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    1. Synergistic effect between Zr-MOF and phosphotungstic acid for oxidative desulfurization
    宗梦雅 赵雨桐 范存正 王丹红
       2020, 22 (4): 56-62.  
    摘要154)      PDF(pc) (919KB)(627)    收藏
    PTA/UiO-66 composites were successfully synthesized by the hydrothermal method. The results showed that the synergistic effect between phosphotungstic acid (PTA) and UiO-66 could enhance the oxidative desulfurization (ODS) activity. The XRD results proved that UiO-66 remtained its structure in the PTA/UiO-66 composites. The SEM results showed that the PTA/UiO-66 catalysts exhibited regular octahedral shape. The Raman spectra revealed that PTA in the composites remtained the Keggin structure. The XPS results showed that the electron transfer occurred from Zr-MOF to PTA. The ODS reaction mechanism was discussed. Electrons transfer from Zr-MOF to PTA can promote the generation of active species (?OH) and thus enhance the ODS activity. This explanation can be confirmed by the formation of oxygen vacancy and W0 as revealed by the XPS analysis.
    相关文章 | 多维度评价
    2. 工业管式反应器中乙烷蒸汽裂解过程的建模与优化
    Mohsin Ali 廖祖维 杨遥 孙婧元 蒋斌波 王靖岱 阳永荣
       2020, 22 (4): 117-125.  
    摘要289)      PDF(pc) (639KB)(605)    收藏
    Ethane steam cracking process in an industrial reactor was investigated. A 1-demsional (1D) steady-state model was developed firstly by using an improved molecular reaction scheme and then simulated in Aspen Plus. A comparison of model results with industrial data and previously reported results showed that the model can predict the process kinetics more accurately. In addition, the validated model was used to study the effects of different process variables, including coil outlet temperature (COT), steam-to-ethane ratio and residence time on ethane conversion, ethylene selectivity, products yields and coking rate. Finally, steady-state optimization was conducted to the operation of industrial reactor. The COT and steam-to-ethane ratio were taken as decision variables to maximize the annual operational profit.
    参考文献 | 相关文章 | 多维度评价
    3. Comparative effect of gasoline formulations on fuel economy and emissions of modern GDI Engine
    韩璐 田华宇 libo 郭莘 卢文彤
    中国炼油与石油化工    2020, 22 (4): 10-20.  
    摘要143)      PDF(pc) (2260KB)(603)    收藏
     Experiments researching about the effect of gasoline formulations on fuel economy and emissions were conducted on a modern gasoline direct inject (GDI) engine. The objective of this study was to explore the gasoline formulations that can alleviate energy crisis and greenhouse effect to some extent. Five gasoline blends with same research octane number (RON) were designed and tested on a calibrated GDI engine under mapping characteristics conditions. Results illustrate that the optimized fuel formulation improves the fuel economy and reduces carbon dioxide (CO2) emissions at medium loads and low speeds of engine. The BSFC decreased by the maximum value of 3.26% mainly owing to the improvement of combustion velocity and the optimization of lower heat value. The optimized fuel formulation simultaneously increases total hydrocarbon (THC) emissions, which barely observed in non-methane hydrocarbon (NMHC) emissions. Nevertheless, the optimized formulation fuel markedly reduces CO2 emissions, reaching the maximum value of 2.34%. The research results can practically applicate by refineries to reduce the CO2 emissions and alleviate the greenhouse effect.
    参考文献 | 相关文章 | 多维度评价
    4. 萃取精馏与变压精馏分离甲醇-乙腈共沸物的研究
    韩东敏 陈艳红
       2020, 22 (4): 137-146.  
