-temperature propane dehydrogenation (PDH) reaction. Promoters and supports have been introduced to prolong the catalyst life. However, it is still necessary to develop novel catalysts with robust stability. Herein, phosphorus-modified carbon nanotube-supported Pt nanoparticles were employed for the PDH process. Phosphorus modification improves the Pt dispersion, effectively promoting the activity of Pt/P-CNTs. Additionally, phosphorus-modified CNTs interact strongly with Pt nanoparticles by improving the electron transfer or hybridization, stabilizing Pt nanoparticles from agglomeration, and significantly enhancing the catalyst stability.
以溶胶凝胶法制备纳米HY分子筛-氧化铝复合物为载体的新颖NiMo柴油加氢脱硫催化剂
尹海亮 刘新亮 周同娜 柳云骐
2019, 21(1):  15-22. 
摘要 ( 141 )   PDF (952KB) ( 1038 )  
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通过溶胶凝胶法制备了纳米HY分子筛-γ-Al2O3复合材料(AZ-x),并用作载体制备了系列NiMo催化剂(NiMo/AZ-x)。XRD, BET, TPD, TPR, HRTEM 和FT-IR分析手段用来表征载体和催化剂。与NiMo/γ-Al2O3相比,NiMo/AZ-x催化剂在FCC柴油加氢脱硫中表现出了更高的活性,并且,在复合载体中纳米HY分子筛含量小于20%的条件下,催化剂的加氢脱硫活性逐渐升高。与γ-Al2O3相比,纳米HY分子筛的引入能够改善复合材料的孔结构,有利于反应物分子在载体孔道中传输扩散。纳米HY分子筛的引入同时能够修饰载体表面特性,提高低温易还原金属比例,并且能够修饰MoS2形貌,导致形成具有较高边角位Mo原子分布的多层MoS2结构。
Influence of Cr3+concentration on SO2 removal of TiO2 based multi-walled carbon nanotubes
杨彦春 贾冯睿 建伟伟 张绍鹏 马丹竹 刘广鑫
2019, 21(1):  23-35. 
摘要 ( 141 )   PDF (1219KB) ( 929 )  
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In this study, titanium dioxide supported by multi-walled carbon nanotubes (MWCNTs/TiO2) and Cr-doped TiO2 supported by MWCNTs (MWCNTs/Cr-TiO2) were synthesized by sol–gel method. The prepared samples were characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, Brunauer–Emmett–Teller analysis, and Raman spectroscopy. The oxidation and removal efficiencies of SO2 in simulated flue gas were investigated experimentally in a fix-bed reactor. The 15% MWCNTs/Cr-TiO2 sample displayed excellent adsorption properties, and 30.415 mg/g of SO2 removal was achieved under optimal conditions (2300 ppm SO2, 8% O2, 5% H2O, 333.15 K, and 1275 h-1). The adsorption was enhanced because Cr doping modified the pore structure and inhibited the grain growth of TiO2. In addition, the Freundlich and Langmuir models revealed that SO2 was mainly adsorbed through chemical adsorption on the sample surfaces, and thermodynamic model analysis indicated that the adsorption was a spontaneous, exothermic, entropy-reducing process. The adsorption kinetics of SO2 can be described by pseudo-second-order kinetic and Bangham dynamics models. The possible reaction mechanism involved in desulfurization was also proposed.
Polycrystalline Phase WO3/g-C3N4 As A High Efficient Catalyst for Removal DBT in Model Oil
李秀萍 赵荣祥 毛春峰
2019, 21(1):  36-45. 
摘要 ( 130 )   PDF (1416KB) ( 1217 )  
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The polycrystalline phase WO3/g-C3N4 was synthesized through stirring method using tungstenic acid (H2WO4) and graphitic carbon nitride (g-C3N4) as raw materials. The catalyst was characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive spectroscopy (EDS),[It should be ”,”. Answer: this has modified.] Fourier transform infrared spectroscopy (FT-IR) and Brunauer-Emmett-Teller analysis (BET). The polycrystalline phase WO3/g-C3N4 was determined by XRD. Oxidation desulfurization process was investigated using WO3/g-C3N4 as catalyst, 30% hydrogen peroxide (H2O2) as oxidant and 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim]BF4) ionic liquids (ILs) as extractant. The operational conditions including H2WO4 amount, IL dose, H2O2 volume, temperature, catalyst dosage and types of sulfur compounds were systematically researched. The desulfurization rate could attached 98.46% for dibenzothiophene (DBT) in the model oil at the optimal reaction condition. In addition, the catalytic activity sightly reduce after five recycles of catalyst. Kinetics analysis shows that the oxidative desulfurization system is in accord with the first-order reaction kinetics equation. The mechanism of oxidative desulfurization was proposed.
