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2012年 第14卷 第4期    刊出日期:2012-12-30
目录
目录
2012, 14(4):  0-01. 
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Catalyst Research
烃分子在FAU和MFI分子筛中扩散的研究
袁帅 刘宇键 田辉平 代振宇 赵毅 周涵 龙军
2012, 14(4):  1-8. 
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采用分子模拟方法,系统地对C4~C24的烷烃、芳烃和环烷烃分子在FAU和MFI分子筛孔道中的扩散过程进行了深入研究,得到了丰富的扩散特性基础数据和一系列烃分子在分子筛孔道中的扩散规律。通过对烃分子在FAU和MFI分子筛孔道中的扩散过程进行深入、细致的分析,发现FAU分子筛中两超笼之间的十二元环是烃分子在孔道中扩散的主要障碍。在MFI分子筛直孔道中,烃分子从孔道交叉处向直孔道移动是扩散的主要障碍。由于MFI正弦孔道中存在拐点原子,烃分子在正弦孔道中扩散比在直孔道中困难。采用重力吸附方法对三种C6烷烃在FAU、MFI分子筛孔道中的扩散进行了实验研究,分子模拟结果与实验研究结果吻合较好,验证了模拟结果的可靠性。
不同Al的含量对PtSn/Al2O3/SBA-15催化剂在丙烷脱氢催化性能的影响
张培新 周钰明 段永正 涨一卫 盛晓莉
2012, 14(4):  9-16. 
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铝修饰过的SBA-15(Al2O3/SBA-15)是在以甲苯为溶剂的非水体系制备的,并以其作为载体负载PtSn催化剂用于丙烷脱氢反应。所得到的催化剂利用BET比表面,氢气化学吸附,红外光谱,NH3-TPD, XPS 和 TPO 进行表征。结果发现Al的添加不但能够修饰载体的酸性功能,而且改变Pt金属的结构,这样将明显的影响到催化剂的催化性能。在这些研究的催化剂中,当Al组分含量为5%时,催化剂具有最佳的催化性能,这是因为具有高的金属分散度和/或Pt组分与Sn组分之间强的作用力所致。
The Preparation of Cu-BiVO4 and Its Photocatalytic Properties for Desulfurization of Model Oil
高晓明 王静 付峰 李稳宏
2012, 14(4):  17-23. 
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a photocatalyst Cu-BiVO4 was synthesized by hydrothermal method and characterized by XRD, UV-vis DRS, N2 adsorption-desorption measurement. Thiophene in n-octane as mode compound of light oil, the desulfurization activity of the Cu-BiVO4 samples was researched by photocatalytic oxidation in visible light. The characterized results indicated that the doping Cu did not change the crystal phase of BiVO4 and the crystallinity of the Cu-BiVO4 sample at pH=7 were better. The Cu-BiVO4 samples had a significant red-shift in the absorption band in the visible region, and the absorption intensity increased for the composite catalyst. The desulfurization experiment results show that the Cu-BiVO4 sample at pH=7 had a better catalytic activity. Under the proper operating conditions, the desulfurization rate of the Cu-BiVO4 sample at pH=7 to the model compound could reach 90%.
MCM-22分子筛催化剂上1-己烯骨架异构化反应的研究
宋毅 商丽艳 翟玉春
2012, 14(4):  24-27. 
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研究了MCM-22分子筛催化剂催化1-己烯异构化的反应性能。在n(H2)/n(1-hexene)=8的条件下考查了水处理温度、反应温度、反应压力对MCM-22分子筛催化剂上1-己烯骨架异构化产物的影响。研究表明:在水处理温度为500℃,反应温度270℃,1-己烯的质量空速1.0h-1,反应压力0.2MPa的条件下,MCM-22分子筛催化剂具有较高的1-己烯骨架异构化性能,骨架异构化产物(i-hexene)达到66.15%。与几种常用的分子筛催化剂相比,MCM-22分子筛催化剂具有更高的催化1-己烯异构化反应的性能。
NiZnO基吸附剂用于反应吸附脱除噻吩的研究
孟璇 翁惠新 施力
2012, 14(4):  28-32. 