    摘要243)      PDF(pc) (1263KB)(592)    收藏
    In the present work, a comparative study of the extractive distillation and pressure swing distillation for methanol-acetonitrile azeotropic separation is performed for the first time. Different separation alternatives, including the conventional extractive distillation, the extractive distillation with vapor or liquid side-stream, the pressure-swing distillation with or without full heat integration, and the heat-pump assisted pressure-swing distillation are rigorously simulated and optimized based on the minimum total annual cost (TAC) via the sequential iterative strategy. The results show that TAC and CO2 emission of the new extractive distillation with vapor side-stream (Vapor-SED) are similar to that of the extractive distillation with liquid side-stream (Liquid-SED). Furthermore, the Vapor-SED and Liquid-SED gives 30.01% and 30.56% reduction in TAC and 23.32% and 23.49% reduction in CO2 emission, respectively, over the most competitive fully heat-integrated PSD configuration. Hence, extractive distillation with vapor or liquid side-stream appears to be better option economically and environmentally for separation of methanol and acetonitrile.
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    5. Study on combustion performance of Mn based binary carrier catalyst for ventilation air methane
    徐鑫 刘文革 齐健 于雷 韩甲业 李志
       2020, 22 (4): 26-34.  
    摘要132)      PDF(pc) (1779KB)(549)    收藏
    La-Al2O3 and Ce-Al2O3 binary monolithic column materials with dual functions of carrier and promoter were prepared in one-step by the sol-gel method. Using the as-synthesized binary monolithic column materials as carrier, the 9%Mn/M-Al2O3 (M=La/Ce) catalyst was prepared by the impregnation method. The binary carrier and catalyst were characterized by BET, SEM, XRD, H2-TPR, and O2-TPD techniques, and the methane combustion performance was tested in a micro fixed-bed reactor. Results showed that the Mn-based binary carrier catalyst with dual functions of carrier and promoter had higher catalytic activity than that with single alumina acting as the carrier. The catalyst activity gradually increased with an increasing content of La, while there was no significant effect with the increase in Ce content. When the ratio of La content in La-Al2O3 is 11%, 1 % of methane contained in the ventilation air can be completely converted over the 9%Mn/11% La-Al2O3 catalyst at a temperature as low as 550℃.
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    6. Simulation and Experimental Study on the Effect of Dispersants on Soot Aggregation
    刘琼 武志强 黄作鑫 张峰 赵毅
    中国炼油与石油化工    2020, 22 (4): 101-107.  
    摘要146)      PDF(pc) (931KB)(544)    收藏
    Diesel engine technology innovation causes excessive soot accumulated in engine oil. Due to its detrimental effect on lubricant and diesel engine, to improveing the dispersibility of engine oil to restrain soot aggregation efficiently is the key technique for formulations. In this study, the aggregation of soot and interaction between dispersant and soot were investigated by molecular dynamic simulation. It was found that the molecular interaction between the dispersant and the soot aggregation system have had a significant influence on disrupting the soot aggregation. Bis-PIBSI was more beneficial to have having more interaction sites with soot molecules and, while the mono-PIBSI with the a high proportion of polar groups had stronger interaction with soot molecules. According to the simulation result, suggestions for use of additives were proposed. Carbon black dispersancy test was exploited to verify the dispersion effect of different dispersants on carbon black. The results indicate that mono-PIBSI and bis-PIBSI added in at suitable mixture ratio to lubricant would could perform good dispersion ability.
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    7. Oil phase molecular compositions of oily sludge using mass spectrometry
    胡林 吕海鹏 王光华 郭宪厚
       2020, 22 (4): 21-25.  
    摘要147)      PDF(pc) (647KB)(527)    收藏
    As the hazardous wastes, recycling the high petroleum hydrocarbon content of oily sludge contributes to clean environment. In this study, Oily sludge was subjected to ultrasonic extraction sequentially with acetone/carbon disulfide mixture solvent. Fourier transform infrared spectroscopy (FTIRS), Gas chromatography/mass spectrometry (GC/MS) and Quadrupole exactive orbitrap mass spectrometry (QPEOTMS) were used to analyze oil phase compounds of oily sludge. The n-alkanes detected in oil phase ranging from C8 to C31. Compared with analysis results of GC/MS, more heteroatom-containing compounds of oil phase such as O3, O4, N2Oo and N3Oo (o=0-3) could be detected in the analysis of QPEOTMS. Overall, these findings will potentially contributed to the clean and efficient utilization of oliy sludge wastes.
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    8. 我国典型中间基原油炼化一体化加工方案的技术经济分析与生命周期评价
    周鑫 闫昊 冯翔 赵辉 刘熠斌 陈小博 杨朝合
       2020, 22 (4): 35-45.  