Scientific Research
Hydrogenation Kinetic Model for Removal of Trace Olefins from Alkylation Mixture of Linear Alkylbenzene Synthesis
任杰 刘冰 慎炼
2019, 21(1):  46-54. 
摘要 ( 129 )   PDF (478KB) ( 1047 )  
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Through the hydrogenation experiments for removal of olefin impurities in effluent mixture obtained from alkylation reactor for linear alkylbenzene synthesis, the reaction kinetics was studied. The experimental results showed that the catalytic activity of Pd/Al2O3 among four kinds of catalysts was the highest, and the olefin conversion reached 100% when the reaction temperature was higher than 140 °C. The kinetic model was established through parameters estimation. The experimental validation of the kinetic model showed that the kinetic model had higher simulation accuracy. The results of prediction by the kinetic model indicated that with the intensification of reaction conditions, the olefin conversion would increase and the bromine index of the linear alkyl benzene would decrease. Under the conditions covering a WHSV of 2.0 h-1, a temperature of 90 °C, and a hydrogen partial pressure of 1.5 MPa, the olefin conversion was 99.67%, and the bromine index of the linear alkyl benzene could be reduced to less than 20.00 mgBr/(100 g).
植物油催化裂解生成低碳烯烃和轻芳烃的研究
成晓洁
2019, 21(1):  55-61. 
摘要 ( 161 )   PDF (549KB) ( 942 )  
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使用含择形分子筛的催化剂在固定流化床(FFB)装置上开展了对以棕榈油为代表的植物油及三种烃类原料的催化裂解试验研究,结合氢转移反应探讨了植物油催化裂解制取低碳烯烃和轻芳烃的优势。结果表明,植物油中的烃基部分具有很好的可裂化性,可生成与烃类原料相当的低碳烯烃及远高于烃类原料的轻芳烃,汽油重芳烃、柴油、重油等低价值、难利用产物的产率较低;植物油中的烃基部分极易发生芳构化,且容易进入择形分子筛孔道,选择性生成C6~C8的轻芳烃;植物油及脂肪酸催化裂解时通过氢转移反应以水的形式脱除了一部分氧,同时避免了烯烃被饱和,有利于兼顾低碳烯烃和轻芳烃的产率。
基于溶胶凝胶法的二氧化硅负载功能化离子液体用于高效脱除硫化氢
马云倩 毛家明 肖聪 李岩 臧立华
2019, 21(1):  62-70. 
摘要 ( 181 )   PDF (728KB) ( 971 )  
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采用溶胶凝胶方法,将几种金属基离子液体([Bmim]Cl?CuCl2, [Bmim]Cl?FeCl3, [Bmim]Cl?ZnCl2, [Bmim]Br?CuCl2和[Bmim]Br?FeCl3)固定于二氧化硅上,开发了一种新型的H2S捕集方法,与纯的粘性离子液体脱硫高温的限制、低传质率和质量损失的缺点,该方法具有显著优势。采用傅里叶变换红外光谱、透射电镜、氮气吸附/脱附、x射线光电子能谱和热重分析技术对吸附剂进行了表征。采用气体流速为100mL/min的动态吸附实验,研究了一系列影响因素包括离子液体中的金属和卤素、离子液体负载量和吸附温度。H2S吸附结果表明,最佳吸附剂为5%[Bmim]Cl?CuCl2/硅胶,最佳吸附温度为20-50?C。H2S可以被捕获并氧化为单质硫,[Bmim]Cl?CuCl2/硅胶可以很容易被空气再生。H2S的高效去除可能是由于在硅胶中形成了纳米级高浓度的[Bmim]Cl?CuCl2,由此表明,采用溶胶凝胶技术将[Bmim]Cl?CuCl2固定于二氧化硅上,有望用于H2S的去除。
烷烃的定容喷射自燃研究
王俊 杨鹤 宋海清 田华宇 王鹏飞
2019, 21(1):  71-79. 
