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    1. 硅钨酸酸化的新型MIL-101(Cr)催化剂及其对正庚烷异构化反应的催化性能
    张微 刘荣江 马守涛 Dimitriy Kuvshinov 所艳华 汪颖军
    中国炼油与石油化工    2022, 24 (1): 68-80.  
    摘要412)      PDF(pc) (1596KB)(34)    收藏
    0.4%Pt/xSTA-MIL-101(Cr) metal-acid bifunctional catalysts were prepared by impregnation using STA-MIL-101(Cr) as the support. The synthesized samples were verified to exhibit a typical octahedral structure of MIL-101(Cr) and the pore structure were arranged orderly. The specific surface area of the samples was extremely high and the samples were micro-mesoporous composite materials. Silicotungstic acid could retain its Keggin structure in the 0.4%Pt/xSTA-MIL-101(Cr) samples and the catalyst possessed moderately strong Br?nsted acid sites. Besides, the dispersion of Pt particles in MIL-101(Cr) was relatively high. n-Heptane isomerization was first used as a probe to test the novel 0.4%Pt/xSTA-MIL-10(Cr) catalyst. Compared with the conventional silicate catalysts, the catalytic performance of 0.4%Pt/30wt%STA-MIL-101(Cr) was significantly improved with n-heptane conversion of 58.93% and iso-heptane selectivity of 95.68%, respectively, when the reaction time was 2 h at the reaction temperature of 260 oC. The catalyst could still maintain a relatively high catalytic performance during the reaction time of 5 h. Compared with the non-noble metal catalysts, the catalytic efficiency is relatively high. The mechanism model of n-heptane isomerization over 0.4%Pt/xSTA-MIL-101(Cr) catalyst was established.
    参考文献 | 相关文章 | 多维度评价
    2. 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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    3. 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.
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    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. Insights into the Reaction Network and Mechanism of Green Aerobic Oxidative Esterification of Methacrolein over Different Heterogeneous Catalysts
    厉晨豪 夏长久 刘聿嘉 黄开盟 彭欣欣 刘金胜 林民 朱斌 罗一斌 舒兴田
    中国炼油与石油化工    2021, 23 (3): 1-11.  
    摘要233)      PDF(pc) (848KB)(251)    收藏
    The oxidative esterification of methacrolein (MAL) is an important way to prepare high-valued methyl methacrylate (MMA), but this process is ultra-complex, due to the highly reactivity of both C=O and C=C bonds within MAL. In order to further improve the selectivity of MMA selectivity, the reaction network and mechanisms over different catalysts have been profoundly investigated in this paper. Five kinds of reactions are involved in this process, including (a) hemiacetal/acetal reaction; (b) aerobic oxidation of aldehyde/alcohol; (c) alkoxylation of C=C double bond; (d) Diels-Alder reaction; (e) hydrogenation reaction of double bond/ carbonyl. Among them, Diels-Alder reaction of MAL is noncatalyzed, and Br?nsted acid sites favor promoting hemiacetal/acetal reaction of MAL with methanol, while alkaline sites enhance the alkoxylation of C=C bond with methanol. In particular, by using Pd-based catalysts, several kinds of hydrogenated products are formed, hence with lower MMA selectivity than those of Au-based catalysts. Notably, it is of necessary to match the hemiacetal reaction of MAL with methanol to and aerobic oxidation of hemiacetal, which is relevant with the amount of Br?nsted acid and redox sites. Consequently, this work provides a good guidance for the further design of both catalysts and processes in future.
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    6. 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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    7. 热集成水网络优化设计的最新进展
    张池金 任聪静 廖祖维 孙婧元 王靖岱 阳永荣
    中国炼油与石油化工    2021, 23 (3): 69-75.  
    摘要188)      PDF(pc) (577KB)(166)    收藏
    It is well known that the process industry is an energy-intense and water-consuming industry and is the main source of industrial water consumption and energy in China. Energy integration and mass integration are important approaches to achieve energy saving and emission reduction in the process industry. Generally, the methods can be classified into two groups: conceptual design methods and mathematical programming methods. The former includes mainly graphical methods based on pinch technology that is operated easily. A feasible solution can be quickly obtained. Conceptual design methods are sequential in nature including targeting and design two steps. The latter is based on superstructure optimization and corresponding algorithm is adopted to solve the model. The trade-offs and connections among the entire network can be established and explored. Multiple factors can be considered and optimized simultaneously by mathematical programming methods. This paper describes the synthesis of heat integrated water allocation networks (HIWAN) based on both conceptual design methods and mathematical programming methods systematically. In addition, the characteristics and shortcomings of the existing research methods are summarized, and the future research direction is prospected.
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    8. 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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    9. 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
    10. 渣油加氢创新失活模型的应用
    张奎 聂红 戴立顺
    中国炼油与石油化工    2021, 23 (2): 11-20.  
    摘要174)      PDF(pc) (2154KB)(254)    收藏
    This article reports a new catalyst deactivation model for residue hydrotreating technology (RHT) with three adjustable parameters, named as "active-region-migration model". Active-region-migration model is proposed to describe the catalyst deactivation of RHT where the catalysts are deactivated due to metal loading. Along with the lumped reaction kinetics, the deactivation model can be applied to simulate the hydrogenation reaction performance in RHT. Industrial data from a commercial RHT unit show reasonably good agreements with the model calculations. Essentially, active-region-migration model can separately simulate the catalytic-activity change of each hydrogenation reaction during the whole run of RHT, with a single curve.
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    11. 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。
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    12. 碳包覆镍纳米复合材料在锂硫电池正极中的应用
    杨宇翔 谢婧新 吴耿煌 朱娜 李欢 荣峻峰
    中国炼油与石油化工    2021, 23 (4): 1-6.  