    摘要167)      PDF(pc) (1920KB)(525)    收藏
    炼化一体化(IRPUs)已成为石化工业可持续发展的必然选择。选择这样的配置可以提高石油资源的利用效率。然而,将经济和环境影响纳入IRPUs模型仍然是一个巨大的挑战。本文在Aspen HYSYSTM平台上建立了TEA-GHG-OPWM(面向全厂的技术经济分析和温室气体排放模型)模型,计算了减压渣油加氢裂化(VRHCRU)和减压渣油脱硫(VRDS-RFCC)两种方案的能耗、技术经济性和温室气体排放。此外,还开发了一种新的加工途径VGOHDT-HTMP-DC(减压蜡油加氢处理-加氢与TMP耦合工艺-延迟焦化),以期在千万元产值的基础上寻求提高经济效益和减少温室气体排放的方法。结果表明,VRHCRU比VRDS-RFCC(817.03 tCO2 eq·TMYOV-1·h-1)和VGOHDT-HTMP-DC(721.96 t CO2 eq·TMYOV-1·h-1)具有更高的能耗和温室气体排放量(877.11 t CO2 eq·TMYOV-1·h-1)。VGOHDT-HTMP-DC工艺的原料消耗、氢气消耗、能耗和温室气体排放最低,表明VGOHDT-HTMP-DC具有良好的经济性和环保性。
    相关文章 | 多维度评价
    9. HTS分子筛催化甲苯无有机溶剂条件下的氧化溴化反应研究
    彭欣欣 夏长久 林民 朱斌 罗一斌 舒兴田
       2020, 22 (4): 1-9.  
    摘要194)      PDF(pc) (877KB)(516)    收藏
    本文研究了双氧水和溴化氢溶液体系中,空心钛硅分子筛(HTS)催化甲苯在无有机溶剂条件下的氧化溴化反应。在优化的反应条件下,甲苯转化率可达90.7%,一溴甲苯选择性达99.0%。采用UV-Raman光谱对甲苯溴化反应的机理进行了研究。结果表明,HTS分子筛可高效催化溴化氢和双氧水氧化反应并生成大量的活性溴物种,该溴物种可通过亲电取代反应进一步促进甲苯溴代制备一溴甲苯。基于拉曼光谱的研究结果,提出了基于HTS分子筛催化的活性溴物种“产生-存储-反应”的甲苯溴化两步反应机理。
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    10. 导向剂法合成多级孔SAPO-11分子筛及其对烷烃加氢异构化的性能
    孟媛 王海彦 SUN Na 杨占旭 王钰佳
       2020, 22 (4): 85-92.  
    摘要106)      PDF(pc) (1023KB)(508)    收藏
    Silicoaluminophosphates SAPO-11 molecular sieves with small particle size and hierarchical pores were synthesized using a directing agent method. The effect of crystallization time on the crystal structure, morphology, pore structure properties and acid properties of SAPO-11 molecular sieves were investigated. The results of XRD, SEM, BET and NH3-TPD showed that the SAPO-11 molecular sieves with fine and uniform morphology could be synthesized in a shorter crystallization time used the directing agent method, which just unlike the SAPO-11 molecular sieves synthesized with the conventional method. With the crystallization time increased, the particle size of SAPO-11 molecular sieve was significantly reduced, and the mesoporous structure (intercrystalline pore) was generated between the particles. Furthermore, the external specific surface area and the total specific surface area reached 81.7 m2g-1 and 192.0 m2g-1, respectively, which effectively reduce the pore mass transfer resistance, significantly increase the number of acid active sites. The results of n-dodecane hydroisomerization revealed that the Pt/SAPO-11 prepared with the novel method exhibited higher catalytic activity and better hydroisomerization selectivity than the Pt/SAPO-11 synthesized by conventional hydrothermal method. Thus, the small particle molecular sieve has promising industrial applications as catalyst support.
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    11. 高岭土/尿素插层复合材料合成ZSM-5分子筛及表征
    郑淑琴 陈欧 刘思成 张培青
       2020, 22 (4): 93-100.  