摘要 ( 155 )   PDF (921KB) ( 954 )  
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In this study, spray auto-ignition experiments were carried out on a constant volume combustion chamber for some alkanes like n-paraffins with different chain length, cyclohexane, n-butyl cyclohexane, and isooctane. The auto-ignition qualities of n-heptane, isooctane and n-decane under different initial chamber temperature were investigated in details. Results showed that n-paraffins’ reaction activity was relatively high. Meanwhile, the auto-ignition characteristics differed significantly with different molecular structure. Adding n-decane with various volume fractions to Standard Blended Fuel and product gasoline would improve the fuel reaction activity to varying degrees. At last, the functional groups effects were formulated to simulate the relationship between molecular topology and auto-ignition quality.
Impacts of gettability on immiscible fluid flow pattern - Microfluidic chip experiment
Xianglei Zheng Jaewon Jang
2019, 21(1):  80-89. 
摘要 ( 199 )   PDF (2273KB) ( 987 )  
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Immiscible fluid flow is frequently found in resource recovery or soil remediation. The flow pattern of the fluids in the porous media is governed by the wettability of pore surface. In this study, quartz substrates and microfluidic chips are treated by silica nanoparticles (SNP) and triethoxy(octyl)silane (TES) to fabricate water-wet and oil-wet surface. The wettability of the treated-surface is measured in terms of contact angle for several combinations of surrounding fluid and a liquid droplet such as water in air, oil in air, water in oil, and oil in water. The effect of the wettability on the fluid flow pattern is explored by injecting oil and water alternately into the surface-treated microfluidic chips. The results show that the SNP-coated quartz substrate shows strong water-wet property; however, the TES coating makes water-repellent/oil-wet surfaces. In addition, the maximum and minimum oil and water saturation during invasion are dependent on the surface wettability of the microfluidic chip. The characteristics in the pore-scale fluid flow pattern are also described.
Compatibility Evaluation between Direct Coal Liquefaction Residue and Bitumen
季节 武昊 许鹰 索智 魏建明 Qing li DAI Ran Zhang Aboelkasim Diab
2019, 21(1):  90-100. 
摘要 ( 187 )   PDF (1249KB) ( 980 )  
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The compatibility between direct coal liquefaction residue (DCLR) and pure bitumen, including five commercial brands (Shell-90, SK-90, ZSY-70, DM-70 and KLMY-50), was investigated in this study. The rheological characteristics, glass state temperature (Tg), solubility parameter (SP) and SARA (saturate, aromatic, resin and asphaltene) fractions of DCLR, pure bitumen and DCLR modified bitumen were measured using the dynamic shear rheometer (DSR), differential scanning calorimetry (DSC), viscosity and SARA tests, respectively. The compatibility between DCLR and different bitumens was analyzed using different approaches including Cole-Cole plot, Tg and solubility parameter difference (SPD) methods. The test results showed that Shell-90 bitumen had the best compatibility with DCLR compared to the other studied four bitumens. The bitumen with higher penetration grade and lower asphaltenes content had a good compatibility with the DCLR. Additionally, the compatibility between the DCLR and bitumen is affected by the DCLR content. To maintain a good compatibility, the bitumen should not be overdosed with DCLR. Moreover, the conclusions for the compatibility between bitumen and DCLR through different methods were in good agreement with each other.
Lubrication Research
改善生物柴油碳烟在液体石蜡中的摩擦学行为的新方法
李川 张俊 吴波 张强强 庄远 胡献国
2019, 21(1):  101-109. 
