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    1. 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356)      PDF(pc) (734KB)(316)    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。
    参考文献 | 相关文章 | 多维度评价
    2. 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222)      PDF(pc) (848KB)(240)    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.
    参考文献 | 相关文章 | 多维度评价
    3. 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185)      PDF(pc) (577KB)(140)    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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    4. 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168)      PDF(pc) (2154KB)(241)    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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    5. 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156)      PDF(pc) (882KB)(168)    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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    6. 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150)      PDF(pc) (1789KB)(150)    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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    7. 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147)      PDF(pc) (1621KB)(125)    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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    8. Fabrication of Fe Nanoparticles into N-doped Mesoporous Carbon Nanotube Derived from rice-like Fe/N-MOF and its ORR catalytic performance for MFC
    卢德成 王文艺 常嘉诚 王雪芹 王园园 宋华
    中国炼油与石油化工    2021, 23 (2): 98-108.  
    摘要142)      PDF(pc) (2540KB)(126)    收藏
    非贵金属氧还原催化剂(ORR)的发展,以改善微生物燃料电池(MFC)的性能仍然是一个极大的挑战。本文以乙腈为氮前体,在低成本的有机溶剂中,以Fe/N-MOF为原料,采用热解法制备了铁基含氮多孔碳纳米管Fe/N-MC-T ORR催化剂。通过SEM、TEM、BET、XRD和XPS对不同热解温度下Fe/N-MC-T催化剂进行了表征。Fe/N-MOF呈光滑的米粒状结构,粒径约为400×50 nm。Fe/N-MC-T中的铁元素主要以零价铁的形式存在,Fe3C含量较低。电化学测试结果表明,Fe/N-MC-T的起始电位和半波电位分别为0.89 V和0.80 V,略低于商用Pt/C的0.92 V和0.82 V,说明Fe/N-MC-700对ORR具有较高的电催化活性。Fe/N-MC-700在MFC中显示的最高功率密度864.1 mW?m - 2,大约是碳布的2.25倍,略低于MFC和Pt / C (20 wt %) (1002.0 mW?m - 2),展示了铁颗粒包裹在碳纳米管是具有高度活跃的氧还原性能。
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    9. Heat transfer and kinetics study of Moroccan oil shale pyrolysis process
    湛晨宇 马跃 岳长涛 李术元 唐勋 文华
    中国炼油与石油化工    2021, 23 (2): 28-33.  
    摘要129)      PDF(pc) (1274KB)(167)    收藏
    The basic properties of Moroccan oil shale were analyzed in this paper. Pyrolysis experiments at different heating rates were carried out by thermogravimetry. The results show that the process of Moroccan oil shale can be divided into three steps. A shrink-nuclear model that considers the internal heat transfer of particles was established. The pyrolysis kinetic parameters of Moroccan oil shale were calculated based on heat transfer data and basic physical parameters. The results show that the apparent activation energy of the reaction is about 120 kJ/mol, the apparent frequency factor is about 2×1014 mol/(s?m2). Therefore, the pyrolysis process of oil shale can be better simulated by shrink-nuclear model considering the internal heat transfer of the particles.
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    10. 表面活性剂对柔性金属有机骨架材料MIL-53(Fe)的孔结构及光催化性能的控制
    张丹 杨萍 张尤华 段林海 孟秀红
    中国炼油与石油化工    2021, 23 (3): 23-29.  
    摘要128)      PDF(pc) (829KB)(127)    收藏
    提出了一种利用表面活性剂控制柔性金属有机骨架材料MIL-53(Fe)孔道结构的方法。表面活性剂四乙基氢氧化铵(TEAOH)控制MIL-53(Fe)的孔道形式为“闭孔”的形式,而表面活性剂聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)或者聚乙烯醇(PVA)控制MIL-53(Fe)的孔道形式为“开孔”的形式。通过紫外光辐射降解罗丹明B水溶液的方式来考察不同孔道形式的MIL-53(Fe)的光催化性能。结果表明“开孔”的MIL-53(Fe)比“闭孔”的MIL-53(Fe)呈现出更高的光催化活性。由表面活性剂PVA改良的MIL-53(Fe)具有最好的光催化活性,90分钟内讲解了100%的罗丹明B水溶液。
    参考文献 | 相关文章 | 多维度评价
    11. Effect of Water on Extractive Desulfurization of Simulated FCC Gasoline Using Ionic Liquid NMP-FeCl3-H2O
    方柳亚 沈陟 沈喜洲 康顺吉
    中国炼油与石油化工    2021, 23 (2): 121-131.  