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以NiZnO基吸附剂为研究基础,采用实验室小型固定床装置,系统研究噻吩在该吸附剂上的反应吸附脱除性能。采用X-射线衍射(XRD)以及程序升温还原(H2-TPR)等分析手段对吸附剂进行了表征。XRD分析结果表明:当吸附剂中Zn/Ni摩尔比为0.4时,此时ZnO与NiO之间的协同效应增强,从而能够形成了一种活性组分高度分散的吸附剂。TPR分析结果表明:NiZnO基吸附剂的较适宜还原温度为350-400℃之间。此外,还考察了反应温度以及反应压力对NiZnO基吸附剂用于反应吸附脱硫噻吩的影响。
Petrochemical Research
A “Green” cyclohexanone oxidation route catalyzed by Hollow Titanium Silicate zeolite to prepare e-Caprolactone,6-Hydrohexanic Acid and Adipic Acid
夏长久 朱斌 林民 舒兴田
2012, 14(4):  33-41. 
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The Hollow Titanium Silicalite (HTS) molecular sieve has been synthesized and investigated its structure information, physicochemical characterization, as well as surface property by using multiplicative analysis techniques, such as XRF, XRD, low temperature N2 adsorption/desorption isotherms, TEM, FT-IR, UV-vis, 29Si MAS NMR and XPS. Characterization results suggest that HTS is of special hollow crystal structure and its mesopore volume is larger than TS-1.The titanium species in this zeolite are including the framework tetrahedral Ti(IV) and extra-framework octahedral Ti(IV) ions, and it inclines to disperse into its bulk phase. This zeolite material also has been applied to catalyze the cyclohexanone oxidation process, and the products are not completely consistent with the results of TS-1, that may due to their difference in pore structure and pore volume, especially mesopore volume. Cyclohexanone oxidation catalyzed by HTS is a representative consecutive reaction, the main target products of are ?-Caprolactone, 6-Hydrohexanic Acid and Adipic Acid. The effects of mole ratio of H2O2/cyclohexanone on the cyclohexanone conversion, the total target product selectivity, the selectivity distribution of three target products and their variations along with reaction time are also researched and analyzed, it indicated that HTS is of high performance for cyclohexanone Baeyer-Villiger reaction and 6-Hydrohexanic Acid catalytic oxidation under the mild conditions, and the quantity of active surface titanium species as well as the pore structure and mesopore volume controlled the mass diffusion are the key factors to determine the HTS catalytic activity and their product selectivity.
由乙烯焦油合成缩合多环芳香烃树脂
吴明铂;Shi Yangyang1; Li Shibin1; Wang Yuwei1; Tan Minghui1;
2012, 14(4):  42-47. 
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乙烯焦油是一种价廉易得的石油炼制副产品,首次用于合成耐热缩合多环芳香烃树脂(COPNAR)。通过红外,核磁,热重,元素分析等,分析了乙烯焦油及产物COPNAR的组成,探讨了合成机理。研究发现:富含芳烃的乙烯焦油(芳烃含量在50%以上)可以合成耐热性COPNAR。包括平均分子结构在内的乙烯焦油的主要结构参数可通过元素分析,分子量分析,核磁分析及改进 Brown -Ladner 方法得到。合成机理被证明为酸催化的阳离子型缩聚反应。本研究为乙烯焦油的高附加值利用提供了一条新途径。
八羰基二钴催化环氧乙烷氢酯基化合成3-羟基丙酸甲酯
张业 周海军 谢鲜梅 陈小平
2012, 14(4):  48-51. 
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本研究以Co2(CO)8为催化剂、甲醇为溶剂,在一定CO压力下催化环氧乙烷氢甲酯化合成3-羟基丙酸甲酯,结果表明该催化剂具有较高的催化活性。考察了反应温度、CO压力、甲醇的量、催化剂的量以及反应时间对该反应的影响,其中反应温度对反应影响较大,而CO压力、甲醇的量、催化剂的量以及反应时间对反应影响较小。在最佳反应条件下,环氧乙烷的转化率、3-羟基丙酸甲酯的选择性和收率分别为92.24%、88.99%和84.35%。
Simulation and Optimization
Estimating the operation status of ethylene cracking furnace using numerical simulation with combustion models
周先锋 杨元一 王国清 张利军 刘逸
2012, 14(4):  52-63. 
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An accurate and complete geometric model was constructed to simulate combustion, flow and temperature in the radiant section of ethylene cracking furnace. Simulations of flow and radiation utilized standard k-ε model and P1 model. Finite-rate/eddy-dissipation (finite-rate/ED) combustion model and non-premixed combustion model were both used to simulate accurately the combustion and the operation status of the ethylene cracking furnace. Three different surfaces of the ethylene cracking furnace were obtained from the simulation: flue gas temperature field of the entrance surface in long flame burners, central surface location of tubes, and crossover section surface. Detailed information on the flue gas temperature and the mass concentration fraction of these different surfaces in the ethylene cracking furnace can also be obtained by the simulation. This paper analyzed and compared the simulation results with the two combustion models, estimated the operation status of the ethylene cracking furnace, and reported that finite-rate/ED model is appropriate to simulate ethylene cracking furnace by comparing key simulation data with actual test data. This work also provided the theoretical basis to simulate and operate ethylene cracking furnace.