    摘要120)      PDF(pc) (1111KB)(485)    收藏
    研究了直接插层法制备高岭土/尿素插层复合材料和以该材料采用原位技术合成含ZSM-5分子筛的催化复合材料。重点研究了插层率、脱嵌速率、插层复合材料加入量对合成分子筛复合材料的影响。采用粉末X射线衍射法(XRD),红外光谱(FT-IR),热重-差热(TG-DTA),N2 静态吸附法和电子扫描电镜(SEM)对样品进行表征。结果表明,在合成体系中加入高岭土/尿素插层复合物合成出的ZSM-5分子筛物相单一。随着插层复合物的插层率增加,ZSM-5分子筛的结晶度先增加随后降低。当插层率为62%时,ZSM-5分子筛的结晶度较低。当22%插层率的插层复合物的加入量为3%时,ZSM-5分子筛的结晶度达到65%。与不添加插层复合物合成的产物相比,ZSM-5分子筛的结晶度提高了54.8%。合成的ZSM-5分子筛复合材料具有较好的热稳定性和多级孔道结构,其粒径约为2.5μm,BET比表面积为236m2/g,孔径为10.6nm。
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    12. Analysis, Prediction and Process Optimization Concerning Ammonium Chloride Corrosion in Ebullated-Bed Hydrogenation Unit Treating Residual Oil
    包振宇 王宁 张宏飞 段永锋 于凤昌
    中国炼油与石油化工    2020, 22 (4): 108-116.  
    摘要110)      PDF(pc) (1113KB)(482)    收藏
    Ammonium chloride corrosion in the reactor effluent system remains to be a barrier for the safe operation of the ebullated-bed hydrogenation unit as impurity contents are higher compared with that of the ordinary hydrogenation units. In this research, a case study in Sinopec was provided with 2.92 μg/g Cl and 0.38% N in the feed oil, and the impurity contents was representative in residue oil. The deposition patterns in heat exchangers were investigated by changing process variables, then water wash strategy was optimized in view of relative humidity, and the minimum water flowrate was obtained, finally, process optimization suggestions concerning the operation of heat exchangers were proposed. Results show that with the measured content of nitrogen and chlorine in the feed, the NH4Cl deposition temperature of hot high-pressure vapor and hot low-pressure vapor are 223.4 °C and 173.7 °C, respectively, and the minimum water wash flowrate for heat exchangers of hot high-pressure vapor with mixed hydrogen and hot low-pressure vapor with cold low-pressure oil are 38.0 t/h and 5.4 t/h, respectively. Water wash should be carried out intermittently upstream of the heat exchanger tube passes. In consideration of energy consumption, it is recommended to reduce the tube pass outlet temperature of the above heat exchangers to 240 °C and 190 °C, respectively.
    参考文献 | 相关文章 | 多维度评价
    13. 炼化一体化项目多个相互连接蒸汽动力系统设计优化
    白浩博 李士雨 王徐鹏 刘昶
       2020, 22 (4): 126-136.  
    摘要175)      PDF(pc) (1898KB)(451)    收藏
    在炼化一体化项目中,有一个动力中心(CUS , centralized utility system)用来集成各生产装置蒸汽需求,还有两个分别位于炼厂和乙烯厂中的子蒸汽动力系统(SUSs, sub-utility systems)为工艺过程提供驱动力。SUSs的结构和操作条件会影响炼油和乙烯装置的蒸汽需求,因此很难确定CUS的蒸汽产量。为了探究CUS和SUSs间复杂的相互影响,本文提出了一个混合整数非线性规划模型(MINLP, mixed-integer nonlinear programming),以实现多个相互连接蒸汽动力系统设计优化,从而降低系统年度总费用(TAC, total annualized cost)。本文还建立了一个包含CUS和SUSs厂间蒸汽连接管道的超结构,同时提出了一个更准确的复杂蒸汽透平模型。将本文建立的MINLP模型用于某新建炼化一体化项目。为探究蒸汽主管温度对系统结构和操作条件的影响,研究了两个不同场景下的案例。通过优化主管温度,使系统TAC降低了$2,700,000。从优化结果可知,本文建立的优化模型可以有效解决多个相互连接蒸汽动力系统设计优化问题。
    参考文献 | 相关文章 | 多维度评价
    14. 通过晶种胶作导向剂的凝胶预陈化路线合成多级孔道FAU/α-Al2O3整体材料
    王佳 靳其兵 赵天波
       2020, 22 (4): 46-55.  