    摘要124)      PDF(pc) (1125KB)(126)    收藏
    A series of novel aqueous ionic liquids (NMP-FeCl3-nH2O) were prepared and the effects of water in the aqueous ionic liquids on desulfurization rate and selectivity of simulated FCC gasoline were investigated. The results showed that adding a small amount of water into the ionic liquid NMP-FeCl3 could effectively improve the desulfurization rate and selectivity, and the optimal added amount of water was 5wt% ~ 10wt% of NMP. Finally, the possible desulfurization mechanism activated by a small amount of water was proposed.
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    12. Heat Exchanger Network Retrofit of Diesel Hydrotreating Unit Using Pinch Analysis
    孙梦迎 张凤娇 刘兴隆 孙兰义
    中国炼油与石油化工    2021, 23 (2): 34-43.  
    摘要123)      PDF(pc) (1302KB)(177)    收藏
    Diesel hydrotreating unit (DHT) is an integral part of the refinery, and its energy-saving optimization is of great significance to the enterprise. In this paper, process simulation software and energy management software are used to simulate the flowsheet and analyze the energy consumption, respectively. Stream data obtained from an existing DHT are applied in the pinch analysis for retrofitting the heat exchanger network (HEN) to achieve maximum energy utilization by using pinch analysis. Since DHT is constrained by pressure, the pressure factor is considered in the process of retrofitting. The results show that the amount of cross-pinch heat transfer is reduced, the inlet temperature of the furnace is increased by 55 ℃, and the amount of hot and cold utilities can be reduced by 70.25% and 50.16%, respectively. The economic evaluation indicates that the operating cost is saved by 4.39×106 $/a, and the payback period is about 2 months.
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    13. The Synthesis of Ultra-High Molecular Weight Polypropylene Using Supported Ziegler-Natta Catalyst via Combining Internal Electron Donor and Cocatalyst Loaded on
    夏晓琪 李红明 李春漫 苗青 李静 朱峰 黄启谷 义建军 赵众
    中国炼油与石油化工    2021, 23 (3): 12-22.  
    摘要123)      PDF(pc) (948KB)(121)    收藏
    Due to the development of the new energy industry, polypropylene with ultra-high molecular weight plays a  crucial role for battery isolation membrane. This work investigated the effect of internal electron donor of Ziegler-Natta  catalyst system on the molecular weight of the obtained polypropylene. The scanning electron microscope (SEM) and  Canon camera were used to characterize the surface morphologies of catalyst particles and polymer particles, respectively.  Compared with the polypropylene particles featuring a spherical shape, these study results confirmed that the morphology  duplication theory from the catalyst particle to the morphology of polymer particle was exhibited. The gel permeation  chromatography (GPC) results revealed that the obtained polypropylene has a much higher average molecular weight than  those prepared by conventional method. The Fourier transform infrared spectrometry (FT-IR) and X-ray photoelectron  spectroscopy (XPS) revealed that the carbonyl oxygen atom on ester group was preferentially bound to Mg and Ti, as  compared to the ether oxygen atom. The XPS results showed that the ratio of Ti3+/Ti4+ could be changed by internal electron  donors. When Ti3+content was nearly 99% in the Ziegler-Natta catalyst system, isotactic polypropylene with an ultra-high  molecular weight of up to 1.42×106 g/mol was obtained by Cat. 3. This result  implied that internal electron donor ID3 could  reduce the β-hydride elimination reaction to further increase the molecular weight of the obtained polymer.
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    14. MOF衍生的高选择性加氢芳香硝基化合物的石墨碳包覆镍催化剂
    吴耿煌 荣峻峰
    中国炼油与石油化工    2021, 23 (3): 40-49.  