    摘要165)      PDF(pc) (882KB)(179)    收藏
    锂硫电池有望成为下一代高能量密度储能设备。近年来,“电催化”的概念被引入锂硫电池领域中,一些过渡金属被证明可以催化含硫物质的电化学转化反应。本工作中,比表面积为146 m2/g的碳包覆镍纳米材料对于硫正极的电化学反应具有电催化作用。加入碳包覆镍材料后,Ni@C/G-S电池获得了比G-S电池更好的电化学性能。在此基础上,通过对碳包覆镍的碳壳表面进行化学改性,进一步提高了锂硫电池的可逆比容量和循环稳定性。此外,本文详细研究了碳壳不同元素掺杂对锂硫电池性能的影响。N-Ni@C-G/S电池在0.2 C、0.5 C和1.0 C倍率下实现了更高的比容量,分别为1229 mAh/g、927 mAh/g和830 mAh/g;而B-Ni@C-G/S电池具有最好的循环稳定性。
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    13. HZSM-5分子筛酸性对苯和甲醇烷基化反应影响的密度泛函理论研究
    魏丕峰 付广斌 牟善良 高继超 闻振浩 朱学栋
    中国炼油与石油化工    2021, 23 (2): 21-27.  
    摘要155)      PDF(pc) (1789KB)(156)    收藏
    通过Al,Ga,In的同晶取代构建了不同酸性的HZSM-5分子筛,并通过密度泛函理论方法探究HZSM-5分子筛酸性对多甲基苯的吸附以及苯和甲醇烷基化反应能垒的影响。结果表明酸性对多甲基苯的吸附影响较小,而酸性和反应能垒则成线性关系。随着分子筛酸性的增强,反应能垒线性减小,在强酸环境中,分步机理起主导作用,而弱酸有利于协同机理。计算结果有助于理解分子筛酸性与其催化的多甲基苯烷基化反应之间的关系。
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    14. 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.
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    15. 不同改性方法处理ZSM-5分子筛对甲苯吸附性能的比较和分析:吸附动力学和机理研究
    张帅 李孟 李炜 李雨薇 刘芳 薛明 王永强 赵朝成
    中国炼油与石油化工    2021, 23 (1): 76-87.  
    摘要153)      PDF(pc) (2234KB)(262)    收藏
    MFI molecular sieve with high specific surface area, adjustable pore size and low production cost have been recognized as an effective adsorbent for VOCs removal. In this paper, NaOH solution was used to etch ZSM-5 to increase specific surface area and micro-mesoporous content. Graphene oxide (GO) was loaded on ZSM-5 by ultrasonic-assisted heating immersion method, and large π-bond structure and oxygen-containing functional groups were added to ZSM-5 for improving the composite adsorption performance. In addition, the properties of OH-ZSM-5 and ZSM-5@GO composites for toluene adsorption under different factors were also studied. It was positively correlated with initial concentration and adsorbent mass, but was negatively correlated with temperature. Meanwhile, the results showed that the saturated adsorption capacity of OH-ZSM-5 (107.3 mg/g) was 1.34 times higher than that of ZG-15% (80.2 mg/g). The pseudo-first-order and pseudo-second-order kinetic model can well describe the adsorption behavior of toluene on the OH-ZSM-5 and ZG-15%,  respectively. The adsorption mechanism of OH-ZSM-5 was mainly pore-filled adsorption. However, the adsorption mechanisms of ZSM-5@GO composite were pore-filled adsorption, π-π interaction, and H-bond interaction. This study will help to design a new strategy for enhancing the performance of traditional adsorbent ZSM-5 in VOCs removal.
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    16. 研究三维电催化体系中粒子电极位置对电催化反应效能的影响
    陆楷天 张永刚
    中国炼油与石油化工    2021, 23 (3): 30-39.  
    摘要152)      PDF(pc) (1621KB)(134)    收藏
    为了探究三维电催化反应器填充粒子的放置位置对电催化反应速率的影响,本文以亚甲基蓝为模拟有机废水,球状石墨颗粒为研究粒子电极,利用COMSOL Multiphysics软件模拟三维电催化反应器内的电势分布。以粒径大小、电势和位置为自变量,以一级反应动力学常数为因变量建立对数回归模型。结合模型预测了反应器不同位置的粒子电极降解有机污染物的效能。模拟结果表明,在三维电催化氧化反应器内粒子电极对污染物降解的反应效能是不均匀的,增加电场强度可以改变粒子电极电催化反应效能的分布,其中越靠近阳极端位置的粒子电极其降解污染物的能力越高。粒子颗粒内部不同位置之间的电催化反应速率的差异较大,按照差异程度可大致分为三个区域并模拟了粒子电极内部不同位置的电催化反应效能分布。
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    17. 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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    18. Heat Exchanger Network Retrofit for Optimization of Crude Distillation Unit Using Pinch Analysis
    孙梦迎 付佃亮 孙兰义
    中国炼油与石油化工    2021, 23 (1): 31-40.  
    摘要148)      PDF(pc) (1784KB)(287)    收藏
    Crude distillation unit (CDU) is regarded as the main energy consumer in the entire refinery process. In this paper, the process simulation software and the energy management software are used to simulate the flowsheet and analyze the energy consumption, respectively. Stream data obtained from an existing CDU are applicable in the pinch analysis. To reduce the amount of cross-pinch heat transfer, three approaches of resequencing, repiping, and adding heat exchangers are adopted. Compared with the existing CDU, the results demonstrate that the inlet temperature of the furnace can be increased by 25.4 ℃, the amount of hot and cold utilities can be reduced by 15.1% and 19.6%, respectively. The economic evaluation indicates that the operating cost is saved by 8×106 $/a, and the payback period is about 9 months.
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    19. 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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    20. 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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