采用组合进料方式的高密度循环流化床径向不均匀性指数研究
耿强 王璐 李志超 李春义 刘熠斌 尤兴华
2012, 14(4):  64-72. 
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应用高密度,高循环量循环流化床提升管(直径为100 mm,高度为10.614 m)在较宽操作范围内(颗粒循环量达到400 kg/m2s,表观气速达到12 m/s)研究了径向颗粒浓度分布的不均性情况。实验过程中使用光纤探头对11个轴向位置的颗粒浓度进行测量。结果表明,高气速、低循环量能够有效降低径向不均匀性指数。高密度循环流化床具有不同于低密度循环流化床的特性:径向颗粒浓度分布曲线峰值出现在r/R=0.8处,而不是传统认识上的提升管边壁处;径向颗粒浓度小于0.2时,径向不均匀性指数与颗粒浓度之间呈现较好的对数关系,当径向颗粒浓度均值大于0.2时,径向不均匀性指数呈现下降趋势。对分层进料进行了系统研究,结果表明分层进料比例对颗粒循环量和颗粒浓度的分布有重要影响:分层进料产生了新型“<”流形;调整上进料比例超过0.5时,提升管内颗粒循环量有明显下降趋势;上进料比例为1时,径向不均匀性指数最低。
Scientific Research
甲基环己烷催化裂解制乙烯和丙烯的反应研究
于珊 张久顺 魏晓丽
2012, 14(4):  73-79. 
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采用小型固定流化床装置研究了工艺参数和分子筛结构对甲基环己烷催化裂解生成乙烯和丙烯反应性能的影响。结果表明,较高的反应温度和较低的重时空速有利于乙烯和丙烯生成,其中反应温度是影响乙烯生成的重要因素;与FAU和BEA结构分子筛催化剂相比,有较多酸性中心和较小孔径的MFI结构分子筛催化剂有利于乙烯和丙烯的生成;甲基环己烷不同位置的C-C键和C-H键发生质子化反应的产物不同,其中环上C-C键的质子化反应有利于乙烯和丙烯的生成。
基于GC FI/FD TOF MS 和 APPI FT-ICR MS的茂名常渣加氢处理分子水平表征
刁瑞 王威 王乃鑫 刘泽龙 戴立顺 田松柏
2012, 14(4):  80-88. 
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Salt-Containing Extractive Distillation for the System of 1-Propanol/Water 1. Prediction of Salt Effect on Vapor Liquid Equilibrium
傅吉全 Fu Die
2012, 14(4):  89-96. 
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This paper studies on vapor-liquid equilibrium (VLE) of salt-containing extractive distillation for the system of 1-propanol/water. Binary VLE data were measured for the systems of 1-propanol (1)/KAc (4), ethanediol (3)/KAc (4) and 1-propanol (1)/ ethanediol (3),and the VLE data were correlated with NRTL model in order to obtain the model parameters of the binary systems. Literature binary VLE data were correlated to obtain the model parameters for others binary systems. Ternary and quaternary system VLE values predicted by NRTL model agreed with literature data. Influence of KAc, ethanediol, and the mixture of KAc and ethanediol on volatility between 1-propanol and water was investigated respectively. Results showed that the above materials (KAc,ethanediol) and mixture (KAc and ethanediol) have different influences on the volatility. When x3=0.5, and x4=0.05, the azeotropic point can be eliminated. NRTL Model Method of salt-containing VLE is simple and effective for the VLE prediction of the system.
纳米氧化物在基础油中的稳定性和摩擦学性能研究
邢锦娟 钱建华 刘琳 王宁 马全亮
2012, 14(4):  97-102. 
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本文以SDS,PEG800作为表面活性剂,采用均匀沉淀法在95℃下反应3h,在400℃焙烧3h后制得了目标产物。产品通过XRD,SEM,FTIR和Zeta电位分析进行了表征。采用不同修饰剂对该产品进行了处理以提高分散稳定性,并确定了最佳用量和最佳zeta电位值。将修饰后的纳米粒子以质量分数1.0%,2.0%,3.0%,4.0%的量加入到基础油中。结果表明,在基础油中添加纳米粒子具有良好的油溶性且对铜无腐蚀,此外还具有抗磨减摩性能。