    摘要116)      PDF(pc) (1352KB)(109)    收藏
    针对芳香硝基化合物的催化选择性加氢反应,开发可替代贵金属催化剂的低成本、高效非贵金属催化剂,对于芳香胺类化合物的绿色生产具有重要意义。利用简易、可规模化的制备方法,以镍—2,5-吡啶二羧酸金属有机框架为前驱体,热解制备了氮掺杂石墨碳包覆镍纳米催化材料(Ni@CN)。采用X射线衍射、扫描电镜、透射电镜、元素分析、N2吸脱附等检测手段对Ni@CN的物化性质进行了表征,并对其催化性能进行了评价。结果表明,Ni@CN可在温和条件下(85℃,1.0 MPa H2)高效加氢含取代官能团的芳香硝基化合物生成对应的芳香胺类化合物。对比试验表明,镍纳米颗粒是Ni@CN的加氢活性中心,而石墨碳壳的存在有利于优先吸附硝基官能团。此外,进一步考察了Ni@CN的循环使用性能以及抗硫化物中毒的特性。
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    15. 固定化双酶在循环冷却水中增强环氧树脂对Q235碳钢的耐腐蚀性
    姜国飞 赵小萱 李炜 车阳丽 刘芳
    中国炼油与石油化工    2021, 23 (2): 109-120.  
    摘要116)      PDF(pc) (1821KB)(121)    收藏
    通过一锅合成法制备羧基官能化的SBA-15(COOH / SBA-15),并通过FT-IR,SEM,XRD和BET对制备的材料进行表征。 使用COOH / SBA-15作为载体,制备了固定化的双酶COOH-SBA-15 / LZM-LP(脂肪酶和溶菌酶)。 正交试验采用缓蚀指数优化了固定化条件。 电化学测试表明,COOH-SBA-15 / LZM-LP可以显着抑制循环冷却水中碳钢的腐蚀。 当用量为0.2 g·L-1时,腐蚀抑制率高于93%。 从羧基和酶的角度提出了抑制机理。 最后,当将COOH-SBA-15 / LZM-LP掺杂到环氧树脂中时,发现可以显着提高环氧树脂涂料的耐腐蚀性,并且在浸泡720 h后其耐腐蚀性仅下降0.23%。
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    16. Study on Reducing Injection Pressure of Low Permeability Reservoirs Characterized by High Temperature and High Salinity
    赵琳 秦冰 吴雄军 王增林 江建林
    中国炼油与石油化工    2021, 23 (2): 44-54.  
    摘要115)      PDF(pc) (1322KB)(157)    收藏
    In view of the problems of high injection pressure and low water injection rate in water injection wells of low permeability reservoirs with high temperature and high salinity, two new surfactants were synthesized, including quaternary ammonium Gemini surfactant and betaine amphoteric surfactant. The composite surfactant system BYJ-1 was formed by mixing two kinds of surfactants. The minimum interfacial tension between BYJ-1 solution and the crude oil could reach 1.4×10-3mN/m. The temperature resistance was up to 140℃, and the salt resistance was up to 120g/L. For the low permeability core fully saturated with water phase, BYJ-1 could obviously reduce the starting pressure gradient of low permeability core. While for the core with residual oil, BAY-1 could obviously reduce the injection pressure and improve the oil recovery. Moreover, the field test showed that BAY-1 could obviously reduce the injection pressure of the water injection well, increase the injection volume, and increase the liquid production and oil production of the corresponding production well.
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    17. 双介孔TiO2-PTA/BMMS的合成及其光催化氧化脱硫性能研究
    杨丽娜 张熙 崔莉程 徐美珍 李剑
    中国炼油与石油化工    2021, 23 (3): 58-68.  
    摘要110)      PDF(pc) (1371KB)(81)    收藏
    为了提高TiO2的光催化氧化脱硫(PODS)活性,利用负载和复合的协同作用,将TiO2与磷钨酸 (PTA)复合,通过两步浸渍法合成制备了TiO2-PTA/BMMS。采用XRD、N2 吸附脱附、XRF、FTIR、UV-vis、SEM、EDS 和 TEM 对催化剂进行了表征;以含二苯并噻吩(DBT)的十二烷溶液为模拟油,评价了催化剂的催化性能。表征结果表明,PTA 的引入为双介孔载体提供更高的表面积和孔体积。在紫外光照射下,TiO2-PTA/BMMS在模拟反应体系中脱硫率可达到 99.6%,脱硫率远高于 TiO2/BMMS 脱硫率。同时对催化剂进行重复使用实验,重复八次后催化活性没有显着下降。
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    18. 甲基环己烷催化转化反应对改性工业Y沸石酸性的表征
    侯凯歌 秦波 韩俊杰 杜艳泽 马静红 李瑞丰
    中国炼油与石油化工    2021, 23 (3): 50-57.  