    摘要142)      PDF(pc) (1483KB)(427)    收藏
    以整体型α-Al2O3为载体,晶种胶作导向剂,通过凝胶预陈化路线合成了多级孔道FAU整体材料。对合成的样品进行了FT-IR、XRD、SEM和N2吸附脱附表征。根据实验结果确定了晶种胶、凝胶预处理及预陈化步骤的作用,同时提出了不同路线生成氧化铝复合物可能的合成机理。结果发现:负载的FAU沸石的粒径、形状及数量可通过改变晶化凝胶的组成,并且α-Al2O3载体的结构没有明显改变。具有简单、可重现且易将三重孔道结构融于成型的整体材料中的特点,通过晶种胶预处理的凝胶预陈化路线可加强载体内表面与沸石间的界面作用,形成纯相FAU晶体沉积在α-Al2O3载体骨架表面的形貌。另外,该方法可为其他的多级孔道沸石的合成提供思路。                           
     
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    15. 金属酞菁的同步合成与固载及其催化分子氧氧化苯乙烯
    刘叶峰 吕迎 李泽宇 申越 王蕊欣
       2020, 22 (4): 73-84.  
    摘要106)      PDF(pc) (1915KB)(408)    收藏
    In this study, the precursor 4-(4-carboxy-phenoxy) phthalonitrile (CPPN) was first bonded onto the silica gel surface modified with poly(glycidyl methacrylate) (PGMA) (PGMA/SiO2) to prepare CPPN-PGMA/SiO2, and metal phthalocyanine (MPc; M=Co, Fe, Cu, Mn) was supported on the PGMA/SiO2 surface to prepare MPc-PGMA/SiO2 by synchronous synthesis and immobilization with phthalonitrile and metal salt in the solution. The chemical composition and surface morphology were characterized by the Fourier transform infrared (FTIR) spectroscopy, UV-Vis spectroscopy, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and thermogravimetry analysis (TGA). The catalytic performance of MPc-PGMA/SiO2 in epoxidation of styrene was also investigated with molecular oxygen acting as the oxidant. The results show that MPc-PGMA/SiO2 can efficiently and selectively catalyze molecular oxygen for oxidation of styrene to styrene oxide under mild conditions. However, the catalytic activity differs substantially depending on the central metal, and a highest catalytic activity is achieved by CoPc-PGMA/SiO2. The CoPc-PGMA/SiO2 amount and temperature can also affect the catalytic oxidation of styrene, and at normal atmospheric pressure, a maximum conversion rate of styrene (99%) and selectivity of styrene oxide (53%) are obtained using 0.1 g of CoPc-PGMA/SiO2 (22.61 μmol of CoPc) at 100 ℃ for 6 h. CoPc-PGMA/SiO2 also has excellent reusability, and the conversion rate of styrene is still over 90% after 5 cycles.
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    16. Stability Enhancement of ZSM-5 zeolite in Olefin Aromatization by Alkali Treatment. Comparison of Medium
    陈小博 安志远 朱超 闫昊 刘熠斌 冯翔 金鑫 杨朝合
       2020, 22 (4): 63-72.  