摘要 ( 144 )   PDF (1227KB) ( 922 )  
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为了改善生物柴油碳烟(BDS)在液体石蜡(LP)中的摩擦学行为,通过500℃的热氧化处理,BDS的有序化程度增加,进一步利用油胺(OLA)修饰改善其油溶性。借助TG、FETEM、拉曼光谱仪、FTIR和Zeta电位仪对BDS和热氧化处理-油胺修饰的BDS(T-BDS-OLA)进行了表征;采用球-盘往复摩擦试验机、FESEM、3D激光扫描显微镜和拉曼光谱仪考察了BDS和T-BDS-OLA的摩擦学行为和作用机理。结果表明:T-BDS-OLA具有洋葱状结构,且比BDS具有更高的有序度;当碳烟的添加量为0.1-0.4 wt%, BDS和T-BDS-OLA均可以改善LP的减摩和抗磨性能,但T-BDS-OLA在LP中的抗磨减摩性能更佳。机理分析显示BDS和T-BDS-OLA均可以阻止摩擦副直接接触且起到滚动轴承的作用;此外,T-BDS-OLA剥离产生的片状石墨形成碳润滑层有利于滑动。
含氮生物降解促进剂对土壤吸附正十六烷的影响
范兴钰 陈波水 吴江 谷科城 丁建华 伍科
2019, 21(1):  110-116. 
摘要 ( 94 )   PDF (482KB) ( 986 )  
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Effects of nitrogen-contained biodegradation enhancers: methyl diethanolamine oleate (MDEAO) and oleic diethanolamide (ODEA) on the adsorption behavior of n-hexadecane in soil were studied by laboratory batch experiments. The effect of two biodegradation enhancers on the partition coefficient (Kd values) and normalized to organic matter (Koc values) were determined. The adsorption isotherm curve of n-hexadecane in soil-water system were plotted. The measured results demonstrated that Koc values changed in the soil-water system with different enhancers but are relatively invariant for the same site soil. The Kd values rose with the increase of the organic matter content in different soil. The average values of Koc in soil-water system with MDEAO, ODEA and blank soil were 0.412, 0.252 and 0.309, respectively. The critical micelle concentration of ODEA and MDEAO were 0.7 mg/L and 1.9 mg/L, respectively, which means the solubilization capacity of ODEA is much stronger than MDEAO in soil-water system. Consequently, adsorption of MDEAO onto the solid surface increases the organic matter content in soil and makes it more effective in enhancing n-hexadecane adsorption. Oppositely, ODEA inhibits the adsorption of n-hexadecane due to less adsorption onto the soil particle surface and higher concentration in the soil-water system. According to the correlation coefficients, it was found that both Henry linear and Freundlich nonlinear isotherm sorption models were fitted to the data very well but the Freundlich model was better.
Simulation and Optimization
浆态床外环流反应器错流微滤过程的建模研究
郑博 唐晓津 张占柱 宗保宁
2019, 21(1):  117-122. 
摘要 ( 113 )   PDF (773KB) ( 937 )  
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<html dir="ltr"><head></head><body>建立了涵盖孔堵塞模型和滤饼层过滤模型的组合模型来描述气升式浆态床外环流反应器内连续错流微滤过程。基于膜孔标准堵塞机理和膜孔中间堵塞机理,建立了孔堵塞耦合模型;基于颗粒流体动力学建立了滤饼层过滤模型,并对该过程中的滤饼层空隙率计算进行了新的修正。采用空气-水-FCC平衡剂体系的冷态过滤实验结果对该模型进行验证。结果表明,模型的计算结果与实验结果吻合较好,计算相对误差在10%以内。</body></html>
Design, Optimization and Control of Extractive Distillation for the Separation of Ethyl Acetate-Ethanol-Water Using Ionic Liquids
马守涛 商先勇 李鲁闽 薛长勇 李杰 孙兰义
2019, 21(1):  123-132. 
摘要 ( 141 )   PDF (1095KB) ( 1354 )  
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In this work, the process simulation of pressure-swing distillation (PSD) and extractive distillation (ED) using ionic liquid (IL) 1-butyl-3-methylimidazolium acetate ([bmim][OAc]) as the entrainer for separation of ethyl acetateethanol-water mixture is performed. The design parameters of the two distillation processes are optimized with the minimum total annual cost (TAC) serving as the objective function. The results show that the TAC saving of ED process is 35.27% in comparison with that of PSD process in the case of achieving the same purity and yield of ethyl acetate. In addition, the dynamic controllability of ED process is further studied. The traditional two-point temperature control structure is proposed for the ED process, and it works pretty well while taking into account the disturbances in both feed rate and feed composition.