    摘要107)      PDF(pc) (512KB)(94)    收藏
    以甲基环己烷(MCH)的催化转化反应为模型反应,并结合吡啶吸附红外光谱和羟基红外光谱技术对三种具有不同硅铝比和介孔孔隙的改性工业脱铝Y沸石的酸性(酸量、酸强和酸性点的可接近性)进行了表征研究。通过MCH催化转化反应的反应结果分析,可以得出,MCH的反应活性(总转化率)依赖于Y沸石催化剂表面的酸量, 而TOF值可反映沸石内质子位酸性点的可接近性。MCH催化转化的产品由裂解、芳香烃和异构三类产品构成,其中裂解产物的产率随着沸石微孔中强质子酸位点的浓度的增加而增加;随着Y沸石脱铝程度的增加,沸石内酸量减少,分子的扩散距离缩短从而导致二次反应的几率降低,从而使芳香烃的产率随之降低;同时,裂解产物中C7产物和烯烃/烷烃比率增加。研究结果还显示出,i-C4产物的选择性随脱铝Y沸石在其羟基红外光谱中3600cm-1处的吸收峰强度的增加而增加,即i-C4产物的选择性可反映沸石内强质子酸位点的数目。
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    19. 加氢苛刻度对烃类组成和催化裂解产品分布的影响
    邓中活 戴立顺 牛传峰 贾燕子 魏晓丽 蔡新恒
    中国炼油与石油化工    2021, 23 (3): 112-118.  
    摘要103)      PDF(pc) (868KB)(109)    收藏
    Residue deep hydrotreating (RDHT) process was developed by the Research Institute of Petroleum Processing (RIPP) to provide high quality feedstock for deep catalytic cracking (DCC) process. In this research work, the effects of RDHT process and reaction severity on heteroatom removal, hydrogen content increase, hydrocarbon composition improvement, and DCC product yields were studied. It was showed that the RDHT process can effectively reduce heteroatoms, increase hydrogen content and improve the hydrocarbon compositions, which can contribute to an increase of light olefins yield in DCC unit.
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    20. Adsorption and regeneration of Volatile Organic Compounds(VOCs) on coal-based activated carbon by ferric nitrate modification
    金春江 王鲁元
    中国炼油与石油化工    2021, 23 (3): 137-150.  
    摘要100)      PDF(pc) (1963KB)(68)    收藏
    In this work, heishan coal was used to prepare a series of activated carbon samples (ACs) l via a vapor depositition method. The effects of the weight ratio (Fe(NO3)3:coal ) on the physicochemical properties of the activated carbon were systematically investigated, and the ACS samples were detected by N2 adsorption-desorption, SEM, XRD, Raman and FTIR. Furthermore, the adsorption properties for ethyl acetate were tested. The results indicated that as the ratio increasing from 1:8 to 1:2, the specific surface area, total pore volume and micropore volume first increase and then decrease,the specific surface area increased from 560.86 m2/g to 685.90 m2/g and then decreased to 299.56m2/g. The total pore volume and micropore volume increased from 0.29cm3/g, 0.17cm3/g to 0.30cm3/g, 0.22cm3/g, and then decreased to 0.16cm3/g and 0.10cm3/g, respectively. The optimized ratio is ~. in the activation process, The iron ions would be infiltrated into the activated carbon could significantly promote the development of pore structure, especially the pores with pore size between 2.5-3nm, which enhance the adsorption capacity of ethyl acetate. It is worth noting thatthe ACs had the largest specific surface area and total pore volume of 685.90 m2/g and 0.30 cm3/g under the optimized activation (950oC, 20 vol.% CO2 ,the ratio is 1:5), the maximum adsorption capacity of ethyl acetate was 962.62mg/g, and after 7 times of repeated thermal regeneration experiments, the saturated adsorption capacity was still above 90%.
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