    摘要132)      PDF(pc) (1237KB)(402)    收藏
    ZSM-5 zeolites with a SiO2/Al2O3 ratio of 40 were synthesized by a hydrothermal method, and treated by 0.3 M tetrapropyl ammonium hydroxide (TPAOH) and 0.3 M sodium hydroxide (NaOH) separately to create hollow structures. The synthesized ZSM-5 zeolite and treated ZSM-5 zeolites were evaluated for aromatization of 1-hexene in a continuous flow reactor. The prepared ZSM-5 zeolites were characterized by XRD, SEM, TEM, NMR, XPS and other analyses. The results showed that the alkali treatment formed mesopores and hollow structures in the ZSM-5 crystals without destroying the topological structure. The acid amount of ZSM-5 zeolite was also increased after alkali treatment. Compared with the ZSM-5 zeolite treated by TPAOH, the ZSM-5 zeolite treated by NaOH had more mesopores and a higher total acid amount but a lower strong acid amount, resulting in higher aromatics yields and catalytic stability in 1-hexene aromatization. The characterization of spent ZSM-5 zeolites suggested that the spent treated ZSM-5 zeolites contained less coke, leading to a smaller reduction of micropore surface area and volume than in the spent parent ZSM-5, which contributed to the stability enhancement.
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    17. DIFFUSION AND ADSORPTION OF TETRALIN HYDROCRACKING REACTION ON DIFFERENT ZEOLITES BY MOLECULAR SIMULATION
    孙立杰 樊亚明 董松涛 羡策 龙湘云 李大东
    中国炼油与石油化工    2021, 23 (1): 1-9.  
    摘要187)      PDF(pc) (1573KB)(358)    收藏
    Three different zeolite catalysts with different pore sizes (MFI-type, BEA-type, and FAU-type zeolites) have been prepared. The influence of different zeolite catalysts on reactivity and product shape selectivity of tetralin is investigated. Clear differences are observed in the reactivity of tetralin and distribution of products produced by different catalysts. The diffusion and adsorption of the reactant tetralin and its intermediates, n-butylbenzene and 1-methyl indan, under the reaction conditions are calculated using molecular simulation methods. Combining simulation results and experimental observations, it is shown that the difference in diffusion coefficient and competitive adsorption capacity can explain the reactivity of tetralin and the selectivity of products. The steric hindrance of MFI-type zeolite mainly limits the key step of ring opening of tetralin, leading lower selectivity of ring-open products. N-butylbenzene molecules diffuse sufficiently fast in the large pores of FAU-type zeolite and the weak adsorption capacity of n-butylbenzene leads to its insufficient cracking. In addition, it also explains the reason that BEA-type zeolite has the best BTX selectivity, because it can satisfy both good ring-opening activity and sufficient butylbenzene cracking depth. Key words: hydrocracking; tetralin; molecular simulation; diffusion; competitive adsorption.
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    18. 石油化工中的结晶
    张得江 范瑛琦 谢丽 丁晖殿 王皓
    中国炼油与石油化工    2021, 23 (2): 1-10.  
    摘要369)      PDF(pc) (734KB)(340)    收藏
    结晶是一种应用广泛的产品精制单元操作。了解石油化工中结晶过程的特点,有助于选择和设计新的结晶工艺。本综述简要介绍了结晶工艺的特点,总结了在石油化工中应用的结晶工艺,讨论了结晶工艺设计中应注意的问题。石油化工工艺中的结晶主要用于聚合物单体的提纯,并且往往是整个精制流程中的一部分。合理的设计一个结晶工艺,需要从全局考虑工艺的安全性、可行性和经济性。
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    19. 分子动力学模拟研究大分子润滑油氧化产物的运动和聚集行为及其对基础油性能的影响
    夏垒 李岩 张红梅 姜正义 龙军
       2020, 22 (3): 101-108.  
    摘要151)      PDF(pc) (1714KB)(328)    收藏

    采用分子动力学模拟研究了大分子润滑氧化产物的运动和聚集行为及其对基础油性能的影响通过计算分子的均方位移研究分子的运动能力,通过观察润滑油氧化产物在模型中的分布研究氧化产物的聚集行为。研究结果表明:大分子润滑油氧化产物的运动能力低于基础油分子。随着润滑油氧化产物分子量的提高,其均方位移不断降低。大分子润滑油氧化产物还可以使基础油分子的运动能力降低,二者之间的相互作用能随着大分子润滑油氧化产物分子量的增大而升高。分子量较大的润滑油氧化产物可以对更多的基础油分子产生更强的限制作用,因此其可以导致基础油运动能力降低的更多。大分子润滑油氧化产物之间可以通过氢键形成聚集体,氢键的数量与温度有关。

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